Ye Wang

Abstract Low temperature solution processed planar‐structure perovskite solar cells gain great attention recently, while their power conversions are still lower than that of high temperature mesoporous counterpart. Previous reports are mainly focused on perovskite morphology control and interface engineering to improve performance. Here, this study systematically investigates the effect of precise stoichiometry, especially the PbI 2 contents on device performance including efficiency, hysteresis and stability. This study finds that a moderate residual of PbI 2 can deliver stable and high efficiency of solar cells without hysteresis, while too much residual PbI 2 will lead to serious hysteresis and poor transit stability. Solar cells with the efficiencies of 21.6% in small size (0.0737 cm 2 ) and 20.1% in large size (1 cm 2 ) with moderate residual PbI 2 in perovskite layer are obtained. The certificated efficiency for small size shows the efficiency of 20.9%, which is the highest efficiency ever recorded in planar‐structure perovskite solar cells, showing the planar‐structure perovskite solar cells are very promising.

The present review synthesizes recent literature on social determinants and mental health outcomes and provides recommendations for how to advance the field. We summarize current studies related to changes in the conceptualization of social determinants, how social determinants impact mental health, what we have learned from social determinant interventions, and new methods to collect, use, and analyze social determinant data. Recent research has increasingly focused on interactions between multiple social determinants, interventions to address upstream causes of mental health challenges, and use of simulation models to represent complex systems. However, methodological challenges and inconsistent findings prevent a definitive understanding of which social determinants should be addressed to improve mental health, and within what populations these interventions may be most effective. Recent advances in strategies to collect, evaluate, and analyze social determinants suggest the potential to better appraise their impact and to implement relevant interventions.

The ethanol oxidation reaction (EOR) has drawn increasing interest in electrocatalysis and fuel cells by considering that ethanol as a biomass fuel has advantages of low toxicity, renewability, and a high theoretical energy density compared to methanol. Since EOR is a complex multiple-electron process involving various intermediates and products, the mechanistic investigation as well as the rational design of electrocatalysts are challenging yet essential for the desired complete oxidation to CO2. This mini review is aimed at presenting an overview of the advances in the study of reaction mechanisms and electrocatalytic materials for EOR over the past two decades with a focus on Pt- and Pd-based catalysts. We start with discussion on the mechanistic understanding of EOR on Pt and Pd surfaces using selected publications as examples. Consensuses from the mechanistic studies are that sufficient active surface sites to facilitate the cleavage of the C–C bond and the adsorption of water or its residue are critical for obtaining a higher electro-oxidation activity. We then show how this understanding has been applied to achieve improved performance on various Pt- and Pd-based catalysts through optimizing electronic and bifunctional effects, as well as by tuning their surface composition and structure. Finally we point out the remaining key problems in the development of anode electrocatalysts for EOR.

The photocatalytic reduction of carbon dioxide with water to fuels and chemicals is a longstanding challenge. This article focuses on the effects of cocatalysts and reaction modes on photocatalytic behaviors of TiO2 with an emphasis on the selectivity of photogenerated electrons for CO2 reduction in the presence of H2O, which has been overlooked in most of the published papers. Our results clarified that the reaction using H2O vapor exhibited significantly higher selectivity for CO2 reduction than that by immersing the photocatalyst into liquid H2O. We examined the effect of noble metal cocatalysts and found that the rate of CH4 formation increased in the sequence of Ag < Rh < Au < Pd < Pt, corresponding well to the increase in the efficiency of electron–hole separation. This indicates that Pt is the most effective cocatalyst to extract photogenerated electrons for CO2 reduction. The selectivity of CH4 in CO2 reduction was also enhanced by Pt. The size and loading amount of Pt affected the activity; a smaller mean size of Pt particles and an appropriate loading amount favored the formation of reduction products. The reduction of H2O to H2 was accelerated more than the reduction of CO2 in the presence of Pt, leading to a lower selectivity for CO2 reduction and limited increases in CH4 formation rate. We demonstrated that the addition of MgO into the Pt–TiO2 catalyst could further enhance the formation of CH4. The formation of H2 was suppressed simultaneously, suggesting the increase in the selectivity for CO2 reduction in the presence of MgO. Furthermore, the MgO- and Pt-modified TiO2 catalyst exhibited a higher CH4 selectivity in CO2 reduction.

This review highlights recent advances in photocatalytic transformations of lignocellulosic biomass (polysaccharides and lignin) into chemicals (in particular organic oxygenates).

Cucurbitacins are triterpenoids that confer a bitter taste in cucurbits such as cucumber, melon, watermelon, squash, and pumpkin. These compounds discourage most pests on the plant and have also been shown to have antitumor properties. With genomics and biochemistry, we identified nine cucumber genes in the pathway for biosynthesis of cucurbitacin C and elucidated four catalytic steps. We discovered transcription factors Bl ( Bitter leaf ) and Bt ( Bitter fruit ) that regulate this pathway in leaves and fruits, respectively. Traces in genomic signatures indicated that selection imposed on Bt during domestication led to derivation of nonbitter cucurbits from their bitter ancestors.

Binary co-catalysts of Pt and Cu2O with a core–shell structure significantly enhance the photocatalytic reduction of CO2 with H2O to CH4 and CO. The Cu2O shell provides sites for the preferential activation and conversion of CO2, whereas the Pt core extracts the photogenerated electrons from TiO2. The deposition of Cu2O shell on Pt nanoparticles markedly suppresses the reduction of H2O to H2 (see picture). As a service to our authors and readers, this journal provides supporting information supplied by the authors. Such materials are peer reviewed and may be re-organized for online delivery, but are not copy-edited or typeset. Technical support issues arising from supporting information (other than missing files) should be addressed to the authors. Please note: The publisher is not responsible for the content or functionality of any supporting information supplied by the authors. Any queries (other than missing content) should be directed to the corresponding author for the article.

<h2>Summary</h2> Metabolic adaptation is essential for cell survival during nutrient deprivation. We report that eukaryotic elongation factor 2 kinase (eEF2K), which is activated by AMP-kinase (AMPK), confers cell survival under acute nutrient depletion by blocking translation elongation. Tumor cells exploit this pathway to adapt to nutrient deprivation by reactivating the AMPK-eEF2K axis. Adaptation of transformed cells to nutrient withdrawal is severely compromised in cells lacking eEF2K. Moreover, eEF2K knockdown restored sensitivity to acute nutrient deprivation in highly resistant human tumor cell lines. In vivo, overexpression of eEF2K rendered murine tumors remarkably resistant to caloric restriction. Expression of <i>eEF2K</i> strongly correlated with overall survival in human medulloblastoma and glioblastoma multiforme. Finally, <i>C. elegans</i> strains deficient in <i>efk-1</i>, the <i>eEF2K</i> ortholog, were severely compromised in their response to nutrient depletion. Our data highlight a conserved role for eEF2K in protecting cells from nutrient deprivation and in conferring tumor cell adaptation to metabolic stress. <h3>PaperClip</h3>

The direct transformation of cellulose, which is the main component of lignocellulosic biomass, into building-block chemicals is the key to establishing biomass-based sustainable chemical processes. Only limited successes have been achieved for such transformations under mild conditions. Here we report the simple and efficient chemocatalytic conversion of cellulose in water in the presence of dilute lead(II) ions, into lactic acid, which is a high-value chemical used for the production of fine chemicals and biodegradable plastics. The lactic acid yield from microcrystalline cellulose and several lignocellulose-based raw biomasses is >60% at 463 K. Both theoretical and experimental studies suggest that lead(II) in combination with water catalyses a series of cascading steps for lactic acid formation, including the isomerization of glucose formed via the hydrolysis of cellulose into fructose, the selective cleavage of the C3-C4 bond of fructose to trioses and the selective conversion of trioses into lactic acid.

Abstract Electrocatalytic CO 2 reduction to CO emerges as a potential route of utilizing emitted CO 2 . Metal‐N‐C hybrid structures have shown unique activities, however, the active centers and reaction mechanisms remain unclear because of the ambiguity in true atomic structures for the prepared catalysts. Herein, combining density‐functional theory calculations and experimental studies, the reaction mechanisms for well‐defined metal–N 4 sites were explored using metal phthalocyanines as model catalysts. The theoretical calculations reveal that cobalt phthalocyanine exhibits the optimum activity for CO 2 reduction to CO because of the moderate *CO binding energy at the Co site, which accommodates the *COOH formation and the *CO desorption. It is further confirmed by experimental studies, where cobalt phthalocyanine delivers the best performance, with a maximal CO Faradaic efficiency reaching 99 %, and maintains stable performance for over 60 hours.

The low-temperature hydrogenation of CO2 to methanol is of great significance for the recycling of this greenhouse gas to valuable products, however, it remains a great challenge due to the trade-off between catalytic activity and selectivity. Here, we report that CO2 can dissociate at sulfur vacancies in MoS2 nanosheets to yield surface-bound CO and O at room temperature, thus enabling a highly efficient low-temperature hydrogenation of CO2 to methanol. Multiple in situ spectroscopic and microscopic characterizations combined with theoretical calculations demonstrated that in-plane sulfur vacancies drive the selective hydrogenation of CO2 to methanol by inhibiting deep hydrogenolysis to methane, whereas edge vacancies facilitate excessive hydrogenation to methane. At 180 °C, the catalyst achieved a 94.3% methanol selectivity at a CO2 conversion of 12.5% over the in-plane sulfur vacancy-rich MoS2 nanosheets, which notably surpasses those of previously reported catalysts. This catalyst exhibited high stability for over 3,000 hours without any deactivation, rendering it a promising candidate for industrial application. The catalytic hydrogenation of CO2 to methanol is a crucial reaction for the recycling of this greenhouse gas, although the selection and related performance of commercial catalysts is still limited. Now, the authors introduce sulfur vacancy-rich MoS2 nanosheets as a superior catalyst for this process, rivalling the commercial benchmark system.

Using a new Arabidopsis (Arabidopsis thaliana) mutant (Atnrt2.1-nrt2.2) we confirm that concomitant disruption of NRT2.1 and NRT2.2 reduces inducible high-affinity transport system (IHATS) by up to 80%, whereas the constitutive high-affinity transport system (CHATS) was reduced by 30%. Nitrate influx via the low-affinity transport system (LATS) was unaffected. Shoot-to-root ratios were significantly reduced compared to wild-type plants, the major effect being upon shoot growth. In another mutant uniquely disrupted in NRT2.1 (Atnrt2.1), IHATS was reduced by up to 72%, whereas neither the CHATS nor the LATS fluxes were significantly reduced. Disruption of NRT2.1 in Atnrt2.1 caused a consistent and significant reduction of shoot-to-root ratios. IHATS influx and shoot-to-root ratios were restored to wild-type values when Atnrt2.1-nrt2.2 was transformed with a NRT2.1 cDNA isolated from Arabidopsis. Disruption of NRT2.2 in Atnrt2.2 reduced IHATS by 19% and this reduction was statistically significant only at 6 h after resupply of nitrate to nitrogen-deprived plants. Atnrt2.2 showed no significant reduction of CHATS, LATS, or shoot-to-root ratios. These results define NRT2.1 as the major contributor to IHATS. Nevertheless, when maintained on agar containing 0.25 mm KNO(3) as the sole nitrogen source, Atnrt2.1-nrt2.2 consistently exhibited greater stress and growth reduction than Atnrt2.1. Evidence from real-time PCR revealed that NRT2.2 transcript abundance was increased almost 3-fold in Atnrt2.1. These findings suggest that NRT2.2 normally makes only a small contribution to IHATS, but when NRT2.1 is lost, this contribution increases, resulting in a partial compensation.

Existing content-based music recommendation systems typically employ a \textit{two-stage} approach. They first extract traditional audio content features such as Mel-frequency cepstral coefficients and then predict user preferences. However, these traditional features, originally not created for music recommendation, cannot capture all relevant information in the audio and thus put a cap on recommendation performance. Using a novel model based on deep belief network and probabilistic graphical model, we unify the two stages into an automated process that simultaneously learns features from audio content and makes personalized recommendations. Compared with existing deep learning based models, our model outperforms them in both the warm-start and cold-start stages without relying on collaborative filtering (CF). We then present an efficient hybrid method to seamlessly integrate the automatically learnt features and CF. Our hybrid method not only significantly improves the performance of CF but also outperforms the traditional feature mbased hybrid method.

Two dimension (2D) layered molybdenum disulfide (MoS2) has emerged as a promising candidate for the anode material in lithium ion batteries (LIBs). Herein, 2D MoSx (2 ≤ x ≤ 3) nanosheet-coated 1D multiwall carbon nanotubes (MWNTs) nanocomposites with hierarchical architecture were synthesized via a high-throughput solvent thermal method under low temperature at 200°C. The unique hierarchical nanostructures with MWNTs backbone and nanosheets of MoSx have significantly promoted the electrode performance in LIBs. Every single MoSx nanosheet interconnect to MWNTs centers with maximized exposed electrochemical active sites, which significantly enhance ion diffusion efficiency and accommodate volume expansion during the electrochemical reaction. A remarkably high specific capacity (i.e., > 1000 mAh/g) was achieved at the current density of 50 mA g(-1), which is much higher than theoretical numbers for either MWNTs or MoS2 along (~372 and ~670 mAh/g, respectively). We anticipate 2D nanosheets/1D MWNTs nanocomposites will be promising materials in new generation practical LIBs.

In this article, we report a novel electrode of NiCo2O4 nanowire arrays (NWAs) on carbon textiles with a polypyrrole (PPy) nanosphere shell layer to enhance the pseudocapacitive performance. The merits of highly conductive PPy and short ion transport channels in ordered NiCo2O4 mesoporous nanowire arrays together with the synergistic effect between NiCo2O4 and PPy result in a high specific capacitance of 2244 F g–1, excellent rate capability, and cycling stability in NiCo2O4/PPy electrode. Moreover, a lightweight and flexible asymmetric supercapacitor (ASC) device is successfully assembled using the hybrid NiCo2O4@PPy NWAs and activated carbon (AC) as electrodes, achieving high energy density (58.8 W h kg–1 at 365 W kg–1), outstanding power density (10.2 kW kg–1 at 28.4 W h kg–1) and excellent cycling stability (∼89.2% retention after 5000 cycles), as well as high flexibility. The three-dimensional coaxial architecture design opens up new opportunities to fabricate a high-performance flexible supercapacitor for future portable and wearable electronic devices.

The electrocatalytic reduction of CO2 with H2O to multi-carbon (C2+) compounds, in particular, C2+ olefins and oxygenates, which have versatile applications in the chemical and energy industries, holds great potential to mitigate the depletion of fossil resources and abate carbon emissions. There are two major routes for the electrocatalytic CO2 reduction to C2+ compounds, i.e., the direct route and the indirect route via CO. The electrocatalytic CO2 reduction to CO has been commercialised with solid oxide electrolysers, making the indirect route via CO to C2+ compounds also a promising alternative. This tutorial review focuses on the similarities and differences in the electrocatalytic CO2 and CO reduction reactions (CO2RR and CORR) into C2+ compounds, including C2H4, C2H5OH, CH3COO- and n-C3H7OH, over Cu-based catalysts. First, we introduce the fundamental aspects of the two electrocatalytic reactions, including the cathode and anode reactions, electrocatalytic reactors and crucial performance parameters. Next, the reaction mechanisms, in particular, the C-C coupling mechanism, are discussed. Then, efficient catalysts and systems for these two reactions are critically reviewed. We analyse the key factors that determine the selectivity, activity and stability for the electrocatalytic CO2RR and CORR. Finally, the opportunities, challenges and future trends in the electrocatalytic CO2RR and CORR are proposed. These insights will offer guidance for the design of industrial-relevant catalysts and systems for the synthesis of C2+ olefins and oxygenates.

CO2 dry reforming of methane (DRM) not only utilized the two greenhouse gases, CO2 and CH4, but also produced synthesis gas, which could be used for Fischer-Tropsch synthesis. Besides, DRM reaction could utilize marsh gas and the gaseous products from pyrolysis of biomass, consequently increasing their value for businesses and reducing environment pollution, thereby providing ways for sustainable development. Nickel based catalyst was widely used in DRM reaction. This paper reviewed the recent progresses of the DRM reaction at low temperature. Suitable supports and promoters improved the catalytic performance by adjusting the interaction between nickel and the support. Besides, the temperature of calcination, the order of materials loading on support, the reduction temperature, and the nickel particle size also altered the performance of the catalysts. It was suggested that by investigating the interaction of supports, promoters with nickel, as well as their structural adjustment, the development of low temperature DRM catalysts was feasible.

Abstract As a prospective next‐generation energy storage solution, lithium–sulfur batteries excel at their economical attractiveness (sulfur abundance) and electrochemical performance (high energy density, ≈2600 Wh kg −1 ). However, their application is impracticable without addressing the following vital issues: i) shuttling effect of lithium polysulfides (LPSs), ii) sluggish redox conversion kinetics of LPSs, iii) large volumetric expansion of S after lithiation (≈80%), and iv) uncontrollable Li dendritic formation. Recently, many strategies have been proposed to solve these issues, which have focused on physical/chemical entrapment of LPSs, catalytic promotion of LPSs conversion and directional regulation of Li plating/stripping. Designing/constructing heterostructured materials is one of the promising approaches to potentially resolve all the above challenges with one material. In this review, the recent advances of heterostructures focused on S cathodes, interlayers and Li anodes are reviewed in detail. First, the fundamental chemistry of Li–S batteries and principles of heterostructures reinforced Li–S batteries are described. Second, the applications of heterostructures in Li–S batteries are discussed comprehensively. Finally, a concise outlook on utilizing the intrinsic and extrinsic properties of heterostructures is delivered, with the aim to provide some inspiration for the design and fabrication of advanced Li–S batteries.

A hybrid nanoarchitecture aerogel composed of WS 2 nanosheets and carbon nanotube‐reduced graphene oxide (CNT‐rGO) with ordered microchannel three‐dimensional (3D) scaffold structure was synthesized by a simple solvothermal method followed by freeze‐drying and post annealing process. The 3D ordered microchannel structures not only provide good electronic transportation routes, but also provide excellent ionic conductive channels, leading to an enhanced electrochemical performance as anode materials both for lithium‐ion batteries (LIBs) and sodium‐ion batteries (SIBs). Significantly, WS 2 /CNT‐rGO aerogel nanostructure can deliver a specific capacity of 749 mA h g −1 at 100 mA g −1 and a high first‐cycle coulombic efficiency of 53.4% as the anode material of LIBs. In addition, it also can deliver a capacity of 311.4 mA h g −1 at 100 mA g −1 , and retain a capacity of 252.9 mA h g −1 at 200 mA g −1 after 100 cycles as the anode electrode of SIBs. The excellent electrochemical performance is attributed to the synergistic effect between the WS 2 nanosheets and CNT‐rGO scaffold network and rational design of 3D ordered structure. These results demonstrate the potential applications of ordered CNT‐rGO aerogel platform to support transition‐metal‐dichalcogenides (i.e., WS 2 ) for energy storage devices and open up a route for material design for future generation energy storage devices.

Lithium sulfur (Li-S) batteries have attracted considerable attention as the next generation rechargeable batteries owing to their much higher energy density in contrast to the conventional lithium ion batteries (LIBs). However, the inferior cycling performance as well as rate capability, resulted from the polysulfides shuttle effect and sluggish reaction kinetics, remains as major hurdles for its practical application. Herein, a high-rate and ultrastable Li-S battery has been demonstrated by using the multifunctional iron phosphide (FeP) nanocrystals as an efficient host material to anchor the polysulfides and regulate the polysulfide redox conversion. Density functional theory (DFT) calculations indicate that FeP can provide strong chemical bonding towards polysulfides. The FeP nanocrystals show high catalytic effect to facilitate the polysulfides conversion reaction and lower the Li2S nucleation energy. Additionally, the 3D rGO-CNTs scaffold enables fast and continuous long-distance electron transportation and accommodates large volumetric change during the charge/discharge processes. As a result, the FeP nanocrystals with intrinsic polysulfide affinity and catalytic activity suppress the polysulfide dissolution and enhance the redox reaction kinetics, enabling ultrastable cycling (0.04% capacity decay per cycle) and excellent rate performance (613.1 mAh g−1 at 3 C). Significantly, the enhanced Li-S performances provide significant insight for realizing high performance Li-S batteries by incorporating the metal phosphides into the sulfur cathode.

A novel deionization technology was reported based on dual-ions electrochemistry technique, which possesses a stable salt removal capacity of 68.5 mg g⁻¹. The salt is removed during the discharge process, and thus the system is called “desalination generator”.

Abstract To flourish, cancers greatly depend on their surrounding tumor microenvironment (TME), and cancer-associated fibroblasts (CAFs) in TME are critical for cancer occurrence and progression because of their versatile roles in extracellular matrix remodeling, maintenance of stemness, blood vessel formation, modulation of tumor metabolism, immune response, and promotion of cancer cell proliferation, migration, invasion, and therapeutic resistance. CAFs are highly heterogeneous stromal cells and their crosstalk with cancer cells is mediated by a complex and intricate signaling network consisting of transforming growth factor-beta, phosphoinositide 3-kinase/AKT/mammalian target of rapamycin, mitogen-activated protein kinase, Wnt, Janus kinase/signal transducers and activators of transcription, epidermal growth factor receptor, Hippo, and nuclear factor kappa-light-chain-enhancer of activated B cells, etc., signaling pathways. These signals in CAFs exhibit their own special characteristics during the cancer progression and have the potential to be targeted for anticancer therapy. Therefore, a comprehensive understanding of these signaling cascades in interactions between cancer cells and CAFs is necessary to fully realize the pivotal roles of CAFs in cancers. Herein, in this review, we will summarize the enormous amounts of findings on the signals mediating crosstalk of CAFs with cancer cells and its related targets or trials. Further, we hypothesize three potential targeting strategies, including, namely, epithelial–mesenchymal common targets, sequential target perturbation, and crosstalk-directed signaling targets, paving the way for CAF-directed or host cell-directed antitumor therapy.

ZnGa₂O₄/SAPO-34 catalysed the direct conversion of CO₂ into lower olefins with 86% selectivity at 13% CO₂ conversion <italic>via</italic> a methanol intermediate.

Most of today's use of transition metal-catalyzed cross-coupling chemistry relies on expensive quantities of palladium (Pd). Here we report that nanoparticles formed from inexpensive FeCl3 that naturally contains parts-per-million (ppm) levels of Pd can catalyze Suzuki-Miyaura reactions, including cases that involve highly challenging reaction partners. Nanomicelles are employed to both solubilize and deliver the reaction partners to the Fe-ppm Pd catalyst, resulting in carbon-carbon bond formation. The newly formed catalyst can be isolated and stored at ambient temperatures. Aqueous reaction mixtures containing both the surfactant and the catalyst can be recycled.

A novel, ultra low-cost surface enhanced Raman spectroscopy (SERS) substrate has been developed by modifying the surface chemistry of cellulose paper and patterning nanoparticle arrays, all with a consumer inkjet printer. Micro/nanofabrication of SERS substrates for on-chip chemical and biomolecular analysis has been under intense investigation. However, the high cost of producing these substrates and the limited shelf life severely limit their use, especially for routine laboratory analysis and for point-of-sample analysis in the field. Paper-based microfluidic biosensing systems have shown great potential as low-cost disposable analysis tools. In this work, this concept is extended to SERS-based detection. Using an inexpensive consumer inkjet printer, cellulose paper substrates are modified to be hydrophobic in the sensing regions. Synthesized silver nanoparticles are printed onto this hydrophobic paper substrate with microscale precision to form sensing arrays. The hydrophobic surface prevents the aqueous sample from spreading throughout the paper and thus concentrates the analyte within the sensing region. A SERS fingerprint signal for Rhodamine 6G dye was observed for samples with as low as 10 femtomoles of analyte in a total sample volume of 1 μL. This extraordinarily simple technique can be used to construct SERS microarrays immediately before sample analysis, enabling ultra low-cost chemical and biomolecular detection in the lab as well as in the field at the point of sample collection.

Plastic wastes represent a largely untapped resource for manufacturing chemicals and fuels, particularly considering their environmental and biological threats. Here we report electrocatalytic upcycling of polyethylene terephthalate (PET) plastic to valuable commodity chemicals (potassium diformate and terephthalic acid) and H2 fuel. Preliminary techno-economic analysis suggests the profitability of this process when the ethylene glycol (EG) component of PET is selectively electrooxidized to formate (>80% selectivity) at high current density (>100 mA cm-2). A nickel-modified cobalt phosphide (CoNi0.25P) electrocatalyst is developed to achieve a current density of 500 mA cm-2 at 1.8 V in a membrane-electrode assembly reactor with >80% of Faradaic efficiency and selectivity to formate. Detailed characterizations reveal the in-situ evolution of CoNi0.25P catalyst into a low-crystalline metal oxy(hydroxide) as an active state during EG oxidation, which might be responsible for its advantageous performances. This work demonstrates a sustainable way to implement waste PET upcycling to value-added products.

Transplantation of bone marrow-derived mesenchymal stem cells (BMSCs) can promote functional recovery of brain after stroke with the mechanism regulating the BMSCs migration to ischemic penumbra poorly understood. Interaction between stromal cell-derived factor-1alpha (SDF-1alpha) and its cognate receptor CXCR4 is crucial for homing and migration of multiple stem cell types. Their potential role in mediating BMSC migration in ischemic brain has not been demonstrated. In this study, ischemic brain lesion model was created in rats by permanent middle cerebral artery occlusion and green fluorescent protein (GFP)-labeled BMSCs were intravenously injected. Immunohistochemical staining showed that BMSCs were able to enter the route from olfactory areas to cortex of the rat brain. Significant recovery of modified Neurological Severity Score was observed at days 14 and 28. Interestingly, the SDF-1alpha mRNA and protein were predominantly localized in the ischemic penumbral, peaked by 3-7 days and retained at least 14 days post-transplantation. On the other hand, the CXCR4 expression by BMSCs was elevated under hypoxia. The pre-treatment with the CXCR4-specific antagonist AMD3100 significantly prevented the migration of BMSCs to the injured brain. Taken together, these observations indicate that systemically administered BMSCs can migrate to the ischemic lesion of brain along with the olfactory-thalamus and hippocampus-cortex route. The interaction of locally produced SDF-1alpha and CXCR4 expressed on the BMSC surface plays an important role in the migration of transplanted cells, suggesting that it might be a potential approach to modulate the expression of the two molecules in order to further facilitate the therapeutic effects using BMSCs.

We demonstrate a paper-based surface swab and lateral-flow dipstick that includes an inkjet-printed surface-enhanced Raman spectroscopy (SERS) substrate for analyte detection. Due to capillary-action wicking of cellulose, the paper dipstick enables extremely simple and pump-free loading of liquid samples into the detection device, and in addition provides inherent analyte concentration within the detection volume. Furthermore, the flexible nature of the paper-based SERS device also enables it to act as a swab to collect analyte molecules directly from a large-area surface; the collected analyte molecules can then be focused into a small-volume SERS-active region by lateral-flow concentration. These capabilities are unseen in today's SERS substrates and microfluidic SERS devices. Using these novel lateral-flow paper SERS devices, we achieved detection limits as low as 95 fg of Rhodamine 6G (R6G), 413 pg of the organophosphate malathion, 9 ng of heroin, and 15 ng of cocaine. Moreover, the measurements show that the technique is quantitative and is repeatable across multiple swabs and dipsticks. The results reported here may lead to ultra-low-cost portable applications in trace chemical detection.

Label-free MoS2 nanosheet-based field-effect biosensor detects cancer marker protein Prostate Specific Antigen in real time with high sensitivity and selectivity, exhibiting great potential in point-of-care diagnostics application.

With the proliferation of smart grid research, the Advanced Metering Infrastructure (AMI) has become the first ubiquitous and fixed computing platform. However, due to the unique characteristics of AMI, such as complex network structure, resource-constrained smart meter, and privacy-sensitive data, it is an especially challenging issue to make AMI secure. Energy theft is one of the most important concerns related to the smart grid implementation. It is estimated that utility companies lose more than $25 billion every year due to energy theft around the world. To address this challenge, in this paper, we discuss the background of AMI and identify major security requirements that AMI should meet. Specifically, an attack tree based threat model is first presented to illustrate the energy-theft behaviors in AMI. Then, we summarize the current AMI energy-theft detection schemes into three categories, i.e., classification-based, state estimation-based, and game theory-based ones, and make extensive comparisons and discussions on them. In order to provide a deep understanding of security vulnerabilities and solutions in AMI and shed light on future research directions, we also explore some open challenges and potential solutions for energy-theft detection.

The activity of a ZrO2-supported nickel catalyst promoted by silica (Ni-Si/ZrO2) in CO2 dry reforming of methane was carried out at 400 and 450 °C. The catalysts were prepared by an impregnation method and characterized by H2-TPR, XRD, TEM, TG-MS, Raman, XPS, and in situ XPS and DRIFTS. It was discovered that Ni-Si/ZrO2 showed higher initial conversion of CH4 (0.50 s–1) and CO2 (0.44 s–1), and stability for low temperature (400 °C) DRM reaction in comparison to an SiO2-supported nickel catalyst promoted by zirconia (Ni-Zr/SiO2) (0.32 s–1 for both CO2 and CH4). The Ni-Si/ZrO2 catalyst featured the formation of active nickel particles with a small size of 6–9 nm and with slightly strong electronic donor ability, stabilization of the initial metal nickel state under the reaction conditions, and the formation of easily removed C1 coke. However, for the 450 °C DRM reaction, the coke that formed on the Ni-Si/ZrO2 catalyst was mainly C2 coke that was difficult to remove, because the CO2 preferred to combine with H species rather than react with the coke. For the Ni-Zr/SiO2 catalyst, the Ni0 species was oxidized to a NiO species under the reaction conditions at 400 °C and could not be restored, leading to its deactivation.

Propane dehydrogenation (PDH) has great potential to meet the increasing global demand for propylene, but the widely used Pt-based catalysts usually suffer from short-term stability and unsatisfactory propylene selectivity. Herein, we develop a ligand-protected direct hydrogen reduction method for encapsulating subnanometer bimetallic Pt-Zn clusters inside silicalite-1 (S-1) zeolite. The introduction of Zn species significantly improved the stability of the Pt clusters and gave a superhigh propylene selectivity of 99.3 % with a weight hourly space velocity (WHSV) of 3.6-54 h-1 and specific activity of propylene formation of 65.5 mol C3H6 gPt-1 h-1 (WHSV=108 h-1 ) at 550 °C. Moreover, no obvious deactivation was observed over PtZn4@S-1-H catalyst even after 13000 min on stream (WHSV=3.6 h-1 ), affording an extremely low deactivation constant of 0.001 h-1 , which is 200 times lower than that of the PtZn4/Al2 O3 counterpart under the same conditions. We also show that the introduction of Cs+ ions into the zeolite can improve the regeneration stability of catalysts, and the catalytic activity kept unchanged after four continuous cycles.

Photocatalytic activity in the reduction of CO2 with H2O to CH4 was significantly enhanced by simply adding MgO to TiO2 loaded with Pt. A positive correlation between CH4 formation activity and basicity was observed. The interface between TiO2, Pt and MgO in the trinary nanocomposite played a crucial role in CO2 photocatalytic reduction.

Gold takes to water: The synthesis of amides directly from alcohols and amines was realized by using a water-soluble Au/DNA nanohybrid as the catalyst. The interactions between the gold nanoparticles, DNA, and water lead to high catalytic efficiency under mild reaction conditions. The wide substrate scope includes less-basic aromatic amines, and this catalyst is recyclable. Detailed facts of importance to specialist readers are published as ”Supporting Information”. Such documents are peer-reviewed, but not copy-edited or typeset. They are made available as submitted by the authors. Please note: The publisher is not responsible for the content or functionality of any supporting information supplied by the authors. Any queries (other than missing content) should be directed to the corresponding author for the article.

High glycolysis, well known as “Warburg effect,” is frequently observed in a variety of cancers. Whether the deregulation of miRNAs contributes to the Warburg effect remains largely unknown. Because miRNA regulates gene expression at both mRNA and protein levels, we constructed a gene functional association network, which allows us to detect the gene activity instead of gene expression, to integratively analyze the microarray data for gene expression and miRNA expression profiling and identify glycolysis-related gene-miRNA pairs deregulated in cancer. Hexokinase 2 (HK2), coding for the first rate-limiting enzyme of glycolysis, is among the top list of genes predicted and potentially regulated by multiple miRNAs including miR-143. Interestingly, miR-143 expression was inversely associated with HK2 protein level but not mRNA level in human lung cancer samples. miR-143, down-regulated by mammalian target of rapamycin activation, reduces glucose metabolism and inhibits cancer cell proliferation and tumor formation through targeting HK2. Collectively, we have not only established a novel methodology for gene-miRNA pair prediction but also identified miR-143 as an essential regulator of cancer glycolysis via targeting HK2.Background: Hexokinase 2 (HK2) is frequently overexpressed in malignant tumors.Results: miR-143 down-regulates HK2 and inhibits glucose metabolism and cancer progression.Conclusion: miR-143 is an essential regulator of cancer glycolysis via targeting HK2.Significance: Discovering the important role of miRNA in cancer metabolism may provide potential targets for cancer therapy. High glycolysis, well known as “Warburg effect,” is frequently observed in a variety of cancers. Whether the deregulation of miRNAs contributes to the Warburg effect remains largely unknown. Because miRNA regulates gene expression at both mRNA and protein levels, we constructed a gene functional association network, which allows us to detect the gene activity instead of gene expression, to integratively analyze the microarray data for gene expression and miRNA expression profiling and identify glycolysis-related gene-miRNA pairs deregulated in cancer. Hexokinase 2 (HK2), coding for the first rate-limiting enzyme of glycolysis, is among the top list of genes predicted and potentially regulated by multiple miRNAs including miR-143. Interestingly, miR-143 expression was inversely associated with HK2 protein level but not mRNA level in human lung cancer samples. miR-143, down-regulated by mammalian target of rapamycin activation, reduces glucose metabolism and inhibits cancer cell proliferation and tumor formation through targeting HK2. Collectively, we have not only established a novel methodology for gene-miRNA pair prediction but also identified miR-143 as an essential regulator of cancer glycolysis via targeting HK2. Background: Hexokinase 2 (HK2) is frequently overexpressed in malignant tumors. Results: miR-143 down-regulates HK2 and inhibits glucose metabolism and cancer progression. Conclusion: miR-143 is an essential regulator of cancer glycolysis via targeting HK2. Significance: Discovering the important role of miRNA in cancer metabolism may provide potential targets for cancer therapy.

Herein, we report the successful application of hybrid Au-Ag nanoparticles (NPs) and nanochains (NCs) in the harvesting of visible light energy for selective hydrogenation reactions. For individual Au@Ag NPs with Au25 cores, the conversion and turnover frequency (TOF) are approximately 8 and 10 times higher than those of Au25 NPs, respectively. Notably, after the self-assembly of the Au@Ag NPs, the conversion and TOF of 1D NCs were approximately 2.5 and 2 times higher than those of isolated Au@Ag NPs, respectively, owing to the coupling of surface plasmon and the increase in the rate at which hot (energetic) electrons are generated with the formation of plasmonic hot spots between NPs. Furthermore, the surface-enhanced Raman scattering (SERS) activity of 1D Au@Ag NCs was strengthened by nearly 2 orders of magnitude.

Abstract The benefits of Zn, despite many of its performance advantages (e.g., high theoretical capacity and low redox potential), are compromised by severe side reactions and Zn dendrite growth in aqueous electrolytes, due to the coordinated H 2 O within the Zn 2+ ‐solvation sheath and reactive free water in the bulk electrolyte. Unlike most efforts focused on costly super‐concentrated electrolytes and single additive species, a universal strategy is proposed to boost Zn reversibility in dilute electrolytes via adding carbonyl‐containing organic solvents. Based on experimental investigations and multiscale simulations, the representative electrolyte with a N ‐methyl‐2‐pyrrolidone polar additive is proved to assist in structural reshaping of Zn 2+ ‐solvation and stabilizing the hydrogen bond network of water. This synergy is instrumental in contributing to suppressed water‐induced parasitic reactions and dendrite formation, which enables high average coulombic efficiency of 99.7% over 1000 cycles in an Zn/Cu asymmetric cell, and an ultralong cycling lifespan of 2000 cycles with 99.4% capacity retention in a Zn/VS 2 @SS full cell. Even with an elevated cathodic mass loading (up to 9.5 mg cm ‐2 ), the cycling stability is still maintained. The proposed strategy provides new insight into electrolyte additive design and sheds light on high‐performance Zn‐ion batteries.

Surface enhanced Raman spectroscopy (SERS) is a powerful spectroscopic technique capable of detecting trace amounts of chemicals and identifying them based on their unique vibrational characteristics. While there are many complex methods for fabricating SERS substrates, there has been a recent shift towards the development of simple, low cost fabrication methods that can be performed in most labs or even in the field. The potential of SERS for widespread use will likely be realized only with development of cheaper, simpler methods. In this Perspective article we briefly review several of the more popular methods for SERS substrate fabrication, discuss the characteristics of simple SERS substrates, and examine several methods for producing simple SERS substrates. We highlight potential applications and future directions for simple SERS substrates, focusing on highly SERS active three-dimensional nanostructures fabricated by inkjet and screen printing and galvanic displacement for portable SERS analysis – an area that we believe has exciting potential for future research and commercialization.

In western North America, the current outbreak of the mountain pine beetle (MPB) and its microbial associates has destroyed wide areas of lodgepole pine forest, including more than 16 million hectares in British Columbia. Grosmannia clavigera (Gc), a critical component of the outbreak, is a symbiont of the MPB and a pathogen of pine trees. To better understand the interactions between Gc, MPB, and lodgepole pine hosts, we sequenced the ∼30-Mb Gc genome and assembled it into 18 supercontigs. We predict 8,314 protein-coding genes, and support the gene models with proteome, expressed sequence tag, and RNA-seq data. We establish that Gc is heterothallic, and report evidence for repeat-induced point mutation. We report insights, from genome and transcriptome analyses, into how Gc tolerates conifer-defense chemicals, including oleoresin terpenoids, as they colonize a host tree. RNA-seq data indicate that terpenoids induce a substantial antimicrobial stress in Gc, and suggest that the fungus may detoxify these chemicals by using them as a carbon source. Terpenoid treatment strongly activated a ∼100-kb region of the Gc genome that contains a set of genes that may be important for detoxification of these host-defense chemicals. This work is a major step toward understanding the biological interactions between the tripartite MPB/fungus/forest system.

Multifunctional cotton fabrics have attracted significant attention as next-generation wearable materials. Herein, we report a facile method for the fabrication of flexible and wearable cotton fabrics with ultra-high electromagnetic interference (EMI) shielding, antibacterial, and superhydrophobic properties. Cotton fabrics were first coated chemically with silver nanoparticles using polydopamine as adhesive and then with hydrophobic polydimethylsiloxane or polyimide. The introduction of polydopamine significantly increased the bond between silver nanoparticles and cotton fibers, thereby preventing silver nanoparticles from falling off the surface. The composite fabrics exhibited a high conductivity of ~1000 S/cm, and their EMI shielding effectiveness increased up to ~110 dB. The composite fabrics exhibited excellent self-cleaning performance and acid-alkali corrosion resistance because of their superhydrophobicity. Notably, the fabric composites showed a significant antibacterial action against Staphylococcus aureus and Escherichia coli.

Miniaturized energy storage devices have attracted considerable research attention due to their promising applications such as power-on-chip units in various smart electronic devices. In this work, a printable micro-supercapacitor (MSC) device was designed and fabricated wherein a novel three dimensional (3D) nanocomposite consisting of cobalt oxide (CoO) nanoflowers woven with carbon nanotubes (CNTs) networks were used as the active material. The CoO/CNT nanocomposites were synthesized via a high-throughput hydrothermal method. High capacitance of 17.4 F/cm3 and energy density of ~3.48 mWh/cm3 were achieved for the CoO/CNT MSC at a current density of 0.25 A/cm3. The high volumetric energy density is attributed to the widened operation voltage window ranging from 0 to 1.2 V. Moreover, the printed CoO/CNT MSCs also showed remarkable cycling stability with ~85% energy density retention after 1700 cycles and high mechanical flexibility which can function well even after bending up to 180°. As a result, the printed CoO/CNT MSC is a possible contender in future energy storage devices for low-cost on-chip power applications.

The structure of alumina-supported copper–cobalt catalysts prepared by incipient co-impregnation was studied by using a combination of various characterization techniques including in situ XRD, XPS, TPR, XANES/EXAFS, in situ magnetic method, and TEM. The results suggest a much higher dispersion of copper than cobalt on γ-Al2O3 and a stronger interaction between cobalt and copper oxide particles, leading to the formation of mixed copper–cobalt oxides in the calcined catalysts. Cobalt reduction was significantly enhanced in the presence of copper. Furthermore, our characterizations indicate the formation of bimetallic Cu–Co particles in the reduced catalysts and enrichment of the surface of bimetallic particles with Cu. The catalytic studies showed dramatic modifications of both the rate and selectivity in the hydrogenation of CO after addition of even small amounts of Cu to supported Co catalysts. The presence of Cu increased the selectivity to alcohols by an order of magnitude and decreased the overall carbon monoxide conversion. Structure-performance correlations suggest that the Cu–Co bimetallic particles may be involved in higher alcohol synthesis.

In the search of alternative resources to make commodity chemicals and transportation fuels for a low carbon future, lignocellulosic biomass with over 180-billion-ton annual production rate has been identified as a promising feedstock. This review focuses on the state-of-the-art catalytic transformation of lignocellulosic biomass into value-added chemicals and fuels. Following a brief introduction on the structure, major resources and pretreatment methods of lignocellulosic biomass, the catalytic conversion of three main components, i.e., cellulose, hemicellulose and lignin, into various compounds are comprehensively discussed. Either in separate steps or in one-pot, cellulose and hemicellulose are hydrolyzed into sugars and upgraded into oxygen-containing chemicals such as 5-HMF, furfural, polyols, and organic acids, or even nitrogen-containing chemicals such as amino acids. On the other hand, lignin is first depolymerized into phenols, catechols, guaiacols, aldehydes and ketones, and then further transformed into hydrocarbon fuels, bioplastic precursors and bioactive compounds. The review then introduces the transformations of whole biomass via catalytic gasification, catalytic pyrolysis, as well as emerging strategies. Finally, opportunities, challenges and prospective of woody biomass valorization are highlighted.

More than a decade since its inception, the benefits and cost efficiency of robot-assisted radical prostatectomy (RARP) continue to elicit controversy. To compare outcomes and costs between RARP and open RP (ORP). A cohort study of 629 593 men who underwent RP for localized prostate cancer at 449 hospitals in the USA from 2003 to 2013, using the Premier Hospital Database. RARP was ascertained through a review of the hospital charge description master for robotic supplies. Outcomes were 90-d postoperative complications (Clavien), blood product transfusions, operating room time (ORT), length of stay (LOS), and direct hospital costs. Propensity-weighted regression analyses accounting for clustering by hospitals and survey weighting ensured nationally representative estimates. RARP utilization rapidly increased from 1.8% in 2003 to 85% in 2013 (p < 0.001). RARP patients (n = 311 135) were less likely to experience any complications (odds ratio [OR] 0.68, p < 0.001) or prolonged LOS (OR 0.28, p < 0.001), or to receive blood products (OR 0.33, p = 0.002) compared to ORP patients (n = 318 458). The adjusted mean ORT was 131 min longer for RARP (p = 0.002). The 90-d direct hospital costs were higher for RARP (+$4528, p < 0.001), primarily attributed to operating room and supplies costs. Costs were no longer signficantly different between ORP and RARP among the highest-volume surgeons (≥104 cases/yr; +$1990, p = 0.40) and highest-volume hospitals (≥318 cases/yr; +$1225, p = 0.39). Limitations include the lack of oncologic characteristics and the retrospective nature of the study. Our contemporary analysis reveals that RARP confers a perioperative morbidity advantage at higher cost. In the absence of large randomized trials because of the widespread adoption of RARP, this retrospective study represents the best available evidence for the morbidity and cost profile of RARP versus ORP. In this large study of men with prostate cancer who underwent either open or robotic radical prostatectomy, we found that robotic surgery has a better morbidity profile but costs more.

<h3>Importance</h3> Use of robotic surgery has increased in urological practice over the last decade. However, the use, outcomes, and costs of robotic nephrectomy are unknown. <h3>Objectives</h3> To examine the trend in use of robotic-assisted operations for radical nephrectomy in the United States and to compare the perioperative outcomes and costs with laparoscopic radical nephrectomy. <h3>Design, Setting, and Participants</h3> This retrospective cohort study used the Premier Healthcare database to evaluate outcomes of patients who had undergone robotic-assisted or laparoscopic radical nephrectomy for renal mass at 416 US hospitals between January 2003 and September 2015. Multivariable regression modeling was used to assess outcomes. <h3>Exposures</h3> Robotic-assisted vs laparoscopic radical nephrectomy. <h3>Main Outcomes and Measures</h3> The primary outcome of the study was the trend in use of robotic-assisted radical nephrectomy. The secondary outcomes were perioperative complications, based on the Clavien classification system, and defined as any complication (Clavien grades 1-5) or major complications (Clavien grades 3-5, for which grade 5 results in death); resource use (operating time, blood transfusion, length of hospital stay); and direct hospital cost. <h3>Results</h3> Among 23 753 patients included in the study (mean age, 61.4 years; men, 13 792 [58.1%]), 18 573 underwent laparoscopic radical nephrectomy and 5180 underwent robotic-assisted radical nephrectomy. Use of robotic-assisted surgery increased from 1.5% (39 of 2676 radical nephrectomy procedures in 2003) to 27.0% (862 of 3194 radical nephrectomy procedures) in 2015 (<i>P</i>for trend &lt;.001). In the weighted-adjusted analysis, there were no significant differences between robotic-assisted and laparoscopic radical nephrectomy in the incidence of any (Clavien grades 1-5) postoperative complications (adjusted rates, 22.2% vs 23.4%, difference, −1.2%; 95% CI, −5.4 to 3.0%) or major (Clavien grades 3-5) complications (adjusted rates, 3.5% vs 3.8%, difference, −0.3%; 95% CI, −1.0% to 0.5%). The rate of prolonged operating time (&gt;4 hours) for patients undergoing the robotic-assisted procedure was higher than for patients receiving the laparoscopic procedure in the adjusted analysis (46.3% vs 25.8%; risk difference, 20.5%; 95% CI, 14.2% to 26.8%). Robotic-assisted radical nephrectomy was associated with higher mean 90-day direct hospital costs ($19 530 vs $16 851; difference, $2678; 95% CI, $838 to $4519), mainly accounted for operating room ($7217 vs $5378; difference, $1839; 95% CI, $1050 to $2628) and supply costs ($4876 vs $3891; difference, $985; 95% CI, $473 to $1498). <h3>Conclusions and Relevance</h3> Among patients undergoing radical nephrectomy for renal mass between 2003 and 2015, the use of robotic-assisted surgery increased substantially. The use of robotic-assistance was not associated with increased risk of any or major complications but was associated with prolonged operating time and higher hospital costs compared with laparoscopic surgery.

The hydrogenation of carbon dioxide to lower (C2–C4) olefins is an important reaction for the utilization of CO2 as a carbon feedstock for the production of building-block chemicals. We found that an Fe/ZrO2 catalyst could catalyze the hydrogenation of CO2, but the main products were CH4 and lower (C2–C4) paraffins. The modification of the Fe/ZrO2 catalyst by alkali metal ions except for Li+ significantly decreased the selectivities to CH4 and lower paraffins and increased those to lower olefins and C5+ hydrocarbons, particularly C5+ olefins. The modification by Na+, K+, or Cs+ also increased the conversion of CO2. The best performance for lower olefin synthesis was obtained over the K+-modified Fe/ZrO2 catalyst with a proper K+ content (0.5–1.0 wt%). Among several typical supports including SiO2, Al2O3, TiO2, ZrO2, mesoporous carbon, and carbon nanotube, ZrO2 provided the highest selectivity and yield to lower olefins. Our characterizations suggest that the modification by K+ accelerates the generation of χ-Fe5C2 phase under the reaction conditions. This together with the decreased hydrogenation ability in the presence of K+ has been proposed to be responsible for the enhanced selectivity to lower olefins.

A novel asymmetric supercapacitor composed of Co₃O₄@C@Ni₃S₂ NNAs as the positive electrode and activated carbon (AC) as the negative electrode can deliver a high energy density and excellent long cycle stability.

Amino acids are the building blocks for protein biosynthesis and find use in myriad industrial applications including in food for humans, in animal feed, and as precursors for bio-based plastics, among others. However, the development of efficient chemical methods to convert abundant and renewable feedstocks into amino acids has been largely unsuccessful to date. To that end, here we report a heterogeneous catalyst that directly transforms lignocellulosic biomass-derived α-hydroxyl acids into α-amino acids, including alanine, leucine, valine, aspartic acid, and phenylalanine in high yields. The reaction follows a dehydrogenation-reductive amination pathway, with dehydrogenation as the rate-determining step. Ruthenium nanoparticles supported on carbon nanotubes (Ru/CNT) exhibit exceptional efficiency compared with catalysts based on other metals, due to the unique, reversible enhancement effect of NH3 on Ru in dehydrogenation. Based on the catalytic system, a two-step chemical process was designed to convert glucose into alanine in 43% yield, comparable with the well-established microbial cultivation process, and therefore, the present strategy enables a route for the production of amino acids from renewable feedstocks. Moreover, a conceptual process design employing membrane distillation to facilitate product purification is proposed and validated. Overall, this study offers a rapid and potentially more efficient chemical method to produce amino acids from woody biomass components.

Abstract Multiple cotton genomes (diploid and tetraploid) have been assembled. However, genomic variations between cultivars of allotetraploid upland cotton ( Gossypium hirsutum L.), the most widely planted cotton species in the world, remain unexplored. Here, we use single-molecule long read and Hi-C sequencing technologies to assemble genomes of the two upland cotton cultivars TM-1 and zhongmiansuo24 (ZM24). Comparisons among TM-1 and ZM24 assemblies and the genomes of the diploid ancestors reveal a large amount of genetic variations. Among them, the top three longest structural variations are located on chromosome A08 of the tetraploid upland cotton, which account for ~30% total length of this chromosome. Haplotype analyses of the mapping population derived from these two cultivars and the germplasm panel show suppressed recombination rates in this region. This study provides additional genomic resources for the community, and the identified genetic variations, especially the reduced meiotic recombination on chromosome A08, will help future breeding.

Transformation of syngas (H2/CO) and hydrogenation of CO2 into lower olefins are attractive routes for chemical utilization of various carbon resources and CO2, but both suffer from limited product selectivity. Tandem catalysis that integrates the activation of CO or CO2 to an intermediate and the subsequent controllable C–C bond formation to form lower olefins offers a promising approach. Here, we report the hydrogenation of both CO and CO2 over bifunctional catalysts composed of a spinel binary metal oxide and SAPO-34. ZnAl2O4/SAPO-34 and ZnGa2O4/SAPO-34 are found to be highly selective for the synthesis of lower olefins from both CO and CO2. Our studies reveal that the oxygen vacancy site on metal oxides plays a pivotal role in the adsorption and activation of CO or CO2, while the −Zn–O– domain accounts for H2 activation. We demonstrate that methanol and dimethyl ether formed on metal oxide are the reaction intermediates, which are subsequently converted to lower olefins by the Brønsted acid sites in zeolite. The hydrogenation of CO and CO2 on metal oxide surfaces proceeds via the same formate and methoxide species. We elucidate that the water–gas shift reaction on oxide surfaces is responsible for CO2 formation during syngas conversion. The cofeeding of CO2 in syngas offers a useful strategy to inhibit CO2 formation.

Abstract The combination of CDK4/6 inhibitors with antiestrogen therapies significantly improves clinical outcomes in ER-positive advanced breast cancer. To identify mechanisms of acquired resistance, we analyzed serial biopsies and rapid autopsies from patients treated with the combination of the CDK4/6 inhibitor ribociclib with letrozole. This study revealed that some resistant tumors acquired RB loss, whereas other tumors lost PTEN expression at the time of progression. In breast cancer cells, ablation of PTEN, through increased AKT activation, was sufficient to promote resistance to CDK4/6 inhibition in vitro and in vivo. Mechanistically, PTEN loss resulted in exclusion of p27 from the nucleus, leading to increased activation of both CDK4 and CDK2. Because PTEN loss also causes resistance to PI3Kα inhibitors, currently approved in the post-CDK4/6 setting, these findings provide critical insight into how this single genetic event may cause clinical cross-resistance to multiple targeted therapies in the same patient, with implications for optimal treatment-sequencing strategies. Significance: Our analysis of serial biopsies uncovered RB and PTEN loss as mechanisms of acquired resistance to CDK4/6 inhibitors, utilized as first-line treatment for ER-positive advanced breast cancer. Importantly, these findings have near-term clinical relevance because PTEN loss also limits the efficacy of PI3Kα inhibitors currently approved in the post-CDK4/6 setting. This article is highlighted in the In This Issue feature, p. 1

Abstract The biomass‐derived alcohol oxidation reaction (BDAOR) holds great promise for sustainable production of chemicals. However, selective electrooxidation of alcohols to value‐added aldehyde compounds is still challenging. Herein, we report the electrocatalytic BDAORs to selectively produce aldehydes using single‐atom ruthenium on nickel oxide (Ru 1 ‐NiO) as a catalyst in the neutral medium. For electrooxidation of 5‐hydroxymethylfurfural (HMF), Ru 1 ‐NiO exhibits a low potential of 1.283 V at 10 mA cm −2 , and an optimal 2,5‐diformylfuran (DFF) selectivity of 90 %. Experimental studies reveal that the neutral electrolyte plays a critical role in achieving a high aldehyde selectivity, and the single‐atom Ru boosts HMF oxidation in the neutral medium by promoting water dissociation to afford OH*. Furthermore, Ru 1 ‐NiO can be extended to selective electrooxidation of a series of biomass‐derived alcohols to corresponding aldehydes, which are conventionally difficult to obtain in the alkaline medium.

Current influenza vaccines provide limited protection against circulating influenza A viruses. A universal influenza vaccine will eliminate the intrinsic limitations of the seasonal flu vaccines. Here we report methodology to generate double-layered protein nanoparticles as a universal influenza vaccine. Layered nanoparticles are fabricated by desolvating tetrameric M2e into protein nanoparticle cores and coating these cores by crosslinking headless HAs. Representative headless HAs of two HA phylogenetic groups are constructed and purified. Vaccinations with the resulting protein nanoparticles in mice induces robust long-lasting immunity, fully protecting the mice against challenges by divergent influenza A viruses of the same group or both groups. The results demonstrate the importance of incorporating both structure-stabilized HA stalk domains and M2e into a universal influenza vaccine to improve its protective potency and breadth. These potent disassemblable protein nanoparticles indicate a wide application in protein drug delivery and controlled release.

The deep ultraviolet photodetectors based on 2D h-BN show a high on/off ratio of &gt;10³ and good spectral selectivity.

A Co₃O₄@Co₃S₄ nanoarray electrode is designed by a facile solution synthesis approach and investigated as a cathode material for an ASC.

Realizing a long coherence time quantum memory is a major challenge of current quantum technology. Here, we report a single \Yb ion-qubit memory with over one hour coherence time, an order of improvement compared to the state-of-the-art record. The long coherence time memory is realized by addressing various technical challenges such as ambient magnetic-field noise, phase noise and leakage of the microwave oscillator. Moreover, systematically study the decoherence process of our quantum memory by quantum process tomography, which enables to apply the strict criteria of quantum coherence, relative entropy of coherence. We also benchmark our quantum memory by its ability in preserving quantum information, i.e., the robustness of quantum memory, which clearly shows that over 6000 s, our quantum memory preserves non-classical quantum information. Our results verify the stability of the quantum memory in hours level and indicate its versatile applicability in various scenarios.

The inert chemical property of RNA modification N6-methyladenosine (m6A) makes it very challenging to detect. Most m6A sequencing methods rely on m6A-antibody immunoprecipitation and cannot distinguish m6A and N6,2'-O-dimethyladenosine modification at the cap +1 position (cap m6Am). Although the two antibody-free methods (m6A-REF-seq/MAZTER-seq and DART-seq) have been developed recently, they are dependent on m6A sequence or cellular transfection. Here, we present an antibody-free, FTO-assisted chemical labeling method termed m6A-SEAL for specific m6A detection. We applied m6A-SEAL to profile m6A landscapes in humans and plants, which displayed the known m6A distribution features in transcriptome. By doing a comparison with all available m6A sequencing methods and specific m6A sites validation by SELECT, we demonstrated that m6A-SEAL has good sensitivity, specificity and reliability for transcriptome-wide detection of m6A. Given its tagging ability and FTO's oxidation property, m6A-SEAL enables many applications such as enrichment, imaging and sequencing to drive future functional studies of m6A and other modifications.

Efficient and stable inorganic lead-free halide perovskites have attracted tremendous attention for next-generation solid-state lighting. However, single perovskite phosphors with strong, tunable-color-temperature white-light emission are rare. Here, a doping strategy was developed to incorporate Sb3+ and Bi3+ ions into Cs2NaInCl6 single crystals. Blue and yellow emission for white light with a 77% quantum yield was observed. The dual-emission originates from different [SbCl6]3– octahedron-related self-trapped excitons (STEs). The blue emission is attributable to limited Jahn–Teller deformation from Sb3+ doping. Large-radii Bi3+ increase the deformation level of the [SbCl6]3– octahedron, enhancing yellow STE emission. Density functional theory calculations indicated that the Bi3+ doping forms a sub-band level, which produces yellow STE emission. Tuning between warm and cold white light can be realized by changing the Sb3+/Bi3+ doping ratio, which suggests a unique interaction mechanism between Sb3+ and Bi3+ dopants, as well as Bi3+-induced lattice distortion in double perovskites.

Manipulating surface organic ligands has emerged as a useful strategy to enhance the efficiency of heterogeneous catalysts. However, ligand-controlled catalysis for biomass valorization remains unexplored because of the limited knowledge of the ligand functions in heterogeneous catalytic systems involving macromolecules. Here, we report a strong dependence of photocatalytic conversion of native lignin into high-value functionalized aromatics on the ligand attached on cadmium sulfide quantum dots (QDs). The formation of a QD colloidal solution by tuning the hydrophilicity/hydrophobicity of ligands is essential to enable intimate contact between QDs and lignin, leading to high catalytic activity. The surface engineering by manipulating the anchor group and the length of ligands demonstrates that the ligand participates in the electron-transfer process, a crucial step of photocatalysis. The electron decay kinetic study reveals a ligand-mediated electron-tunneling mechanism. These insights offer useful guidance for the design of efficient QD photocatalysts for biomass valorization through ligand modification.

Abstract Although carbon itself acts as a catalyst in various reactions, the classical carbon materials (e.g., activated carbons, carbon aerogels, carbon black, carbon fiber, etc.) usually show low activity, stability, and oxidation resistance. With the recent availability of nanocarbon catalysts, the application of carbon materials in catalysis has gained a renewed momentum. The research is concentrated on tailoring the surface chemistry of nanocarbon materials, since the pristine carbons in general are not active for heterogeneous catalysis. Surface functionalization, doping with heteroatoms, and creating defects are the most used strategies to make efficient catalysts. However, the nature of the catalytic active sites and their role in determining the activity and selectivity is still not well understood. Herein, the types of active sites reported for several mainstream nanocarbons, including carbon nanotubes, graphene‐based materials, and 3D porous nanocarbons, are summarized. Knowledge about the active sites will be beneficial for the design and synthesis of nanocarbon catalysts with improved activity, selectivity, and stability.

We summarize the progress in organic–inorganic hybrid and all-inorganic wide- E g perovskite solar cells. Key challenges and effective strategies are discussed, followed by applications in tandems. We outline perspectives to design superior devices.

2D metal-organic frameworks (2D-MOFs) have recently emerged as promising materials for gas separations, sensing, conduction, and catalysis. However, the stability of these 2D-MOF catalysts and the tunability over catalytic environments are limited. Herein, it is demonstrated that 2D-MOFs can act as stable and highly accessible catalyst supports by introducing more firmly anchored photosensitizers as bridging ligands. An ultrathin MOF nanosheet-based material, Zr-BTB (BTB = 1,3,5-tris(4-carboxyphenyl)benzene), is initially constructed by connecting Zr6-clusters with the tritopic carboxylate linker. Surface modification of the Zr-BTB structure was realized through the attachment of porphyrin-based carboxylate ligands on the coordinatively unsaturated Zr metal sites in the MOF through strong Zr-carboxylate bond formation. The functionalized MOF nanosheet, namely PCN-134-2D, acts as an efficient photocatalyst for 1O2 generation and artemisinin production. Compared to the 3D analogue (PCN-134-3D), PCN-134-2D allows for fast reaction kinetics due to the enhanced accessibility of the catalytic sites within the structure and facile substrate diffusion. Additionally, PCN-134(Ni)-2D exhibits an exceptional yield of artemisinin, surpassing all reported homo- or heterogeneous photocatalysts for the artemisinin production.

It is highly desirable to discover MOFs matrix composites with controlled reduction selectivity in the general understanding of the CO2 reduction reaction (CO2RR) in electro- and photocatalytic process. Herein, we demonstrate a facile strategy to prepare metal organic framework hybrid composites (xCMC) using the Co-based MOF [Co2(TMTA)(HCOO)(bidb)(H2O)]∙DMF (H3TMTA = 1,3,5-trimethyl-2,4,6- tricarboxyl- phenylbenzene, bidb = 1,4-bis(1-imidazoly)benzene) and nanocrystalline cuprous oxide. The resulting hybrid catalyst with p-n heterojunction exhibited enhanced photocatalytic CO2 reduction activity with remarkable CO production rate of 3.83 μmol g−1h−1, ca. 9.6 times higher than that of pure Cu2O. Compared with other reaction routes, the present photocatalytic reduction of CO2 with superior selectivity to CO occurs in the interface of solid–gas reaction without the use of photosensitizers or sacrificing reagents. In addition, the mechanism for photocatalytic CO2 reduction was also well discussed. The present work provides unique insight into constructing MOF-based photocatalysts with heterojunction for visible-light-driven CO2 reduction under solid–gas reaction conditions.

Thermal management plays an important role in battery modules, especially under extreme operating conditions. Phase change materials (PCMs)-based cooling has been recognized as a promising approach that can prolong the life span of batteries and endure the passive thermal accumulation in the module. In this study, various mass fractions (0 wt%, 5 wt%, 10 wt%, 15 wt%, 20 wt%, and 25 wt%) of aluminum nitride (AlN) were added to composite PCMs to serve as heat-transfer promoters. The effect of the AlN additives on the thermal conductivity, mechanical properties, and volume resistivity were analyzed, and the root causes originating from the morphologies and structures of the composite PCMs were further examined. The results indicated that adding 20 wt% of the AlN in the composite PCMs was an optimal strategy. In addition, an AlN/paraffin (PA)/expanded graphite (EG)/epoxy resin composite PCMs-based 18650 LiFePO4 battery module was designed for thermal management. This battery module exhibited much better heat dissipation and temperature uniformity than an air-cooled battery module, leading to a 19.4% decrease of the maximum temperature and a less than 1 °C temperature difference at a high discharge rate of 3C. Thus, it could be concluded that the AlN-enhanced composite PCMs thermal management system exhibited a prominent controlling temperature and balancing temperature capacity for the battery module.

Irrigated agriculture has important implications for achieving the United Nations Sustainable Development Goals. However, there is a lack of systematic and quantitative analyses of its impacts on food-energy-water-CO2 nexus. Here we studied impacts of irrigated agriculture on food-energy-water-CO2 nexus across food sending systems (the North China Plain (NCP)), food receiving systems (the rest of China) and spillover systems (Hubei Province, affected by interactions between sending and receiving systems), using life cycle assessment, model scenarios, and the framework of metacoupling (socioeconomic-environmental interactions within and across borders). Results indicated that food supply from the NCP promoted food sustainability in the rest of China, but the NCP consumed over four times more water than its total annual renewable water, with large variations in food-energy-water-CO2 nexus across counties. Although Hubei Province was seldom directly involved in the food trade, it experienced substantial losses in water and land due to the construction of the South-to-North Water Transfer Project which aims to alleviate water shortages in the NCP. This study suggests the need to understand impacts of agriculture on food-energy-water-CO2 nexus in other parts of the world to achieve global sustainability.

Abstract: Berberine (BBR) has been extensively studied in vivo and vitro experiments. BBR inhibits cell proliferation by regulating cell cycle and cell autophagy, and promoting cell apoptosis. BBR also inhibits cell invasion and metastasis by suppressing EMT and down-regulating the expression of metastasis-related proteins and signaling pathways. In addition, BBR inhibits cell proliferation by interacting with microRNAs and suppressing telomerase activity. BBR exerts its anti-inflammation and antioxidant properties, and also regulates tumor microenvironment. This review emphasized that BBR as a potential anti-inflammation and antioxidant agent, also as an effective immunomodulator, is expected to be widely used in clinic for cancer therapy. Keywords: berberine, anti-tumor, traditional Chinese medicine, cancer

Metallic sodium is a promising anode material due to its remarkably high theoretical capacity (1165 mA h g−1) and favorable redox voltage (−2.71 V versus the standard hydrogen electrode). However, unstable solid-electrolyte-interface (SEI) film and uncontrollable dendritic sodium formation induce low Coulombic efficiency, inferior cycling performance and even severe safety issues, dragging the sodium metal anode out of practical applications. Recently, the reviving of lithium metal and application of related characterization techniques bring a new era of the alkali metal anode. Carbonaceous materials have been employed as the interface engineering layer or the host of sodium metal. The advantageous of carbon nanostructure are including high mechanical strength, low weight, high conductivity, various nanoarchitecture, large surface area, easy functionalization, and sustainable. With these merits, sodium metal is guided and uniformly deposited into/through carbon nanostructures without dendrite formation as the stable sodium metal anode. In this review, we summarize the recent progress in the strategies of suppressing the dendritic sodium by carbon nanostructures, and comprehensively analysis the related dendrite depression mechanism. We expect that this work can provide important insights into scientific and practical application of sodium metal batteries.

This paper investigates interval estimation methods for discrete-time linear time-invariant systems. We propose a novel interval estimation method by integrating robust observer design with reachability analysis. By introducing <inline-formula xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink"><tex-math notation="LaTeX">$H_{\infty }$</tex-math></inline-formula> design into interval estimation, the proposed method is effective in improving the accuracy of interval estimation. Moreover, the comparisons and relationships between the existing methods and the proposed method are discussed in detail. Finally, simulation results are presented to demonstrate the effectiveness of the proposed method.

In situ Raman spectroscopy is a powerful technique for probing the structure and phase composition of the electrode materials that are undergoing charge-discharge process. Herein, the charge storage mechanism of as-prepared Ni(HCO3)2 nanomaterial is successfully studied by using the in situ Raman spectroscopy. The charge storage can be attributed to the deep oxidation of Ni2+ into Ni3+, and the irreversible phase transformation of γ-NiOOH into disordered β-Ni(OH)2 damages the crystal structure of Ni(HCO3)2, arousing the capacity loss of the electrode during the long-term cycling process. Under the guidance of the experimental investigations, a porous Ni(HCO3)2/reduced graphene oxide (rGO) nanocomposite is designed and synthesized, exhibiting ultrahigh specific capacity (846 C g−1) and excellent rate capability (618 C g−1 at 20 A g−1). When coupled with an negative electrode based on rGO, the resulting hybrid supercapacitor shows an ultrahigh energy density of 66 Wh kg−1 at power density of 1.9 kW kg−1 and good cycling stability. These findings provide important insight into the mechanism of charge storage, and scientific basis for design of high-performance energy storage materials.

Abstract Micro/nanoprocessing of graphene surfaces has attracted significant interest for both science and applications due to its effective modulation of material properties, which, however, is usually restricted by the disadvantages of the current fabrication methods. Here, by exploiting cylindrical focusing of a femtosecond laser on graphene oxide (GO) films, we successfully produce uniform subwavelength grating structures at high speed along with a simultaneous in situ photoreduction process. Strikingly, the well-defined structures feature orientations parallel to the laser polarization and significant robustness against distinct perturbations. The proposed model and simulations reveal that the structure formation is based on the transverse electric (TE) surface plasmons triggered by the gradient reduction of the GO film from its surface to the interior, which eventually results in interference intensity fringes and spatially periodic interactions. Further experiments prove that such a regular structured surface can cause enhanced optical absorption (&gt;20%) and an anisotropic photoresponse (~0.46 ratio) for the reduced GO film. Our work not only provides new insights into understanding the laser-GO interaction but also lays a solid foundation for practical usage of femtosecond laser plasmonic lithography, with the prospect of expansion to other two-dimensional materials for novel device applications.

Photocatalysis and electrocatalysis have been emerging as important methods for the transformation of abundant C1 molecules into high-value C₂₊compounds.

It is highly desirable to achieve solar-driven conversion of CO2 to valuable fuels with controlled selectivity. The existing catalysts are mainly explored for CO production but rarely for formate generation. Herein, highly selective photoreduction of CO2 to formate (99.7%) was achieved with a high yield of 3040 μmol g–1 in 10 h by hierarchical integration of photosensitizers and monometallic [bpy-Cu/ClX] (X = Cl or adenine) catalysts into a stable Eu-bpy metal–organic framework. However, replacing X with pyridine in [bpy-CuCl/X] significantly reduced formate production while increasing the CO yield to 960 μmol g–1. Systematic investigations revealed that the catalytic process is mediated by the H-bond synergy between Cu-bound X and CO2-derived species, and the selectivity of HCOO– can be controlled by simply replacing the coordination ligands. This work provides a molecularly precise structural model to provide mechanistic insights for selectivity control of CO2 photoreduction.

Developing an excellent photocatalysis system to remove pesticides from water is an urgent problem in current environment purification field. Herein, a Z-scheme WO3/g-C3N4 photocatalyst was prepared by a facile in-situ calcination method, and the photocatalytic activity was investigated for degradation of nitenpyram (NTP) under visible light. The optimal Z-scheme WO3/g-C3N4 photocatalyst displayed the highest rate constant (0.036 min−1), which is about 1.7 and 25 times higher than that of pure g-C3N4 and WO3, respectively. The improvement of photocatalytic performance is attributed to fast transfer of photogenerated carriers in the Z-scheme structure, which are testified by electron spin resonance (ESR) experiments, photocurrent and electrochemical impedance spectra (EIS) measurements. Moreover, the effects of typical water environmental factors on the degradation NTP were systematically studied. And the possible degradation pathways of NTP were deduced by the intermediates detected by high-performance liquid chromatography-mass spectrometry (HPLC-MS). This work will not only contribute to understand the degradation mechanism of pesticides in real water environmental condition, but also promote the development of new technologies for pesticide pollution control as well as environmental remediation.

Abstract Low‐bandgap mixed tin–lead perovskite solar cells (PSCs) have been attracting increasing interest due to their appropriate bandgaps and promising application to build efficient all‐perovskite tandem cells, an effective way to break the Shockley–Queisser limit of single‐junction cells. Tin fluoride (SnF 2 ) has been widely used as a basis along with various strategies to improve the optoelectronic properties of low‐bandgap SnPb perovskites and efficient cells. However, fully understanding the roles of SnF 2 in both films and devices is still lacking and fundamentally desired. Here, the functions of SnF 2 in both low‐bandgap (FASnI 3 ) 0.6 (MAPbI 3 ) 0.4 perovskite films and efficient devices are unveiled. SnF 2 regulates the growth mode of low‐bandgap SnPb perovskite films, leading to highly oriented topological growth and improved crystallinity. Meanwhile, SnF 2 prevents the oxidation of Sn 2+ to Sn 4+ and reduces Sn vacancies, leading to reduced background hole density and defects, and improved carrier lifetime, thus largely decreasing nonradiative recombination. Additionally, the F − ion preferentially accumulates at hole transport layer/perovskite interface with high SnF 2 content, leading to more defects. This work provides in‐depth insights into the roles of SnF 2 additives in low‐bandgap SnPb films and devices, assisting in further investigations into multiple additives and approaches to obtain efficient low‐bandgap PSCs.

<h2>Summary</h2><h3>Background & aims</h3> In the newly emerged Coronavirus Disease 2019 (COVID-19) disaster, little is known about the nutritional risks for critically ill patients. It is also unknown whether the modified Nutrition Risk in the Critically ill (mNUTRIC) score is applicable for nutritional risk assessment in intensive care unit (ICU) COVID-19 patients. We set out to investigate the applicability of the mNUTRIC score for assessing nutritional risks and predicting outcomes for these critically ill COVID-19 patients. <h3>Methods</h3> This retrospective observational study was conducted in three ICUs which had been specially established and equipped for COVID-19 in Wuhan, China. The study population was critically ill COVID-19 patients who had been admitted to these ICUs between January 28 and February 21, 2020. Exclusion criteria were as follows: 1) patients of <18 years; 2) patients who were pregnant; 3) length of ICU stay of <24 h; 4) insufficient medical information available. Patients' characteristics and clinical information were obtained from electronic medical and nursing records. The nutritional risk for each patient was assessed at their ICU admission using the mNUTRIC score. A score of ≥5 indicated high nutritional risk. Mortality was calculated according to patients' outcomes following 28 days of hospitalization in ICU. <h3>Results</h3> A total of 136 critically ill COVID-19 patients with a median age of 69 years (IQR: 57–77), 86 (63%) males and 50 (37%) females, were included in the study. Based on the mNUTRIC score at ICU admission, a high nutritional risk (≥5 points) was observed in 61% of the critically ill COVID-19 patients, while a low nutritional risk (<5 points) was observed in 39%. The mortality of ICU 28-day was significantly higher in the high nutritional risk group than in the low nutritional risk group (87% vs 49%, <i>P</i> <0.001). Patients in the high nutritional risk group exhibited significantly higher incidences of acute respiratory distress syndrome, acute myocardial injury, secondary infection, shock and use of vasopressors. Additionally, use of a multivariate Cox analysis showed that patients with high nutritional risk had a higher probability of death at ICU 28-day than those with low nutritional risk (adjusted HR = 2.01, 95% CI: 1.22–3.32, <i>P</i> = 0.006). <h3>Conclusions</h3> A large proportion of critically ill COVID-19 patients had a high nutritional risk, as revealed by their mNUTRIC score. Patients with high nutritional risk at ICU admission exhibited significantly higher mortality of ICU 28-day, as well as twice the probability of death at ICU 28-day than those with low nutritional risk. Therefore, the mNUTRIC score may be an appropriate tool for nutritional risk assessment and prognosis prediction for critically ill COVID-19 patients.

A patient's response to immune checkpoint inhibitors (ICIs) is a complex quantitative trait, and determined by multiple intrinsic and extrinsic factors. Three currently FDA-approved predictive biomarkers (progra1mmed cell death ligand-1 (PD-L1); microsatellite instability (MSI); tumor mutational burden (TMB)) are routinely used for patient selection for ICI response in clinical practice. Although clinical utility of these biomarkers has been demonstrated in ample clinical trials, many variables involved in using these biomarkers have poised serious challenges in daily practice. Furthermore, the predicted responders by these three biomarkers only have a small percentage of overlap, suggesting that each biomarker captures different contributing factors to ICI response. Optimized use of currently FDA-approved biomarkers and development of a new generation of predictive biomarkers are urgently needed. In this review, we will first discuss three widely used FDA-approved predictive biomarkers and their optimal use. Secondly, we will review four novel gene signature biomarkers: T-cell inflamed gene expression profile (GEP), T-cell dysfunction and exclusion gene signature (TIDE), melanocytic plasticity signature (MPS) and B-cell focused gene signature. The GEP and TIDE have shown better predictive performance than PD-L1, and PD-L1 or TMB, respectively. The MPS is superior to PD-L1, TMB, and TIDE. The B-cell focused gene signature represents a previously unexplored predictive biomarker to ICI response. Thirdly, we will highlight two combined predictive biomarkers: TMB+GEP and MPS+TIDE. These integrated biomarkers showed improved predictive outcomes compared to a single predictor. Finally, we will present a potential nucleic acid biomarker signature, allowing DNA and RNA biomarkers to be analyzed in one assay. This comprehensive signature could represent a future direction of developing robust predictive biomarkers, particularly for the cold tumors, for ICI response.

Electrochemical reduction of biomass-derived 5-hydroxymethylfurfural (HMF) represents an elegant route toward sustainable value-added chemicals production that circumvents the use of fossil fuel and hydrogen. However, the reaction efficiency is hampered by the high voltage and low activity of electrodes (Cu, Bi, Pb). Herein, we report a Ru1 Cu single-atom alloy (SAA) catalyst with isolated Ru atoms on Cu nanowires that exhibits an electrochemical reduction of HMF to 2,5-dihydroxymethylfuran (DHMF) with promoted productivity (0.47 vs. 0.08 mmol cm-2 h-1 ) and faradic efficiency (FE) (85.6 vs. 71.3 %) at -0.3 V (vs. RHE) compared with Cu counterpart. More importantly, the FE (87.5 %) is largely retained at high HMF concentration (100 mM). Kinetic studies by using combined electrochemical techniques suggest disparate mechanisms over Ru1 Cu and Cu, revealing that single-atom Ru promotes the dissociation of water to produce H* species that effectively react with HMF via an electrocatalytic hydrogenation (ECH) mechanism.

Abstract Cu–ZnO–Al 2 O 3 catalysts are used as the industrial catalysts for water gas shift (WGS) and CO hydrogenation to methanol reactions. Herein, via a comprehensive experimental and theoretical calculation study of a series of ZnO/Cu nanocrystals inverse catalysts with well-defined Cu structures, we report that the ZnO–Cu catalysts undergo Cu structure-dependent and reaction-sensitive in situ restructuring during WGS and CO hydrogenation reactions under typical reaction conditions, forming the active sites of Cu Cu(100) -hydroxylated ZnO ensemble and Cu Cu(611) Zn alloy, respectively. These results provide insights into the active sites of Cu–ZnO catalysts for the WGS and CO hydrogenation reactions and reveal the Cu structural effects, and offer the feasible guideline for optimizing the structures of Cu–ZnO–Al 2 O 3 catalysts.

SHP2 inhibitors offer an appealing and novel approach to inhibit receptor tyrosine kinase (RTK) signaling, which is the oncogenic driver in many tumors or is frequently feedback activated in response to targeted therapies including RTK inhibitors and MAPK inhibitors. We seek to evaluate the efficacy and synergistic mechanisms of combinations with a novel SHP2 inhibitor, TNO155, to inform their clinical development.The combinations of TNO155 with EGFR inhibitors (EGFRi), BRAFi, KRASG12Ci, CDK4/6i, and anti-programmed cell death-1 (PD-1) antibody were tested in appropriate cancer models in vitro and in vivo, and their effects on downstream signaling were examined.In EGFR-mutant lung cancer models, combination benefit of TNO155 and the EGFRi nazartinib was observed, coincident with sustained ERK inhibition. In BRAFV600E colorectal cancer models, TNO155 synergized with BRAF plus MEK inhibitors by blocking ERK feedback activation by different RTKs. In KRASG12C cancer cells, TNO155 effectively blocked the feedback activation of wild-type KRAS or other RAS isoforms induced by KRASG12Ci and greatly enhanced efficacy. In addition, TNO155 and the CDK4/6 inhibitor ribociclib showed combination benefit in a large panel of lung and colorectal cancer patient-derived xenografts, including those with KRAS mutations. Finally, TNO155 effectively inhibited RAS activation by colony-stimulating factor 1 receptor, which is critical for the maturation of immunosuppressive tumor-associated macrophages, and showed combination activity with anti-PD-1 antibody.Our findings suggest TNO155 is an effective agent for blocking both tumor-promoting and immune-suppressive RTK signaling in RTK- and MAPK-driven cancers and their tumor microenvironment. Our data provide the rationale for evaluating these combinations clinically.

Across diverse taxa, selfing species have evolved independently from outcrossing species thousands of times. The transition from outcrossing to selfing decreases the effective population size, effective recombination rate and heterozygosity within a species. These changes lead to a reduction in genetic diversity, and therefore adaptive potential, by intensifying the effects of random genetic drift and linked selection. Within the nematode genus Caenorhabditis, selfing has evolved at least three times, and all three species, including the model organism Caenorhabditis elegans, show substantially reduced genetic diversity relative to outcrossing species. Selfing and outcrossing Caenorhabditis species are often found in the same niches, but we still do not know how selfing species with limited genetic diversity can adapt to these environments. Here, we examine the whole-genome sequences from 609 wild C. elegans strains isolated worldwide and show that genetic variation is concentrated in punctuated hyper-divergent regions that cover 20% of the C. elegans reference genome. These regions are enriched in environmental response genes that mediate sensory perception, pathogen response and xenobiotic stress response. Population genomic evidence suggests that genetic diversity in these regions has been maintained by long-term balancing selection. Using long-read genome assemblies for 15 wild strains, we show that hyper-divergent haplotypes contain unique sets of genes and show levels of divergence comparable to levels found between Caenorhabditis species that diverged millions of years ago. These results provide an example of how species can avoid the evolutionary dead end associated with selfing. The genomes of 609 wild Caenorhabditis elegans strains isolated across the world reveal hyper-divergent regions, often shared among many wild strains, that are enriched for genes that mediate environmental response, which might have enabled the species to thrive in diverse environments.

The rapid development of portable spectroscopic detectors has given rise to a great demand for small light sources, and near-infrared (NIR) phosphor-converted light-emitting diodes (pc-LEDs) are preferred for their compactness and low cost, while phosphors used in NIR spectroscopy require broadband emission, high quantum yield and good absorption efficiency as well as the spectral range required to achieve detection. Inspired by the tunable structure of Gd3Ga5O12 (GGG), a series of broadband phosphors Gd3ZnxGa5-2xGexO12:1.5%Cr3+ (x = 0–2.0) with continuously tunable emission in the long-wave direction were designed using Zn2+-Ge4+ instead of Ga3+-Ga3+ in GGG to modulate the crystal field environment of Cr3+. The crystal field intensity of the octahedra occupied by Cr3+ decreases with increasing co-substitution, and its full-width at half maximum (FWHM) from 105 nm to a maximum of 211 nm due to the change of local symmetry. In Gd3Zn0.8Ga3.4Ge0.8O12 (GZGG):5%Cr3+, the internal quantum yield (IQY) and external quantum yield (EQY) reaches 79.6% and 31.2% with impressive absorption efficiency (41.1%). The obtained phosphors were made into pc-LED with blue light chips, which was applied to glucose solution degree detection. The results show that the GZGG:Cr3+ will hopefully provide a new strategy for non-destructive testing.

High-temperature solar thermal energy systems make use of concentrated solar radiation to generate electricity, produce chemical fuels, and drive energy-intensive processing of materials. Heat transfer analyses are essential for system design and optimisation. This article reviews the progress, challenges and opportunities in heat transfer research as applied to high-temperature solar thermal and thermochemical energy systems. The topics discussed include fundamentals of concentrated solar energy collection, convective heat transfer in solar receivers, application of liquid metals as heat transfer media, and heat transfer in non-reacting and reacting two-phase solid–gas systems such as particle–gas flows and gas-saturated porous structures.

Aqueous zinc‐ion batteries (AZIBs) are an appealing battery system due to their low cost, intrinsic safety, and environmental‐friendliness, while their application is plagued by the obstacles from the cathode, electrolyte, and zinc anode. Summarizing the design principles and strategies toward the optimization of cathode, electrolyte, and zinc anode is crucial for the development of AZIBs. Herein, we present a comprehensive analysis of the design principles and promising strategies toward the improvement of AZIBs. Firstly, the various reaction mechanisms are summarized and the existing issues associated with the cathode, electrolyte, and zinc anode are discussed to guide the rational design of AZIBs. Subsequently, we provide an in‐depth and comprehensive discussion on the design principles and strategies for the electrodes/electrolyte/separator optimization, and analyze the advantages and disadvantages of various strategies. Importantly, the design principles and strategies of the newly appeared conversion‐type AZIBs, such as Zn‐S battery and Zn‐Se battery, are also discussed and analyzed. The effect of design strategies on the electrochemical performance and the relationship between the current issues and strategies are also unveiled in detail. Finally, some research trends and perspectives are provided for designing better AZIBs.

Absorption-dominant electromagnetic shielding materials can effectively reduce secondary pollution in the shielding process, and have greater significance in practical applications. Herein, silver (Ag) micro-tubes with superstructure, which were fabricated via using poly(lactic acid) (PLA) fibers as templates, were used to achieve the composites with ultrahigh, lightweight, and absorption-dominant electromagnetic shielding performance. The Ag nanoparticles were firstly deposited on the surface of PLA fibers by chemical reduction. The Ag micro-tubes were obtained by etching the PLA fibers in the core. The Ag nanoparticles were stuck together to form the Ag micro-tubes by polymer chains. The ultrahigh electromagnetic interference (EMI) shielding effectiveness (SE) of ∼110 dB was found in the Ag micro-tubes composed with polydimethylsiloxane or PLA with 1.5 mm in thickness. Due to the micro-tube structure, the composites containing with Ag micro-tubes exhibited absorption dominant shielding mechanism and low density. The absorption coefficient (A) value could reach 0.79 in the composites with Ag micro-tubes. The ultrahigh EMI SE performance and absorption dominant shielding mechanism of the composites was ascribed to the superstructure of the Ag micro-tubes which could efficiently create surface plasmon resonance, electronic vibration, interfacial polarization, capacitance effect and conductive loss. The work provides a new idea for preparing ultrahigh electromagnetic shielding materials with high absorption and low density.

Fabrication of high-performance and multiple-function conductive polymer composites with uniform distribution and high content of carbon-based nanofillers has been a formidable challenge. In this study, a new strategy was introduced to fabricate polyoxymethylene (POM)/multi-walled carbon nanotube (MWCNT) and POM/graphene nanoplate (GNP) composites (PMCNT and PMGNP, respectively), with uniform distributions and high contents of MWCNT and GNP, by assisting of miscible poly(l-lactide) (PLLA). As expected, the composites exhibit robust electromagnetic interference (EMI) shielding, Joule heating, thermal conductivity, and anti-dripping performance. Specifically, the EMI shielding effectiveness of PMCNT40 (with 40 wt% MWCNT) and PMGNP48 (with 48 wt% GNP) reached 45.7 and 44.7 dB with 0.15 mm in thickness. The high electrical and through plane thermal conductivities were 3484 S/m and 1.95 Wm−1K−1, respectively, for PMCNT40, and the corresponding values for PMGNP48 were 2695 S/m and 4.24 Wm−1K−1, respectively. Furthermore, the fabricated composites achieved excellent Joule heating performance, resulting in increases in surface temperature increase to 101.4 °C and 107.6 °C rapidly at the driving voltages of 3.0 V (in case of PMCNT40) and 6.0 V (in case of PMGNP48), respectively. In addition, the composites exhibited excellent solvent resistance and anti-dripping performance, indicating high potential applicability in extreme environments.

High conductivity can give materials excellent electromagnetic shielding performance, but it leads to serious impedance mismatching and causes inevitable secondary pollution. Developing materials with both excellent microwave absorption and microwave shielding performance remains a formidable challenge. Herein, absorption-type electromagnetic shielding materials with high electromagnetic shielding effectiveness (EMW SE) values were successfully prepared by combining hollow silver micro-tubes and magnetic nano-barium ferrites. The electromagnetic parameters and impedance matching of the composites could be easily regulated by changing the ratio of silver micro-tubes (C) and nano-barium ferrites (M). Thanks to micro-tube structure and the electric-magnetic synergism of the fillers, the composites with the C:M ratio of 9:1 exhibited a high absorption coefficient (A) value of ∼0.77 and a high EMW SE value of ∼100 dB, simultaneously. The absorption-type shielding mechanism of the composites was also evaluated via discussing real and imaginary parts of complex permittivity, real and imaginary parts of complex permeability, and Cole-Cole curves. Furthermore, the composites with the C:M ratio of 3:7 exhibited excellent microwave adsorption performance with the minimum reflection loss of −46.3 dB at thickness of 3.0 mm and a maximum effective absorption band-width of 6.13 GHz.

The renewable electricity-driven electrocatalytic oxidation of biomass represents a pathway to produce value-added chemicals from waste biomass such as glycerol (a byproduct of industrial biodiesel production). However, it remains difficult to design an efficient electrocatalyst with explicit structure–property relationships. Herein, we report a single-atom bismuth (Bi)-doping strategy to endow Co3O4 with enhanced activity and selectivity toward electrocatalytic glycerol oxidation reaction (GOR). Experimental characterizations and theoretical calculations reveal that single-atom Bi substitutes cobalt at octahedral sites (CoOh3+) in Co3O4, facilitating the generation of reactive hydroxyl species (OH*) at adjacent tetrahedral Co sites (CoTd2+). Mechanism studies demonstrate that OH* accelerates the oxidation of hydroxyl groups and carbon–carbon (C–C) bond cleavage, achieving GOR activity (400 mA cm–2 at 1.446 V vs reversible hydrogen electrode, RHE) and high faradaic efficiency of formate (97.05 ± 2.55%). Our study shows a promising way to promote the electro-oxidation activity of spinel oxides for biomass valorization by a single-atom doping strategy.

Additive manufacturing, also known as three-dimensional (3D) printing technology, has recently emerged as a promising fabrication technology for a variety of applications with diverse complex architectures, as it allows for simple printing of desired pattern, fast prototyping, reduced fabrication process and low cost. As an important type of 3D printing technology, direct ink writing (DIW) endows the electrochemical energy storage devices (EESDs) with excellent electrochemical performance with high areal energy density and excellent rate capability owing to enhanced ion/electron transportation and surface kinetics induced by the designed patterns and device architecture. In view of the current infancy and urgency, as well as the lack of in-depth discussion, we critically overview the DIW 3D printing technology for EESDs devices in terms of materials selectivity principle for ink formulation and rheology, technical challenges (design principles and optimization strategies) and various EESDs applications in a comprehensive yet concise fashion. In this review, firstly, we introduce the typical features of DIW 3D printing technology. Subsequently, we discuss the design and optimization strategies towards several key parameters of DIW, including printable ink formulation, printing process and post treatment, device configuration and electrode pattern, porosity and tortuosity, as well as the package. Thereafter, we summarize the advances and recent progress of various EESDs devices fabricated by DIW technology, including conventional lithium/sodium ion batteries, newly emerged lithium sulfur/selenide/oxygen batteries, lithium/sodium-metal batteries, Ni-Fe batteries, zinc-air batteries, zinc ion batteries and supercapacitors, with a detailed analysis of rational design mechanism of each EESD. At last, the remaining challenges and research orientations in this booming field are proposed to motivate the future research and development of 3D printed EESDs.

Abstract This paper introduces a simple framework of counterfactual estimation for causal inference with time‐series cross‐sectional data, in which we estimate the average treatment effect on the treated by directly imputing counterfactual outcomes for treated observations. We discuss several novel estimators under this framework, including the fixed effects counterfactual estimator, interactive fixed effects counterfactual estimator and matrix completion estimator. They provide more reliable causal estimates than conventional two‐way fixed effects models when treatment effects are heterogeneous or unobserved time‐varying confounders exist. Moreover, we propose a new dynamic treatment effects plot, along with several diagnostic tests, to help researchers gauge the validity of the identifying assumptions. We illustrate these methods with two political economy examples and develop an open‐source package, fect , in both R and Stata to facilitate implementation.

Understanding the heterogeneity of the nanoscale pore structure is critical for assessment of hydrocarbon flow and storage in porous reservoirs. Multifractal theory is a powerful method to acquire the detailed heterogeneity information of the multiple pore system. The generalized dimension spectrum and singularity spectrum are two forms to depict the multifractal feature. Hurst exponent (H) and the width of singularity spectrum (Δα) are two parameters to effectively assess the pore connectivity and heterogeneity, respectively. In this study, multifractal analysis was performed on over-mature Wufeng-Longmaxi shales and their corresponding isolated organic matter (OM) via gas physisorption (CO2 and N2) test to ascertain the pore heterogeneity and its governing factors. Micropore (diameter<2 nm) structure in bulk shale contains stronger pore heterogeneity but weaker connectivity than meso-macropore (diameter = 2–100 nm) structure. The comparison of heterogeneity features of shale versus its isolated OM reveals that micropore associated with minerals could enhance the micropore heterogeneity in bulk shale, while meso-macropore existing in minerals could reduce the meso-macropore heterogeneity in bulk shale. Besides, the total organic carbon content has a positive effect on the micropore heterogeneity. The micropore and meso-macropore volume have a certain impact on the pore heterogeneity in the corresponding pore size ranges. Compared with the low-mature Bakken shale, the over-mature Wufeng-Longmaxi shale contains the stronger micropore heterogeneity but weaker meso-macropore heterogeneity, where less difference between the micropore and meso-macropore heterogeneities was also observed. We deduced that the whole shale pore spectrum likely tends to be homogeneous along with the OM thermal maturation.

Featuring a high theoretical capacity, low cost, and abundant resources, sodium metal has emerged as an ideal anode material for sodium ion batteries. However, the real feasibility of sodium metal anodes is still hampered by the uncontrolled sodium dendrite problems. Herein, an artificial three-dimensional (3D) hierarchical porous sodiophilic V2CTx/rGO-CNT microgrid aerogel is fabricated by a direct-ink writing 3D printing technology and further adopted as the matrix of Na metal to deliver a Na@V2CTx/rGO-CNT sodium metal anode. Upon cycling, the V2CTx/rGO-CNT electrode can yield a superior cycling life of more than 3000 h (2 mA cm-2, 10 mAh cm-2) with an average Coulombic efficiency of 99.54%. More attractively, it can even sustain a stable operation over 900 h at 5 mA cm-2 with an ultrahigh areal capacity of 50 mAh cm-2. In situ and exsitu characterizations and density functional theory simulation analyses prove that V2CTx with abundant sodiophilic functional groups can effectively guide the sodium metal nucleation and uniform deposition, thus enabling a dendrite-free morphology. Moreover, a full cell pairing a Na@V2CTx/rGO-CNT anode with a Na3V2(PO4)3@C-rGO cathode can deliver a high reversible capacity of 86.27 mAh g-1 after 400 cycles at 100 mA g-1. This work not only clarifies the superior Na deposition chemistry on the sodiophilic V2CTx/rGO-CNT microgrid aerogel electrode but also offers an approach for fabricating advanced Na metal anodes via a 3D printing method.

The synthesis of novel two-dimensional (2D) materials displaying an unprecedented composition and structure via the exfoliation of layered systems provides access to uncharted properties. For application in optoelectronics, a vast majority of exfoliated 2D semiconductors possess n-type or more seldom ambipolar characteristics. The shortage of p-type 2D semiconductors enormously hinders the extensive engineering of 2D devices for complementary metal oxide semiconductors (CMOSs) and beyond CMOS applications. However, despite the recent progress in the development of 2D materials endowed with p-type behaviors by direct synthesis or p-doping strategies, finding new structures is still of primary importance. Here, we report the sonication-assisted liquid-phase exfoliation of violet phosphorus (VP) crystals into few-layer-thick flakes and the first exploration of their electrical and optical properties. Field-effect transistors based on exfoliated VP thin films exhibit a p-type transport feature with an Ion/Ioff ratio of 104 and a hole mobility of 2.25 cm2 V-1 s-1 at room temperature. In addition, the VP film-based photodetectors display a photoresponsivity (R) of 10 mA W-1 and a response time down to 0.16 s. Finally, VP embedded into CMOS inverter arrays displays a voltage gain of ∼17. This scalable production method and high quality of the exfoliated material combined with the excellent optoelectronic performances make VP an enticing and versatile p-type candidate for next-generation more-than-Moore (opto)electronics.

Preclinical and clinical studies have suggested a neuroprotective effect of remote ischemic conditioning (RIC), which involves repeated occlusion/release cycles on bilateral upper limb arteries; however, robust evidence in patients with ischemic stroke is lacking.To assess the efficacy of RIC for acute moderate ischemic stroke.This multicenter, open-label, blinded-end point, randomized clinical trial including 1893 patients with acute moderate ischemic stroke was conducted at 55 hospitals in China from December 26, 2018, through January 19, 2021, and the date of final follow-up was April 19, 2021.Eligible patients were randomly assigned within 48 hours after symptom onset to receive treatment with RIC (using a pneumatic electronic device and consisting of 5 cycles of cuff inflation for 5 minutes and deflation for 5 minutes to the bilateral upper limbs to 200 mm Hg) for 10 to 14 days as an adjunct to guideline-based treatment (n = 922) or guideline-based treatment alone (n = 971).The primary end point was excellent functional outcome at 90 days, defined as a modified Rankin Scale score of 0 to 1. All end points had blinded assessment and were analyzed on a full analysis set.Among 1893 eligible patients with acute moderate ischemic stroke who were randomized (mean [SD] age, 65 [10.3] years; 606 women [34.1%]), 1776 (93.8%) completed the trial. The number with excellent functional outcome at 90 days was 582 (67.4%) in the RIC group and 566 (62.0%) in the control group (risk difference, 5.4% [95% CI, 1.0%-9.9%]; odds ratio, 1.27 [95% CI, 1.05-1.54]; P = .02). The proportion of patients with any adverse events was 6.8% (59/863) in the RIC group and 5.6% (51/913) in the control group.Among adults with acute moderate ischemic stroke, treatment with remote ischemic conditioning compared with usual care significantly increased the likelihood of excellent neurologic function at 90 days. However, these findings require replication in another trial before concluding efficacy for this intervention.ClinicalTrials.gov Identifier: NCT03740971.

Plastic waste triggers a series of concerns because of its disruptive impact on the environment and ecosystem. From the point of view of catalysis, however, end-of-life plastics can be seen as an untapped feedstock for the preparation of value-added products. Thus, the development of diversified catalytic approaches for plastics valorization is urgent. Previous reviews of this field have systematically summarized progress made for plastic reclamation. In this review, we emphasize the design of processes by leveraging state-of-the-art technologies from other developed fields to derive a series of valuable polymers, functional materials, and chemicals from waste plastics. The principles, mechanisms, and opportunities for plastic valorization by leveraging chemical catalytic technologies (thermo-, electro-, and photocatalytic) as well as biocatalytic ones are summarized and discussed, which may provide more insights for the future design of catalytic processes. Finally, the outlooks and perspectives to accelerate progress toward a feasible plastic economy are discussed.

The direct solar-driven CO2 conversion to high-value-added chemicals with high selectivity represents an attractive approach to address the energy crisis and environmental pollution. Herein, we report a facile dye-anchoring strategy with a metal–organic framework (MOF) to construct a series of low-cost visible-light-driven composite photocatalysts of rhodamine B (RhB)-sensitized Zr-MOF, x-RhB@Zr-MOF (x = 1–4). Benefiting from the coupling mode of chemical bonding rather than physical adsorption, the RhB molecules were firmly anchored in Zr-MOF, resulting in the improvement of visible-light absorption and the efficient transfer of photogenerated electrons from RhB to Zr-MOF. Significantly, 3-RhB@Zr-MOF exhibits enhanced photocatalytic performance for the reduction of CO2 to CO under visible-light illumination. The evolution rate of CO can reach 10.27 μmol·g–1 in 4 h and the selectivity of >99% without the use of any organic sacrificial agents or photosensitizers, much superior to that of Zr-MOF. This work provides insight that will help in the construction of selective visible-light-driven catalysts for the photoreduction of CO2 through a solid–gas mode.

Improving the stability of sensitive catalytic systems is an emerging research topic in the catalysis field. However, the current design of heterogeneous catalysts mainly improves their catalytic performance. This paper presents a single-atom catalyst (SAC) strategy to improve the cobalt-catalysed fluorination of acyl chlorides. A stable Co-F intermediate can be formed through the oxidative fluorination of Co1 -N4 @NC SAC, which can replace the unstable high-valent cobalt catalytic system and avoid the use of phosphine ligands. In the SAC system, KF can be employed as a fluorinating reagent to replace the AgF, which can be applied to various substrates and scale-up conversion with high turnover numbers (TON=1.58×106 ). This work also shows that inorganic SACs have tremendous potential for organofluorine chemistry, and it provides a good reference for follow-up studies on the structure-activity relationship between catalyst design and chemical reaction mechanisms.

When rolling aluminum (Al)/magnesium (Mg)/aluminum (Al) composite plates with large reduction, there are often differences in the matrix structure and hard brittle properties of interfacial intermetallic compounds, which have a negative impact on the mechanical properties. Therefore, it is necessary to adjust the evolution of the diffusion layer and homogenize the internal structure of the metal plate by annealing to achieve the best performance. In this study, Al/Mg/Al composite plates were formed by hard-plate rolling (HPR) with a single pass of 60% reduction and annealed. The results show that the tensile strength (UTS) of rolled plate is 235.4 MPa and the elongation to failure (A) is 6.2%. It is found that after annealing at 300 °C for 1 h, the interface bonding property is suitable, the microstructure is gradually uniformly refined by the joint action of shear band expansion and twin induced static recrystallization, the UTS reaches 265.1 MPa. The A is increased by 18.5%. In conclusion, annealing treatment can significantly improve the microstructure and connection strength of hard-plate rolling Al/Mg/Al composite plates and provide scientific guidance and technical support for the forming and manufacturing high-performance lightweight composite plates.

Abstract Electroreduction of CO 2 (CO 2 RR) into high value‐added chemicals is an attractive route to achieve carbon neutrality. However, the development of an efficient catalyst for CO 2 RR is still largely by trial‐and‐error and is very time‐consuming. Herein, we built an electrocatalyst testing platform featuring a home‐built automatic flow cell to accelerate the discovery of efficient catalysts. A fast screening of 109 Cu‐based bimetallic catalysts in only 55 h identifies Mg combined with Cu as the best electrocatalyst for CO 2 to C 2+ products. The thus designed Mg−Cu catalyst achieves a Faradaic efficiency (FE) of C 2+ products up to 80 % with a current density of 1.0 A cm −2 at −0.77 V versus reversible hydrogen electrode (RHE). Systematic experiments with in situ spectroelectrochemistry analyses show that Mg 2+ species stabilize Cu + sites during CO 2 RR and promote the CO 2 activation, thus enhancing the *CO coverage to promote C−C coupling.