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In-situ construction of epitaxial phase for boosting zinc nucleation on three-dimensional interface

Progress in Natural Science:Materials International 2024年第3期34卷 578-584页

作者： Xin He Zhe Zhu Xiaoqiao Liao Kai Yang Yixue Duan Linfeng Lv Chuan Zhao Wei Zhao Jibing Chen peng tian Xiaoyu Liu Liang He School of Mechanical Engineering State Key Laboratory of Intelligent Construction and Healthy Operation and Maintenance of Deep Underground Engineering Sichuan University School of Chemistry Faculty of Science University of New South Wales School of Materials Science and Engineering Sichuan University of Science & Engineering School of Mechanical Engineering Wuhan Polytechnic University Med+X Center for Manufacturing West China Hospital Sichuan University Yibin Industrial Technology Research Institute of Sichuan University Yibin R&D Park of Sichuan University

Interface modification of zinc（Zn） metal anode with conductive three-dimensional（3D） structure is widely utilized in zinc ion batteries. However, the uniformity of zinc nucleation on surface microstructure is rarely investigated which exacerbates the tip effect and raises unstable risk. Herein, a strategy via the initial copper（Cu）alloying and following sulfurization treatment is reported to accomplish boosted uniform nucleation of zinc on the modified layer with dense microstructures. This epitaxial sulfide phase not only improves the wetting area to revitalize the microstructural surface, but also forms a bifunctional zincophilic Cu2S/CuZn alloy interface layer,which combines the merits of guided local ions diffusion and improved zinc nucleation environment. As a result, a homogeneous growth of zinc on the 3D structural substrate can be realized, and cycling stability of the achieved Cu2S/CuZn electrode with a practical capacity of 1 mAh cm-2under 1 mA cm-2or amplified current density of 10 mA cm-2is significantly enhanced. This work provides an epitaxial strategy in constructing a bifunctional zincophilic interface layer for boosting zinc nucleation, and offers a new perspective on the modification of 3D surface structure for stabilization of zinc anode.

关键词： CuZn alloy Hydrophilicity Sulfide Zn anode Zn metal battery

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High-silica faujasite zeolite-tailored metal encapsulation for the low-temperature production of pentanoic biofuels

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Journal of Energy Chemistry 2024年第1期88卷 552-560,I0012页

作者： Wenhao Cui Yuanshuai Liu pengfei Guo Zhijie Wu Liqun Kang Huawei Geng Shengqi Chu Linying Wang Dong Fan Zhenghao Jia Haifeng Qi Wenhao Luo peng tian Zhongmin Liu National Engineering Research Center of Lower-Carbon Catalysis Technology Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China Qingdao Institute of Bioenergy and Bioprocess Technology Chinese Academy of SciencesQingdao 266101ShandongChina College of Chemistry and Chemical Engineering Inner Mongolia UniversityHohhot 010021Inner MongoliaChina State Key Laboratory of Heavy Oil Processing and Key Laboratory of Catalysis of CNPC China University of PetroleumBeijing 102249China Department of Inorganic Spectroscopy Max Planck Institute for Chemical Energy ConversionMülheim an der Ruhr 45470Germany Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China Division of Energy Research Resources Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina Leibniz-Institut für Katalyse Albert-Einstein-Straβe 29aRostock 18059Germany

Zeolite-encapsulated metal nanoclusters are at the heart of bifunctional catalysts,which hold great potential for petrochemical conversion and the emerging sustainable biorefineries.Nevertheless,efficient encapsulation of metal nanoclusters into a high-silica zeolite Y in particular with good structural integrity still remains a significant challenge.Herein,we have constructed Ru nanoclusters(~1 nm)encapsulated inside a high-silica zeolite Y(SY)with a SiO_(2)/Al_(2)O_(3) ratio(SAR)of 10 via a cooperative strategy for direct zeolite synthesis and a consecutive impregnation for metal encapsulation.Compared with the benchmark Ru/H-USY and other analogues,the as-prepared Ru/H-SY markedly boosts the yields of pentanoic biofuels and stability in the direct hydrodeoxygenation of biomass-derived levulinate even at a mild temperature of 180℃,which are attributed to the notable stabilization of transition states by the enhanced acid accessibility and properly sized constraints of zeolite cavities owing to the good structural integrity.

关键词： High-silica zeolite Y Metal encapsulation Bifunctional catalysis Hydrodeoxygenation Biofuels

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Fabrication of Molecularly Imprinted Electrospun Nanofibers with Mono-amidoxime Functional Ligand for Efficient Decontamination of Toxic Organophosphates

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Chinese Journal of Polymer Science 2024年第4期42卷 446-456页

作者： Lan Wang peng Jiang Ya-Lin Niu Jun-peng Cao tian-Ying Guo Key Laboratory of Functional Polymer Materials Ministry of EducationInstitute of Polymer ChemistryCollege of Chemistry and Frontier Science Center for the Creation of New Organic SubstancesNankai UniversityTianjin300071China

There is an urgent imperative to discover practical and efficacious artificial catalysts for the expeditious decontamination of toxic organophosphates. Herein, we propose a novel molecularly imprinted approach utilizing electrospun fiber scaffolds. Specifically, an amidoxime-based functional polymer (PMAOX) has been synthesized, which contains amidoxime groups that can act as nucleophiles and ligands for the formation of catalytic active sites. This polymer was blended with polyacrylonitrile (PAN), a well-processable material, to prepare a nanofiber mat using electrospinning techniques. Then, the amidoxime side groups on fiber surface were further cross-linked after the molecular coordination of templates to complete the molecularly imprinting process. This approach can not only enhance the content of functional molecularly imprinted polymers without affecting structural stability, but also combines surface MI technology to fully expose and leverage the advantages of active sites. The as prepared molecularly imprinted electrospun nanofibers MIF-Zn-PMAOX/PAN-6/4 catalyzes the degradation of paraoxon with a half-life of 32 min, and MIF-Ag-PMAOX/PAN catalyzes the degradation of parathion with a half-life of 18 min. The maximum catalytic rate evidence rate enhancements nearly 3700-fold of the self-hydrolysis. Thus, the mono-amidoxime based molecularly imprinted fibers demonstrate the versatility and superiority as self-detoxifying for organophosphates.

关键词： Organophosphateshydrolysis Electrospinning Molecular imprinting

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APTAnet: an atom-level peptide-TCR interaction affinity prediction model

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Biophysics Reports 2024年第1期10卷 1-14页

作者： peng Xiong Anyi Liang Xunhui Cai tian Xia School of Artificial Intelligence and Automation Huazhong University of Science and Technology Institute of Pathology Tongji Hospital Tongji Medical College Huazhong University of Science and Technology

The prediction of affinity between TCRs and peptides is crucial for the further development of TIL(Tumor-Infiltrating Lymphocytes) immunotherapy. Inspired by the broader research of drug-protein interaction(DPI), we propose an atom-level peptide-TCR interaction(PTI) affinity prediction model APTAnet using natural language processing methods. APTAnet model achieved an average ROC-AUC and PR-AUC of 0.893 and 0.877, respectively, in ten-fold cross-validation on 25,675 pairs of PTI data.Furthermore, experimental results on an independent test set from the McPAS database showed that APTAnet outperformed the current mainstream models. Finally, through the validation on 11 cases of real tumor patient data, we found that the APTAnet model can effectively identify tumor peptides and screen tumor-specific TCRs.

关键词： Immunotherapy TCR Antigen Natural language processing Transfer learning

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Co-influence of the start of thermal growing season and precipitation on vegetation spring green-up on the Tibetan Plateau

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Advances in Climate Change Research 2024年第2期15卷 327-337页

作者： Chen-peng WANG Meng-tian HUANG Pan-Mao ZHAI State Key Laboratory of Severe Weather and Institute of Global Change and Polar Meteorology Chinese Academy of Meteorological SciencesBeijing 100081China University of Chinese Academy of Sciences Beijing 100049China

The climate in the Tibetan Plateau(TP)has undergone significant change in recent decades,mainly in thermal and water conditions,which plays a crucial role in phenological changes in vegetation spring phenology.However,how the start of the thermal growing season(SOS-T)and the start of the rainy season(SORS)as key climatic factors affect vegetation green-up remains unclear.Given that these factors characterize thermal and water conditions required for vegetation green-up,this study investigated changes in the SOS-T and SORS from 1961 to 2022,using observation-based datasets with long time series.We found that the SOS-T and SORS have advanced across the TP in 1961-2022 and have shown a spatial pattern of advancement in the east and delay in the west in 2000-2022.Further,the co-effect of temperature and precipitation change on the start of vegetation growing season(SOS-V)in 2000-2022 was observed.Averaged across TP,the SOS-V had an early onset of 1.3 d per decade during 2000-2022,corresponding to advanced SOS-T and SORS.Regionally,the SOS-V generally occurred nearly at the same time as the SOS-T in the high-altitude meadow region.A substantial delay in the SOS-V relative to the SOS-T was observed in the desert,shrub,grassland and forest regions and generally kept pace with the SORS.Furthermore,for 50%of the vegetated regions on the TP,inter-annual variation in the delay in the SOS-V relative to the SOS-T was dominated by precipitation change,which was profound in warm-climate regions.This study highlights the co-regulation of precipitation and temperature change in the SOS-V in different vegetation cover regions in the TP,offering a scientific foundation for comprehending the impact of climate change and prospects for vegetation phenology on the TP.

关键词： Tibetan Plateau Start of growing season Temperature Precipitation Climate change

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Spin effect on redox acceleration and regioselectivity in Fe-catalyzed alkyne hydrosilylation

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National Science Review 2024年第2期11卷 155-167页

作者： peng He Meng-Yang Hu Jin-Hong Li tian-Zhang Qiao Yi-Lin Lu Shou-Fei Zhu Frontiers Science Center for New Organic Matter State Key Laboratory and Institute of Elemento-Organic Chemistry Nankai University

Iron catalysts are ideal transition metal catalysts because of the Earths abundant, cheap, biocompatible features of iron salts. Iron catalysts often have unique open-shell structures that easily undergo spin crossover in chemical transformations, a feature rarely found in noble metal catalysts. Unfortunately, little is known currently about how the open-shell structure and spin crossover affect the reactivity and selectivity of iron catalysts, which makes the development of iron catalysts a low efficient trial-and-error program. In this paper, a combination of experiments and theoretical calculations revealed that the iron-catalyzed hydrosilylation of alkynes is typical spin-crossover catalysis. Deep insight into the electronic structures of a set of well-defined open-shell active formal Fe(0) catalysts revealed that the spin-delocalization between the iron center and the 1,10-phenanthroline ligand effectively regulates the iron center's spin and oxidation state to meet the opposite electrostatic requirements of oxidative addition and reductive elimination, respectively,and the spin crossover is essential for this electron transfer process. The triplet transition state was essential for achieving high regioselectivity through tuning the nonbonding interactions. These findings provide an important reference for understanding the effect of catalyst spin state on reaction. It is inspiring for the development of iron catalysts and other Earth-abundant metal catalysts, especially from the point of view of ligand development.

关键词： spin effect spin-delocalization spin crossover iron-catalysis alkyne hydrosilylation

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Why lowland riparian trees are difficult to use for streamflow reconstruction

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Journal of Forestry Research 2024年第3期35卷 219-230页

作者： Xiaomei peng Shengchun Xiao Bao Yang Quanyan tian Vladimir V.Shishov Key Laboratory of Ecological Safety and Sustainable Development in Arid Lands Northwest Institute of Eco-Environment and ResourcesChinese Academy of SciencesLanzhou 730000People's Republic of China School of Geography and Ocean Science Nanjing UniversityNanjing 210023People's Republic of China Institute of Fundamental Biology and Biotechnology Siberian Federal UniversityKrasnoyarskRussia 660041

Existing streamflow reconstructions based on tree-ring analysis mostly rely on species from upland,mainly montane areas,while lowland species(generally plain)areas are rarely used.This limits the understanding of streamflow change history in the lowlands,which is an important basis for water resource management.This study focused on Populus euphratica stands located along the main stream,eastern and western tributaries in the lower reaches of the Heihe River basin(HRb),in arid northwestern China.We investigated how streamflow regulation interferes with ripar-ian trees in lowlands when they used for streamflow recon-struction.Tree-ring width chronologies were developed and analyzed in conjunction with meteorological and hydrologic observation data.The results show streamflow regulation leads in sharp fluctuations in the streamflow allocation between the eastern tributaries and western tributaries.This resulted in instability of the correlation between streamflow at the two tributaries and at the Zhengyixia hydrologic station,with corresponding fluctuations in radial growth of poplar trees on the banks of the two tributaries and at the station.Streamflow regulation altered the natural patterns of seasonal streamflow below the station,changing the time window of poplar response.This study provides useful insight into tree-ring width based streamflow reconstruction in the lowlands.

关键词： Tree-ring width-Dendrochronology Populus euphratica The Ejina Oasis Streamflow

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The Roadmap of 2D Materials and Devices Toward Chips

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Nano-Micro Letters 2024年第6期16卷 343-438页

作者： Anhan Liu Xiaowei Zhang Ziyu Liu Yuning Li Xueyang peng Xin Li Yue Qin Chen Hu Yanqing Qiu Han Jiang Yang Wang Yifan Li Jun Tang Jun Liu Hao Guo Tao Deng Songang peng He tian tian‑Ling Ren School of Integrated Circuits and Beijing National Research Center for Information Science and Technology(BNRist) Tsinghua UniversityBeijing 100049People’s Republic of China School of Microelectronics Fudan UniversityShanghai 200433People’s Republic of China State Key Laboratory of Dynamic Measurement Technology Shanxi Province Key Laboratory of Quantum Sensing and Precision MeasurementNorth University of ChinaTaiyuan 030051People’s Republic of China High‑Frequency High‑Voltage Device and Integrated Circuits R&D Center Institute of MicroelectronicsChinese Academy of SciencesBeijing 100029People’s Republic of China School of Electronic and Information Engineering Beijing Jiaotong UniversityBeijing 100044People’s Republic of China School of Integrated Circuits University of Chinese Academy of SciencesBeijing 100049People’s Republic of China IMECAS-HKUST-Joint Laboratory of Microelectronics Beijing 100029People’s Republic of China

Due to the constraints imposed by physical effects and performance degra certain limitations in sustaining the advancement of Moore’s law.Two-dimensional(2D)materials have emerged as highly promising candidates for the post-Moore era,offering significant potential in domains such as integrated circuits and next-generation computing.Here,in this review,the progress of 2D semiconductors in process engineering and various electronic applications are summarized.A careful introduction of material synthesis,transistor engineering focused on device configuration,dielectric engineering,contact engineering,and material integration are given first.Then 2D transistors for certain electronic applications including digital and analog circuits,heterogeneous integration chips,and sensing circuits are discussed.Moreover,several promising applications(artificial intelligence chips and quantum chips)based on specific mechanism devices are introduced.Finally,the challenges for 2D materials encountered in achieving circuit-level or system-level applications are analyzed,and potential development pathways or roadmaps are further speculated and outlooked.

关键词： Two-dimensional materials Roadmap Integrated circuits Post-Moore era

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Chromosome-scale genomes of Quercus sichourensis and Quercus rex provide insights into the evolution and adaptation of Fagaceae

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Journal of Genetics and Genomics 2024年第5期51卷 554-565页

作者： Xue Liu Weixiong Zhang Yongting Zhang Jing Yang peng Zeng Zunzhe tian Weibang Sun Jing Cai Shaanxi Key Laboratory of Qinling Ecological Intelligent Monitoring and Protection School of Ecology and EnvironmentNorthwestern Polytechnical UniversityXi'anShaanxi 710072China Yunnan Key Laboratory for Integrative Conservation of Plant Species with Extremely Small Populations Kunming Institute of BotanyChinese Academy of SciencesKunmingYunnan 650201China

The Fagaceae,a plant family with a wide distribution and diverse adaptability,has garnered significant interest as a subject of study in plant speciation and adaptation.Meanwhile,certain Fagaceae species are regarded as highly valuable wood resources due to the exceptional quality of their wood.In this study,we present two high-quality,chromosome-scale genome sequences for Quercus sichourensis(848.75 Mb)and Quercus rex(883.46 Mb).Comparative genomics analysis reveals that the difference in the number of plant disease resistance genes and the nonsynonymous and synonymous substitution ratio(Ka/Ks)of protein-coding genes among Fagaceae species are related to different environmental adaptations.Interestingly,most genes related to starch synthesis in the investigated Quercoideae species are located on a single chromosome,as compared to the outgroup species,Fagus sylvatica.Furthermore,resequencing and population analysis of Q.sichourensis and Q.rex reveal that Q.sichourensis has lower genetic diversity and higher deleterious mutations compared to Q.rex.The high-quality,chromosome-level genomes and the population genomic analysis of the critically endangered Q.sichourensis and Q.rex will provide an invaluable resource as well as insights for future study in these two species,even the genus Quercus,to facilitate their conservation.

关键词： Adaptation Quercus sichourensis Quercusrex Chromosome-scale genome assembly Tandemduplicationgenes Extremelysmallpopulations

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Preparation, Crystallization and Mechanical Properties of Potassium Aluminosilicate Glass-ceramics

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Journal of Wuhan University of Technology(Materials Science) 2024年第3期39卷 587-595页

作者：郑伟宏黄猛 GAO Zipeng ZHANG Hang YUAN Jian tian Peijing peng Zhigang State Key Laboratory of Silicate Materials for Architectures Wuhan University of TechnologyWuhan 430070China Shahe Research Institute of Glass Technology Shahe 054100China

In this study,transparent K_(2)O-Al_(2)O_(3)-SiO_(2)(KAS)glass-ceramics with leucite as the main crystalline phase were prepared by melting-quench method and two-step heat treatment.The effects of SiO_(2)/Al_(2)O_(3) ratio and heat treatment on crystallization and mechanical properties were studied.The crystallization kinetics and X-Ray Diffraction(XRD)results showed that SiO_(2)/Al_(2)O_(3) ratio and heat treatment system had a direct impact on the crystallization behavior of potassium aluminosilicate glass-ceramics.When heat-treated at 680℃/2 h and 780℃/1 h,cracks generated on the surface of the sample with the addition of SiO_(2)/Al_(2)O_(3)=4.8(in mol)due to the huge difference in the coefficient of thermal expansion between glass matrix and surface.When the addition of SiO_(2)/Al_(2)O_(3)(in mol)was 4,the sample with leucite as the main crystalline phase showed an excellent fracture toughness(1.46 MPa·m^(0.5))after the heat treatment of 680℃/2 h and 780℃/5 h.And there was a phase transformation from kaliophilite to leucite.The crystalline phases of the sample heat-treated at 680℃/8 h and 780℃/1 h were leucite and kaliophilite,which resulted in the visible light transmittance of 63%and the fracture toughness of 0.91 MPa·m^(0.5).Furthermore,after the heat treatment of 680℃/2 h and 780℃/5 h,the main crystalline phase of the sample with SiO_(2)/Al_(2)O_(3)=3.2(in mol)was still kaliophilite.Because leucite only grows on the surface of the sample and is hard to grow inward,it is hard to achieve the bulk crystallization of leucite in the sample with SiO_(2)/Al_(2)O_(3)=3.2(in mol).

关键词： leucite glass-ceramic kaliophilite crystallization kinetics

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