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Heteroepitaxial growth of Au@Pd core–shell nanocrystals with intrinsic chiral surfaces for enantiomeric recognition

Rare Metals 2024年第1期43卷 225-235页

作者： Feng-Xia Wu Feng-Hua Li Xia-Li Lv Qi-Xian Zhang Guo-Bao Xu Wen-Xin Niu State Key Laboratory of Electroanalytical chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China Shaoxing institute of Technology Shanghai UniversityShaoxing 312000China University of Science and Technology of China Hefei 230026China School of Materials Science and Engineering Shanghai UniversityShanghai 200436China Zhejiang institute of Advanced Materials Shanghai UniversityJiashan 314113China University of Chinese Academy of Sciences Beijing 100039China

Noble metal surfaces with intrinsic chirality serve as an ideal candidate for investigating enantioselective chemistry due to their superior chemical durability and high catalytic ***,significant advance has been made in synthesizing metal nanocrystals with intrinsic ***,the majority reports are limited to ***,through a heteroepitaxial growth strategy,the synthesis of metal nanocrystals with intrinsic chirality to palladium was extended for the first time and their application in enantioselective recognition was *** heteroepitaxial growth strategy allows for transferring the chirality of homochiral Au nanocrystals to Au@Pd core–shell *** employing the chiral Au@Pd nanocrystals as enantiomeric recognizing elements,a series of electrochemical sensors for chiral discrimination were *** optimal conditions,the peak potential between D-dihydroxyphenylalanine(D-DOPA)and L-dihydroxyphenylalanine(L-DOPA)is about 80 m V,and the peak current of D-DOPA is 2 times as much as that of L-DOPA,which enables the determination of the enantiomeric excess(EE,%)of ***,this report not only introduces a heteroepitaxial growth strategy to synthesize metal nanocrystals with intrinsic chirality,but also demonstrates the superior capability of integrating intrinsic chirality and catalytic properties into metal nanocrystals for chiral recognition.

关键词： Core–shell nanostructures Chirality transfer Electrochemical sensors Chiral recognition Chiroplasmonics

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Cobalt(Ⅲ)hydride HAT mediated enantioselective intramolecular hydroamination access to chiral pyrrolidines

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Science China chemistry 2024年第6期67卷 2002-2008页

作者： Qi Meng Tao Qin Huanran Miao Ge Zhang Qian Zhang Jilin Province Key Laboratory of Organic Functional Molecular Design&Synthesis Department of ChemistryNortheast Normal UniversityChangchun130024China State Key Laboratory of Organometallic chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai200032China

Enantioenriched pyrrolidines and derivatives are ubiquitous substructures in compounds of importance to medicinal and biological ***,we report an efficient cobalt-catalyzed intramolecular asymmetric hydroamination reaction that produces chiral pyrrolidines with good to excellent yield and *** with previously reported radicalinvolved methodologies for enantioenriched pyrrolidines,these conditions feature two elegant versatilities,enabling(1)the use of cobalt-catalyzed hydrogen atom transfer(HAT)to generate organocobalt intermediates that bring radical reaction to organometallic chemistry,and(2)enantioselective intramolecular C-N bond forging through an S_(N)2-like displacement involving dynamic kinetic resolution(DKR).This approach provides a new alternative and efficient methodology for enantioselective radical-involved C-N bond construction that can be used in the synthesis of both chiral pyrrolidines and homologous nitrogen heterocycles.

关键词： asymmetric catalysis radical hydroamination cobalt catalysis hydrogen atom transfer

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Antimony oxides-protected ultrathin Ir-Sb nanowires as bifunctional hydrogen electrocatalysts

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Nano Research 2024年第3期17卷 1042-1049页

作者： Bingyan Xu Xuan Huang Shangheng Liu Zhiwei Hu Cheng-Wei Kao Ting-Shan Chan Hongbo Geng Ying Zhang Xiaoqing Huang Country State Key Laboratory of Physical chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Max Planck institute for Chemical Physics of Solids Dresden 01187Germany “National Synchrotron Radiation Research Center” Hsinchu 30076TaiwanChina School of Materials Engineering Changshu Institute of TechnologyChangshu 215500China institute for Carbon Neutralization College of Chemistry and Materials EngineeringWenzhou UniversityWenzhou 325035China

Developing electrocatalysts with fast kinetics and long-term stability for alkaline hydrogen oxidation reaction(HOR)and hydrogen evolution reaction(HER)is of considerable importance for the industrial production of green and sustainable ***,an ultrathin Ir-Sb nanowires(Ir-Sb NWs)protected by antimony oxides(SbO_(x))was synthesized as an efficient bifunctional catalyst for both HOR and HER under alkaline *** from the much higher mass activities of Ir-Sb nanowires than those of Ir nanowires(Ir NWs)and commercial Pt/C,the SbO_(x) protective layer also contributes to the maintenance of morphology and anti-CO poisoning ability,leading to the long-term cycling performance in the presence of ***,the Ir-Sb NW/SbO_(x) exhibits the highest catalytic activities,which are about 3.5 and 4.8 times to those of Ir NW/C and commercial Pt/C toward HOR,*** work provides that the ultrathin morphology and H_(2)O-occupied Sb sites can exert the intrinsic high activity of Ir and effectively optimize the absorption of OH*both in alkaline HER/HOR electrolysis.

关键词： Ir nanowire amorphous antimony oxides bifunctional mechanism hydrogen evolution reaction hydrogen oxidation reaction

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Tuning microstructures of Mg-Ce-Ni hydrogen storage alloys via Cu and carbon nanotube additions

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Nano Research 2024年第8期17卷 7203-7211页

作者： Linlin Zhang Liang Xiong Bingyang Gao Qingyun Shi Ying Wang Zhiya Han Zhenhua Zhang Chunli Wang Limin Wang Yong Cheng State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of Applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026China Purification Equipment Research institute of CSIC Handan 056002China

Mg-based alloys are regarded as highly promising materials for hydrogen *** significant improvements of the properties for Mg-based alloys,challenges such as slow hydrogen absorption/desorption kinetics and high thermodynamic stability continue to limit their practical *** this study,to assess hydrogen storage alloys with enhanced properties,incorporating both internal microstructure modulation through the preparation of amorphous/nanocrystalline structures and surface property enhancement with the addition of Cu and carbon nanotubes(CNTs),the kinetic properties of activation and hydrogenation,thermodynamic properties,and dehydrogenation kinetics are *** results reveal a complementary interaction between the added Cu and CNTs,contributing to the superior hydrogen storage performance observed in sample 7A-2Cu-1CNTs with an amorphous/nanocrystalline structure compared to the other experimental ***,the samples are fully activated after the initial hydrogen absorption and desorption cycle,demonstrating outstanding hydrogenation kinetics under both high and low temperature experimental *** noteworthy is that the hydrogen absorption exceeds 1.8 wt.%within one hour at 333 ***,the activation energy for dehydrogenation is decreased to 64.71 kJ·mol^(–1).This research may offer novel insights for the design of new-type Mg-based hydrogen storage alloys,which possess milder conditions for hydrogen absorption and desorption.

关键词： Mg-Ni-Ce alloy hydrogen storage amorphous/nanocrystalline structure kinetics Cu and carbon nanotubes(CNTs)codoping

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Exploring the impact of Nafion modifier on electrocatalytic CO_(2) reduction over Cu catalyst

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Journal of Energy chemistry 2024年第1期88卷 543-551,I0012页

作者： Yingshi Su Yonghui Cheng Zhen Li Yanjia Cui Caili Yang Ziyi Zhong Yibing Song Gongwei Wang Lin Zhuang College of chemistry&Chemical Engineering and Key Laboratory for Preparation and Application of Ordered Structural Materials of Guangdong Province Shantou UniversityShantou 515063GuangdongChina College of chemistry and Molecular Sciences Hubei Key Lab of Electrochemical Power SourcesWuhan UniversityWuhan 430072HubeiChina The institute for Advanced Studies Wuhan UniversityWuhan 430072HubeiChina Department of chemistry Engineering Guangdong Technion-Israel Institute of Technology(GTIIT)Shantou 515063GuangdongChina Technion-Israel institute of Technology(IIT) Haifa 32000Israel

Nafion as a universal polymer ionomer was widely applied for nanocatalysts electrode ***,the effect of Nafion on electrocatalytic performance was often overlooked,especially for CO_(2)***,the key roles of Nafion for CO_(2)RR were systematically studied on Cu nanoparticles(NPs)*** found that Nafion modifier not only inhibit hydrogen evolution reaction(HER)by decreasing the accessibility of H_(2)O from electrolyte to Cu NPs,and increase the CO_(2)concentration at electrocatalyst interface for enhancing the CO_(2)mass transfer process,but also activate CO_(2)molecule by Lewis acid-base interaction between Nafion and CO_(2)to accelerate the formation of^(*)CO,which favor of C–C coupling for boosting C_(2)product *** to these features,the HER selectivity was suppressed from 40.6%to 16.8%on optimal Cu@Nafion electrode at-1.2 V versus reversible hydrogen electrode(RHE),and as high as 73.5%faradaic efficiencies(FEs)of C_(2)products were achieved at the same applied potential,which was 2.6 times higher than that on bare Cu electrode(~28.3%).In addition,Nafion also contributed to the long-term stability by hinder Cu NPs morphology ***,this work provides insights into the impact of Nafion on electrocatalytic CO_(2)RR performance.

关键词： Nafion modifier CO_(2)reduction Cu nanoparticles In situ ATR-SEIRAS C_(2)product

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Unsaturated bi-heterometal clusters in metal-vacancy sites of 2D MoS2 for efficient hydrogen evolution

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Carbon Energy 2024年第3期6卷 264-275页

作者： Gonglei Shao Jie Xu Shasha Gao Zhang Zhang Song Liu Xu Zhang Zhen Zhou Interdisciplinary Research Center for Sustainable Energy Science and Engineering(IRC4SE2) School of Chemical EngineeringZhengzhou UniversityZhengzhouHenanChina College of chemistry and Materials Engineering Wenzhou UniversityWenzhouZhejiangChina Key Laboratory of Advanced Energy Materials chemistry(Ministry of Education) College of ChemistryNankai UniversityTianjinChina State Key Laboratory of Chemo/Biosensing and Chemometrics Institute of Chemical Biology and Nanomedicine(ICBN)College of Chemistry and Chemical EngineeringHunan UniversityChangshaHunanChina institute of New Energy Material chemistry School of Materials Science and EngineeringNankai UniversityTianjinChina

The valence states and coordination structures of doped heterometal atoms in two-dimensional(2D)nanomaterials lack predictable regulation ***,a robust method is proposed to form unsaturated heteroatom clusters via the metal-vacancy restraint mechanism,which can precisely regulate the bonding and valence state of heterometal atoms doped in 2D molybdenum *** unsaturated valence state of heterometal Pt and Ru cluster atoms form a spatial coordination structure with Pt–S and Ru–O–S as catalytically active *** them,the strong binding energy of negatively charged suspended S and O sites for H+,as well as the weak adsorption of positively charged unsaturated heterometal atoms for H*,reduces the energy barrier of the hydrogen evolution reaction proved by theoretical ***,the electrocatalytic hydrogen evolution performance is markedly improved by the ensemble effect of unsaturated heterometal atoms and highlighted with an overpotential of 84 mV and Tafel slope of 68.5 mV dec^(−1).In brief,this metal vacancy-induced valence state regulation of heterometal can manipulate the coordination structure and catalytic activity of heterometal atoms doped in the 2D atomic lattice but not limited to 2D nanomaterials.

关键词： clusters hydrogen evolution reaction metal vacancy MoS2 unsaturated heterometal

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Semisynthesis of homogeneous spike RBD glycoforms from SARS-CoV-2 for profiling the correlations between glycan composition and function

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National Science Review 2024年第2期11卷 145-154页

作者： Farong Ye Cheng Li Feng-Liang Liu Xinliang Liu Peng Xu Rong-Hua Luo Wenping Song Yong-Tang Zheng Tianlei Ying Biao Yu Ping Wang Center for Chemical Glycobiology Frontiers Science Center for Transformative Molecules Zhangjiang Institute for Advanced Study School of Chemistry and Chemical Engineering Shanghai Jiao Tong University MOE/NHC/CAMS Key Laboratory of Medical Molecular Virology Shanghai Frontiers Science Center of Pathogenic Microorganisms and Infection Shanghai Institute of Infectious Disease and BiosecurityShanghai Engineering Research Center for Synthetic ImmunologySchool of Basic Medical Sciences Shanghai Medical College Fudan University Key Laboratory of Animal Models and Human Disease Mechanisms of Chinese Academy of Sciences/Key Laboratory of Bioactive Peptides of Yunnan Province Center for Biosafety Mega-Science Kunming Institute of ZoologyChinese Academy of Sciences State Key Laboratory of Bioorganic and Natural Products chemistry Center for Excellence in Molecular Synthesis Shanghai Institute of Organic Chemistry Chinese Academy of Sciences Shenzhen Research institute of Shanghai Jiao Tong University

Vaccines have been the primary remedy in the global fight against coronavirus disease 2019（COVID-19）.The receptor-binding domain（RBD） of the spike protein, a critical viral immunogen, is affected by the heterogeneity of its glycan structures and relatively low immunogenicity. Here, we describe a scalable synthetic platform that enables the precise synthesis of homogeneously glycosylated RBD, facilitating the elucidation of carbohydrate structure–function relationships. Five homogeneously glycosylated RBDs bearing biantennary glycans were prepared, three of which were conjugated to T-helper epitope(Tpep) from tetanus toxoid to improve their weak immune response. Relative to natural HEK293-derived RBD, synthetic RBDs with biantennary N-glycan elicited a higher level of neutralising antibodies against SARS-CoV-2 in mice. Furthermore, RBDs containing Tpepelicited significant immune responses in transgenic mice expressing human angiotensin-converting enzyme 2. Our collective data suggest that trimming the N-glycans and Tpepconjugation of RBD could potentially serve as an effective strategy for developing subunit vaccines providing efficient protection.

关键词： peptide ligation glycosylation glycoprotein

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Flame-retardant ammonium polyphosphate/MXene decorated carbon foam materials as polysulfide traps for fire-safe and stable lithium-sulfur batteries

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Journal of Energy chemistry 2024年第2期89卷 313-323,I0008页

作者： Yang Li Yong-Cheng Zhu Sowjanya Vallem Man Li Seunghyun Song Tao Chen Long-Cheng Tang Joonho Bae Department of Physics Gachon UniversitySeongnam-siGyeonggi-do 13120South Korea Key Laboratory of Organosilicon chemistry and Material Technology of Ministry of Education College of MaterialChemistry and Chemical EngineeringHangzhou Normal UniversityHangzhou 311121ZhejiangChina Key laboratory of Advanced Energy Materials chemistry(Ministry of Education) College of ChemistryNankai UniversityTianjin 300071China School of Materials Engineering Changzhou Vocational Institute of Industry TechnologyChangzhou 213164JiangsuChina

Lithium-sulfur(Li-S)batteries are one of the most promising modern-day energy supply systems because of their high theoretical energy density and low ***,the development of high-energy density Li-S batteries with high loading of flammable sulfur faces the challenges of electrochemical performance degradation owing to the shuttle effect and safety issues related to fire or explosion *** this work,we report a three-dimensional(3D)conductive nitrogen-doped carbon foam supported electrostatic self-assembled MXene-ammonium polyphosphate(NCF-MXene-APP)layer as a heat-resistant,thermally-insulated,flame-retardant,and freestanding host for Li-S batteries with a facile and costeffective synthesis ***,through the use of NCF-MXene-APP hosts that strongly anchor polysulfides,the Li-S batteries demonstrate outstanding electrochemical properties,including a high initial discharge capacity of 1191.6 mA h g^(-1),excellent rate capacity of 755.0 mA h g^(-1)at 1 C,and long-term cycling stability with an extremely low-capacity decay rate of 0.12%per cycle at 2 *** importantly,these batteries can continue to operate reliably under high temperature or flame attack ***,this study provides valuable insights into the design of safe high-performance Li-S batteries.

关键词： Flame-retardant MXene Ammonium polyphosphate Safety Lithium-sulfur battery

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Unveiling the chemistry behind the electrolytic production of hydrogen peroxide by oxygenated carbon

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Journal of Energy chemistry 2024年第9期96卷 49-58页

作者： Pan Xiang Kunshang Yang Qihao Yang Yang Gao Wenwen Xu Zhiyi Lu Liang Chen Zhiming Wang Ziqi Tian institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of ChinaChengdu 610054SichuanChina Key Laboratory of Advanced Fuel Cells and Electrolyzers Technology of Zhejiang Province Ningbo Institute of Materials Technology and EngineeringChinese Academy of SciencesNingbo 315201ZhejiangChina institute for Advanced Study Chengdu UniversityChengdu 610106SichuanChina

Oxygenated carbon materials exhibit outstanding electrocatalytic performance in the production of hydrogen peroxide(H2O2)through a two-electron oxygen reduction *** nature of the active functional group and underlying reaction mechanism,however,remain ***,a comprehensive workflow was established to identify the active sites from the numerous possible *** common hydroxyl group at the notched edge demonstrates a key role in the two-electron *** local chemical environment weakens the binding of OOH intermediate to substrate while enhancing interaction with solution,thereby promoting the H_(2)O_(2)*** increasing pH,the intramolecular hydrogen bond between OOH intermediate and hydroxyl decreases,facilitating OOH ***,the rise in selectivity with increasing potential stems from the suppression of the four-electron *** active site was further validated through *** by theoretical understanding,optimal performance was achieved with high selectivity(>95%)and current density(2.06 mA/cm^(2))in experiment.

关键词： First-principles calculation Oxygen reductionreaction Hydrogen peroxide production Fixed-potential method Oxygenated carbon materials

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Fast prototype and rapid construction of three-dimensional and multi-scaled pitcher for controlled drainage by systematic biomimicry

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International Journal of Extreme Manufacturing 2024年第3期6卷 489-503页

作者： Tao Shen Ning Li Shijie Liu Cunlong Yu Chengqi Zhang Kang Yang Xingfei Li Ruochen Fang Lei Jiang Zhichao Dong Research institute for Frontier Science Key Laboratory of Bio-Inspired Smart Interfacial Science and Technology of Ministry of Education BeijingSchool of ChemistryBeihang UniversityBeijing 100191People’s Republic of China CAS Key Laboratory of Bio-inspired Materials and Interfacial Science Technical Institute of Physics and ChemistryChinese Academy of SciencesBeijing 100190People’s Republic of China CAS Center for Excellence in Nanoscience Beijing Key Laboratory of Micro-nano Energy and SensorBeijing Institute of Nanoenergy and NanosystemsChinese Academy of SciencesBeijing 100083People’s Republic of China School of Future Technology&School of Nanoscience and Engineering University of Chinese Academy of SciencesBeijing 101407People’s Republic of China School of chemistry and Materials Science University of Science and Technology of China230026 HefeiAnhuiPeople’s Republic of China Suzhou institute for Advanced Research University of Science and Technology of China215123 SuzhouJiangsuPeople’s Republic of China State Key Laboratory of Precision Measuring Technology and Instruments Tianjin University300072 TianjinPeople’s Republic of China

Biomimetic materials that use natural wisdom to solve practical problems are developing *** trend for systematic biomimicry is towards in-situ characterization of naturalcreatures with high spatial ***,rapid reconstruction of digital twin models with the same complex features as the prototype is ***,it faces bottlenecks and limits in fast characterization and fabrication,precise parameter optimization,geometricdeviations control,and quality *** solve these challenges,here,we demonstrate astate-of-the-art method taking advantage of micro-computed tomography and three-dimensional printing for the fast characterization of the pitcher plant Nepenthes x ventrata and fabrication of its biomimetic model to obtain a superior drainage controller with multiscale structures withprecise surface morphology optimization and geometric deviation ***-rupture-based drainage dynamic and mechanisms are characterized by x-ray and high-speed videography,which determines the crucial structures for unique *** the optimized artificial pitchers are further developed into sustained drainage devices with novel applications,such as detection,reaction,and smoke control.

关键词： systematic biomimicry biomimetic materials Micro-CT drainage digital twin

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