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Pd single atoms cooperate with S vacancies in ZnIn_(2)S_(4) nanosheets for photocatalytic pure-water splitting

Science China chemistry 2024年第3期67卷 855-861页

作者： Lin Sun Huiping Peng Fei Xue Shangheng Liu Zhiwei Hu Hongbo Geng Xiaozhi Liu Dong Su Yong Xu Xiaoqing Huang state key laboratory of physical chemistry of solid surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Guangzhou key laboratory of Low-Dimensional Materials and Energy Storage Devices Collaborative Innovation Center of Advanced Energy MaterialsSchool of Materials and EnergyGuangdong University of TechnologyGuangzhou 510006China Max Planck Institute for chemical Physics of solids Nothnitzer Strasse 40Dresden 01187Germany School of Materials Engineering Changshu Institute of TechnologyChangshu 215500China Beijing National laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of SciencesBeijing 100190China Innovation laboratory for Sciences and Technologies of Energy Materials of fujian province(IKKEM) Xiamen 361005China

Photocatalytic water splitting has emerged as a new frontier for converting solar energy to green H_(2) and value-added ***,great challenges still remain for developing efficient photocatalysts for pure water splitting without sacrificial *** this work,we demonstrate that doping hexagonal ZnIn_(2)S_(4)(ZIS) with Pd single atoms(Pd_(0.03)/ZIS) can serve as a highly efficient photocatalyst for pure water splitting to simultaneously produce H_(2) and H_(2)O_(2) without any sacrificial *** from aberration-corrected high-angle annular dark field scanning transmission electron microscopy,X-ray fine spectroscopy,insitu electron paramagnetic resonance and diffuse Fourier transform infrared spectroscopy reveal that doping ZIS with Pd single atoms facilitates the formation of S vacancies(S_(v)),where the photogenerated electrons can transfer to Pd single atoms,as a result of enhanced separation of electron-hole pairs and improved photocatalytic ***,Pd_(0.03)/ZIS displays a stoichiometric ratio of H_(2) and H_(2)O_(2) with the productivity of 1,037.9 and 1,021.4μmol g^(-1)h^(-1),respectively,which has largely outperformed pure ZIS and other reported catalysts for pure water *** work provides an efficient photocatalyst for water splitting to produce H_(2) and H_(2)O_(2),which may attract rapid interest in materials science,chemistry,and heterogeneous catalysis.

关键词： ZnIn_(2)S_(4) Pd single atom S vacancy pure water splitting H_(2)O_(2)

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Bioinspired nanofluidic iontronics for brain-like computing

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Nano Research 2024年第2期17卷 503-514页

作者： Lejian Yu Xipeng Li Chunyi Luo Zhenkang Lei Yilan Wang Yaqi Hou Miao Wang Xu Hou state key laboratory of physical chemistry of solid surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Institute of Artificial Intelligence Xiamen UniversityXiamen 361005China Department of Physics Research Institute for Biomimetics and Soft MatterFujian Provincial Key Laboratory for Soft Functional Materials ResearchJiujiang Research InstituteCollege of Physical Science and TechnologyXiamen UniversityXiamen 361005China The Higher Educational key laboratory for Biomedical Engineering of fujian province Department of BiomaterialsResearch Center of Biomedical Engineering of XiamenCollege of MaterialsXiamen UniversityXiamen 361005China The Institute of Flexible Electronics(IFE Future Technologies)Xiamen UniversityXiamen 361005China Binzhou Institute of Technology Binzhou 256600China Innovation laboratory for Sciences and Technologies of Energy Materials of fujian province(IKKEM) Xiamen 361102China Engineering Research Center of Electrochemical Technologies of Ministry of Education Xiamen UniversityXiamen 361005China

The human brain performs computations via a highly interconnected network of *** inspiration from the information delivery and processing mechanism of the human brain in central nervous systems,bioinspired nanofluidic iontronics has been proposed and gradually engineered to overcome the limitations of the conventional electron-based von Neumann architecture,which shows the promising potential to enable efficient brain-like *** and tunable nanofluidic ion transport behaviors and spatial confinement show promising controllability of charge carriers,and a wide range of structural and chemical modification paves new ways for realizing brain-like ***,a comprehensive framework of mechanisms and design strategy is summarized to enable the rational design of nanofluidic systems and facilitate the further development of bioinspired nanofluidic *** review provides recent advances and prospects of the bioinspired nanofluidic iontronics,including ion-based brain computing,comprehension of intrinsic mechanisms,design of artificial nanochannels,and the latest artificial neuromorphic functions ***,the challenges and opportunities of bioinspired nanofluidic iontronics in the pioneering and interdisciplinary research fields are proposed,including brain–computer interfaces and artificial neurons.

关键词： human brain ion transport nanofluidics brain-like computing memristive effect

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Hierarchical Homochiral Assembly of Polyhedral Cage-Type Nanoclusters

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CCS chemistry 2024年第10期6卷 2537-2548页

作者： Cheng-Long Deng Bao-Liang Han Ze-Yu Liu Zhong-Hua Pan Jiao He Yu-Long Li Zhi-Lin Yang Geng-Geng Luo Chen-Ho Tung Di Sun Lan-Sun Zheng key laboratory of Environmentally Friendly Function Materials Ministry of EducationCollege of Materials Science and EngineeringHuaqiao UniversityXiamen 361021 School of chemistry and chemical Engineering State Key Laboratory of Crystal MaterialsShandong UniversityJi’nan 250100 College of physical Science and Technology Xiamen UniversityXiamen 361005 College of chemistry and Environmental Engineering Sichuan University of Science and EngineeringZigong 643000 state key laboratory for physical chemistry of solid surfaces Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005

Hierarchical chiral self-assembly is of profound significance for biomolecules for their biological ***-precise metal nanoclusters(NCs)offer better opportunities to construct hierarchical ***,achieving hierarchical homochiral assembly of nanocrystals protected by achiral ligands has proven to be a formidable task,with existing examples primarily limited to heterochiral *** we put forward a hierarchical assembly strategy towards precisely fabricating highly ordered homochiral ***,clusterin-nanocage type copper-hydride NCs act as synthons,of which entity is featured with a hexagonal close-packed Cu_(9)kernel embedded in a C_(3)-symmetric trigonal-prismatic metallacage,leading to a chiral core-shell primary structure with either P or M *** four homochiral NCs combined with guests through synergistic noncovalent interactions spontaneously organize into a supramolecular tetrahedral secondary structure within a unit ***,these nanoscopic supramolecular motifs pack into tertiary hierarchical superlattice of chiral cubic crystalline ***,the crystalline material shows excellent robustness,and fascinating blueexcitable near-infrared thermally activated delayed fluorescence *** work not only exhibits that nanocage-type NCs can be smart as proteins to translate chiral primary structure into tertiary chiral hierarchical complexity,but also provides new insights into structure-to-superstructure,enabling bottom-up creation of higher-level hierarchical homochiral superlattice structures.

关键词： polyhydrido copper nanoclusters chiral polyhedral metallacage hierarchical homochiral assembly thermally activated delayed fluorescence

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Dynamic asymmetric mechanical responsive carbon nanotube fiber for ionic logic gate

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Chinese chemical Letters 2024年第6期35卷 249-253页

作者： Pei Cao Yilan Wang Lejian Yu Miao Wang Liming Zhao Xu Hou state key laboratory of physical chemistry of solid surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Innovation laboratory for Sciences and Technologies of Energy Materials of fujian province(IKKEM) Xiamen 361005China The Higher Educational key laboratory for Biomedical Engineering of fujian province Department of BiomaterialsResearch Center of Biomedical Engineering of XiamenCollege of MaterialsXiamen UniversityXiamen 361005China key laboratory of Multifunctional Nanomaterials and Smart Systems Advanced Materials DivisionSuzhou Institute of Nano-Tech and Nano-BionicsChinese Academy of SciencesSuzhou 215123China Institute of Artificial Intelligence Xiamen UniversityXiamen 361005China Department of Physics Research Institute for Biomimetics and Soft MatterFujian Provincial Key Laboratory for Soft Functional Materials ResearchJiujiang Research InstituteCollege of Physical Science and TechnologyXiamen UniversityXiamen 361005China Engineering Research Center of Electrochemical Technologies of Ministry of Education Xiamen UniversityXiamen 361005China

Inspired by biological ion channels,numerous artificial asymmetric ion channels have been synthesized to facilitate the fabrication of ionic ***,the creation of biomimetic asymmetric ion channels necessitates expensive scientific apparatus and intricate material processing procedures,which constrains its advancement within the realm of ionic *** this study,we have devised dynamic asymmetric ion channels with mechanical responsiveness by combining polymers of varying elastic modulus along the longitudinal axis of carbon nanotube fiber(CNTF).The ion rectification can be modulated via the disparate response of CNTF-based ion channels to mechanical *** have effectively employed these asymmetric ion channels with mechanical sensitivity in the design of a logic gate device,achieving logic operations such as“AND”and“OR”.The conception of these dynamic asymmetric ion channels with mechanical sensitivity offers a straightforward,cost-effective,and versatile approach for generating ion channels,highlighting their potential application in intricate,highly integrated ionic circuits.

关键词： Carbon nanotubes fibers Mechanical response Rectification effect Ionic logic gate

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Deciphering molecular response of cell-cell interactions at the single-cell level by precise on-demand cell assembly

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Science Bulletin 2024年第15期69卷 2342-2345页

作者： Weizhi Liu Shanqing Huang Ye Guo Xingrui Li He Dong Juan Li Chaoyong Yang Zhi Zhu state key laboratory of physical chemistry of solid surfaces Key Laboratory for Chemical Biology of Fujian ProvinceThe Key Laboratory of Spectrochemical Analysis&Instrumentation(Ministry of Education)Department of Chemical BiologyCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Discipline of Intelligent Instrument and Equipment Xiamen UniversityXiamen 361005China Xinjiang key laboratory of Biological Resources and Genetic Engineering College of Life Science and TechnologyXinjiang UniversityUrumqi 830000China

Multicellular systems rely on the interactions between cells to coordinate cell signaling and regulate cell functions [1]. Understanding the mechanism of cell–cell interactions (CCIs) is critical to many physiological and pathological processes, such as embryogenesis,differentiation, cancer metastasis, and immunological interactions.

关键词： metastasis precise interactions

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Editorial:special topic on biomaterials and bioinspired materials

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Science China Materials 2024年第8期67卷 2373-2375页

作者： Mingjie Liu Xu Hou Dan Wang key laboratory of Bio-Inspired Smart Interfacial Science and Technology of Ministry of Education School of ChemistryBeihang UniversityBeijing 100191China International Research Institute for Multidisciplinary Science Beihang UniversityBeijing 100191China state key laboratory of physical chemistry of solid surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Research Institute for Biomimetics and Soft Matter Fujian Provincial Key Laboratory for Soft Functional Materials ResearchCollege of Physical Science and TechnologyXiamen UniversityXiamen 361005China state key laboratory of Biochemical Engineering Key Laboratory of Biopharmaceutical Preparation and DeliveryInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China

Biomaterials have been persistently focused owing to their intricate design and efficient *** order to satisfy the demands of life and medical sciences,large amounts of biomaterials capable of interacting with living systems have been created,thereby achieving the diagnosis,treatment or replacement of cells,tissues,and *** continuous evolution for billions of years,living organisms have eventually developed sophisticated multi-scale structures with diverse biological functions to adapt to the external environment.

关键词： organs diagnosis biomaterials

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Efficient and stable PtFe alloy catalyst for electrocatalytic methanol oxidation with high resistance to CO

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Journal of Energy chemistry 2024年第3期90卷 327-336,I0008页

作者： Qian Yang Sifan Zhang Fengshun Wu Lihua Zhu Guang Li Mingzhi Chen An Pei Yingliang Feng Jiangxi Provincial key laboratory of Functional Molecular Materials chemistry College of Chemistry and Chemical EngineeringFaculty of Materials Metallurgy and ChemistryJiangxi University of Science and TechnologyGanzhou 341000JiangxiChina College of chemistry and chemical Engineering Xiamen UniversityXiamen 361005FujianChina

Direct methanol fuel cells(DMFC) are widely considered to be an ideal green energy conversion device but their widespread applications are limited by the high price of the Pt-based catalysts and the instability in terms of surface CO toxicity in long-term ***,the PtFe alloy nanoparticles(NPs) with small particle size(~4.12 nm) supported on carbon black catalysts with different Pt/Fe atomic ratios(Pt_(1)Fe_(2)/C,Pt_(3)Fe_(4)/C,Pt_(1)Fe_(1)/C,and Pt_(2)Fe_(1)/C) are successfully prepared for enhanced anti-CO poisoning during methanol oxidation reaction(MOR).The optimal atomic ratio of Pt/Fe for the MOR is 1:2,and the mass activity of Pt_(1)Fe_(2)/C(5.40 A mg_(Pt)^(-1)) is 13.5 times higher than that of conventional commercial Pt/C(Pt/C-JM)(0.40 A mg_(Pt)^(-1)).The introduction of Fe into the Pt lattice forms the PtFe alloy phase,and the electron density of Pt is reduced after forming the PtFe ***-situ Fourier transform infrared results indicate that the addition of oxyphilic metal Fe has reduced the adsorption of reactant molecules on Pt during the *** doping of Fe atoms helps to desorb toxic intermediates and regenerate Pt active sites,promoting the cleavage of C-O bonds with good selectivity of CO_(2)(58.1%).Moreover,the Pt_(1)Fe_(2)/C catalyst exhibits higher CO tolerance,methanol electrooxidation activity,and long-term stability than other Pt_(x)Fe_(y)/C catalysts.

关键词： Alloy catalyst PtFe Methanol oxidation In-situ FTIR CO resistance

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Surface Ligand Evolution:Sulfur-Directed Covalent Bonding of PPh_(3) on Pd_(4)S with Improved Semi-hydrogenation of Terminal Alkynes

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Precision chemistry 2024年第5期2卷 200-207页

作者： Wentong Jing Shiguang Mo Weijie Zhang Wenting Zhou Kunlong Liu Jie Wei Ruixuan Qin Nanfeng Zheng New Cornerstone Science laboratory State Key Laboratory for Physical Chemistry of Solid SurfacesCollaborative Innovation Center of Chemistry for Energy Materialsand National&Local Joint Engineering Research Center of Preparation Technology of NanomaterialsCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China China Resources Cement Technology R&D(Guangxi)Co Ltd. Nanning 530008China Innovation laboratory for Sciences and Technologies of Energy Materials of fujian province(IKKEM) Xiamen 361102China

Surface modification of metallic nanocatalysts with organic ligands has emerged as an effective strategy to enhance catalytic selectivity,although offten at the expense of catalytic *** this study,we demonstrate a compelling approach by surface modifying Pd2S nanocrystals with PPhz ligands,resulting in a catalyst with excellent catalytic activity and durable selectivity for the semi-hydrogenation of terminal *** and theoretical investigations reveal that the presence of S sites on the Pd surface directs PPh_(3) ligands to preferentially form covalent bonds with S,creating distinctive surface S=PPh_(3) *** configuration induces a partial positive charge on Pd,facilitating hydrogen transfer and thus promoting catalytic ***,the covalent bond between the ligand and catalyst surface forms a robust network,ensuring ligand stability and increasing the hydrogenation energy barrier of ***,the Pd_(4)S@PPhz catalyst exhibits an improved catalytic selectivity with durability in terminal alkyne *** study introduces an effective strategy for designing selective hydrogenation catalysts with an enhanced performance.

关键词： Pd nanocatalysts surface modification selective hydrogenation catalytic stability alkyne semi-hydrogenation

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MOF-derived Cu embedded into N-doped mesoporous carbon as a robust support of PdAu nanocatalysts for ethanol electrooxidation

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Rare Metals 2024年第3期43卷 1083-1094页

作者： Yu-Fu Huang Peng Wu Jun-Ping Tang Jian Yang Jing Li Shuai Chen Xue-Ling Zhao ChengChen Bin-Wei Zhang Yan-Yun Ma Wei-Heng Shi Dong-Hai Lin Shi-Gang Sun School of Energy and Materials Shanghai Engineering Research Center of Advanced Thermal Functional MaterialsShanghai Key Laboratory of Engineering Materials Application and EvaluationShanghai Polytechnic UniversityShanghai201209China state key laboratory of physical chemistry of solid surfaces Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen361005China School of chemistry and chemical Engineering Chongqing UniversityChongqing401331China Center of Advanced Energy Technology and Electrochemistry Institute of Advanced Interdisciplinary StudiesChongqing UniversityChongqing400044China Institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesSoochow UniversitySuzhou215123China Department of Materials Science and Engineering Drexel UniversityPhiladelphiaPA19104USA

Metal-organic frameworks(MOFs)h ave attracted widespread attention due to their large surface area and porous *** designing the nanostructures of MOFs to promote their application in ethanol electrooxidation is still a ***,a novel Cu-NCNs(Cu-nitrogen-doped carbon nanotubes)support was synthesized by pyrolysis of melamine(MEL)and Cu-ZIF-8 together,and then,Pd-Au nanoalloys were loaded by sodium borohydride reduction method to prepare PdAu@Cu-NCNs *** generating mesoporous carbon with high specific surface area and favorable electron and mass transport can be used as a potential excellent carrier for PdAu *** addition,the balance of catalyst composition and surface structure was tuned by controlling the content of Pd and ***,the best-performed Pd_(2)Au_(2)@Cu-NCN-1000-2(where 1000 means the carrier calcination temperature,and 2 means the calcination constant temperature time)catalyst exhibits better long-term stability and electrochemical activity for ethanol oxidation in alkaline media(4.80 A·mg^(-1)),which is 5.05 times higher than that of commercial Pd/C(0.95 A·mg^(-1)).Therefore,this work is beneficial to further promoting the application of MOFs in direct ethanol fuel cells(DEFCs)and can be used as inspiration for the design of more efficient catalyst support structures.

关键词： Metal-organic frameworks(MOFs) N-doped Mesoporous carbon PdAu Ethanol electrooxidation

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Phase engineering of Pd–Te nanoplates via potential energy trapping

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eScience 2024年第2期4卷 117-126页

作者： Mengjun Wang Jun Jia Hao Yan Guang Li Qiming Hong Yuzheng Guo Yong Xu Xiaoqing Huang state key laboratory of physical chemistry of solid surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen361005China Guangzhou key laboratory of Low-Dimensional Materials and Energy Storage Devices Collaborative Innovation Center of Advanced Energy MaterialsSchool of Materials and EnergyGuangdong University of TechnologyGuangdong510006China School of Electrical Engineering and Automation Wuhan UniversityHubei430072China Testing and Analysis Center College of Chemistry and Chemical EngineeringXiamen UniversityXiamen361005China Innovation laboratory for Sciences and Technologies of Energy Materials of fujian province(IKKEM) Xiamen361005China

Phase modulation of noble metal alloys(NMAs)is critically important in nanoscience since the distinct atomic arrangements can largely determine their physicochemical ***,the precise modulation of NMAs is formidably challenging,because thermodynamically stable phases are generally preferential compared to those metastable ***,we proposed a potential energy trapping strategy for phase modulation of Pd–Te alloys with ***,ethylene glycol can increase the energy barrier for both Pd leaching and Te introduction,forming metastable Pd20Te7 ***,N,N-dimethylformamide is unable to trap metastable phase,inducing the phase evolution to thermodynamically stable PdTe phase,and the precise phase modulation was realized including Pd20Te7,PdTe and PdTe2 *** Pd–Te alloys displayed phase-dependent formic acid oxidation catalytic performance with PdTe phase showing the *** work proposes a strategy for creating metastable phase with potential energy trap,which may deepen the understanding of phase engineering for noble metal-based nanocrystals.

关键词： Potential energy trap Phase modulation Metastable Pd-Te alloys

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