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Cathodic corrosion as a facile and universal method for scalable preparation of powdery single atom electrocatalysts

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Nano Research 2024年第6期17卷 4943-4950页

作者： Rui Li Xiayan Yan Meng Liu Qingkai Zhao Jie Du Xinxin Tan Jingwen Ba Rongguang Zeng Wenhua Luo Jingsong Xu institute of Materials China Academy of Engineering PhysicsJiangyou 621907China Science and Technology on surface Physics and chemistry Laboratory Jiangyou 621908China

Top-down strategy has been widely applied for synthesis of metal single atom catalysts(SACs)via converting metal nanoparticles or bulk metals into atomically dispersed ***,we report a simple electrochemical atomic migration strategy for top-down synthesis of SACs via a facile cathodic corrosion process without involving high temperature or harsh *** of metal nanoparticles on cathode are firstly disbanded under high negative voltage,and emitted into the electrolyte in the form of atomic metal anions in Zintl *** escaped atomically dispersed metal species are then oxidized by water molecules and captured by the defects on the pre-added nitrogen doped carbon carriers in the *** cathodic corrosion strategy is confirmed to be suitable for scalable synthesis of kinds of metal SACs(e.g.,Pt,Pd,and Ir)on doped carbon ***,the as-prepared nitrogen doped carbon powder supported Pt SACs exhibit superior catalytic activity toward hydrogen evolution reaction(HER)with a low overpotential of 0.024 V at 10 mA·cm^(−2)and a low Tafel slope of 29.7 mV·dec^(−1)as well as a long-term durability.

关键词： cathodic corrosion top-down strategy powdery single atom catalysts hydrogen evolution reaction scalable synthesis

Nanodiamond:a promising metal-free nanoscale material in photocatalysis and electrocatalysis

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Rare Metals 2024年第8期43卷 3501-3552页

作者： Xiao-Wu Gao Zi-Wei Zhao Yang He Sai-Fei Fan Ke-Ran Jiao Si-Yu Lou Xin-Yue Han Peng-Fei Song Rong Cai Zhun Hu Zhong-Jie Jiang Yong-Jie Wang Jia-Qi Zhu Guangdong Provincial Key Laboratory of Semiconductor Optoelectronic Materials and Intelligent Photonic Systems School of ScienceHarbin Institute of Technology National Key Laboratory of Science and Technology on Advanced Composites in Special Environments Harbin Institute of Technology School of Advanced Technology Xi'an Jiaotong-Liverpool University Department of Biosciences Rice University institute of Industrial Catalysis School of Chemical Engineering and TechnologyXi'an Jiaotong University Guangzhou Key Laboratory for surface chemistry of Energy Materials New Energy Research Institute & Guangdong Engineering and Technology Research Center for Surface Chemistry of Energy MaterialsCollege of Environment and EnergySouth China University of Technology

Benefiting from its surface-rich functional groups,eco-friendliness,impressive electrochemical properties,excellent light absorption,structural tunability at the atomic/morphological level,and ultra-high stability under harsh conditions,nanodiamond has emerged as a promising carbon-based non-metallic material in the field of energy conversion such as electrocatalysis and ***,nanodiamond,as a new generation of green catalysts,can overcome the poisoning of catalysts by complex pollutants in advanced oxidation processes,thus effectively removing organic matter from water,which is unparalleled in reducing the cost of water purification and avoiding secondary cross-contamination of water by traditional heavy metal-based ***,we review the research and development of nanodiamonds as major electrocatalysts and photocatalysts for energy conversion and for air/water treatment for environmental *** relevant properties,trimming strategy,mechanistic understanding,and design principles of nanodiamond as a catalyst are described,as well as the challenges and prospects of this emerging field.

关键词： Carbon materials Nanodiamond Electrocatalysis Photocatalysis Energy conversion Pollutant treatment

surface reconstruction and structural transformation of twodimensional Ni-Fe MOFs for oxygen evolution in seawater media

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Nano Research 2024年第4期17卷 2429-2437页

作者： Liyuan Xiao Xue Bai Jingyi Han Tianmi Tang Siyu Chen Hui Qi Changmin Hou Fuquan Bai Zhenlu Wang Jingqi Guan institute of Physical chemistry College of ChemistryJilin UniversityChangchun 130021China The Second Hospital of Jilin University Changchun 130021China State Key Laboratory of Inorganic Synthesis and Preparative chemistry College of ChemistryJilin UniversityChangchun 130012China Laboratory of Theoretical and Computational chemistry Institute of Theoretical ChemistryCollege of ChemistryChangchun 130023China

As a four-electron transfer reaction,oxygen evolution reaction(OER)is limited by large overpotential and slow ***,we in-situ synthesized two-dimensional(2D)Ni-Fe metal-organic framework nanosheets on nickel foam(NixFe-TPA/NF,TPA=terephthalic acid)for oxygen evolution in alkaline and alkaline seawater *** 1 M KOH,Ni3Fe-TPA/NF shows a low overpotential(η10)of 189 mV at 10 mA·cm^(-2) and an ultra-low overpotential of only 260 mV at 500 mA·cm^(-2).In alkaline seawater,Ni3Fe-TPA/NF still provides impressive OER performance,with anη10 of 265 ***-situ Raman characterization results show that the phase transition occurs during the OER,and Ni3FeOOH with more oxygen vacancies is in-situ formed,reducing the OER energy *** functional theory(DFT)reveals that the synergy between Ni and Fe reduces the energy barrier and accelerates the rate-determining *** addition,the ultra-thin 2D sheet structure and the close combination of Ni3FeOOH and highly conductive NF support ensure the high catalytic OER ***,the surface reconstruction and structural modification strategy can be used to design and prepare high-performance OER electrocatalysts for energy-related applications.

关键词： density functional theory(DFT)calculation Ni3FeOOH oxygen evolution reaction seawater electrolysis surface reconstruction

Quick and automatic detection of co-seismic landslides with multifeature deep learning model

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Science China Earth Sciences 2024年第7期67卷 2311-2325页

作者： Wenchao HUANGFU Haijun QIU Peng CUI Dongdong YANG Ya LIU Bingzhe TANG Zijing LIU Mohib ULLAH College of Urban and Environmental Sciences Northwest UniversityXi'an 710127China institute of Mountain Hazards and Environment Chinese Academy of SciencesChengdu 610041China Shaanxi Key Laboratory of Earth surface System and Environmental Carrying Capacity Northwest UniversityXi'an 710127China institute of Earth surface System and Hazards Northwest UniversityXi'an 710127China

Co-seismic landslide detection is essential for post-disaster rescue and risk assessment after an earthquake ***,a variety of ground objects,including roads and bare land,have spectral characteristics similar to those of co-seismic landslides,making it difficult to gather information and assess their impact rapidly and ***,an automatic detection method based on a deep learning model,named ENVINet5,with multiple features(ENVINet5_MF)was proposed to solve this problem and improve the detection accuracy of co-seismic *** ENVINet5_MF method is advantageous for co-seismic landslide detection because it features a landslide gain index(LGI)that effectively eliminates the spectral interference of bare land and *** conducted two experiments using multi-temporal PlanetScope images acquired in Hokkaido,Japan,and Mainling,*** accuracy evaluation and rationality analysis show that ENVINet5_MF performed better than comparative methods and that the co-seismic landslide areas detected by ENVINet5_MF were the most consistent with ground reference *** findings of this study suggest that ENVINet5_MF can provide an efficient and accurate method for coseismic landslide detection to ensure a rapid response to co-seismic landslide disasters.

关键词： Co-seismic landslide Automatic detection Deep learning Landslide gain index PlanetScope images

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Plant life form determines spatiotemporal variability and climate response of plant seed rain in subtropical forests

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Forest Ecosystems 2024年第2期11卷 193-201页

作者： Yuyang Xie Zehao Shen Xuejing Wang Liu Yang Jie Zhang MOE Laboratory for Earth surface Processes Institute of EcologyCollege of Urban and Environmental SciencesPeking UniversityBeijing100871China

Spatiotemporal variation of seed rain reflects the response of plants in terms of their reproductive strategy to environmental *** this study,we collected seeds from four sites in the Dalaoling Nature Reserve,Hubei Province,China,between 2011 and 2014,measured seed output and seed mass as seed rain traits,and compared their interannual and elevational ***,we ran phylogenetic generalized mixed linear models(PGLMMs) to explore the effects of temperature and precipitation as well as interspecific differences on seed rain,and fitted the best regression models for seed rain *** of canopy and understory *** results showed no correlation between values of seed output and seed ***,the variation of the two traits showed significantly positive *** output of canopy species generally decreased with increasing elevation,and showed significant interannual difference;however,seed output of understory species and seed mass for both canopy and understory species did not show consistency tends along elevational or in interannual *** output was significantly affected by temperature and precipitation,while seed mass mainly varied due to interspecific *** explained more the variation of the seed output of canopy species than that of understory species,with R^(2) values of 43.0%and 29.9%,*** results suggested that canopy plants contributed more to the reproductive dynamics of the whole communities,and the canopy's buffer effect on the underground weakened the response of understory plants to weather variation in terms of their reproductive strategy.

关键词： Seed rain Seed output Seed mass Elevation Interannual variation Lifeform

Evolution exploration and structure prediction of Keggin-type group IVB metal-oxo clusters

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Chinese Chemical Letters 2024年第5期35卷 487-492页

作者： Run-Han Li Tian-Yi Dang Wei Guan Jiang Liu Ya-Qian Lan Zhong-Min Su School of chemistry South China Normal UniversityGuangzhou 510006China institute of Functional Material chemistry Faculty of ChemistryNortheast Normal UniversityChangchun 130024China institute of Theoretical chemistry Jilin UniversityChangchun 130023China

The fascinating chemical structure and broad application prospect of Keggin-type polyoxometalates(POMs)have attracted many chemists to explore and discover *** the traditional Keggin,larger metal atomic radius,higher metal coordinated numbers,lower metal valence states and other features allow the group IVB metal-based Keggin(IVB-Keggin)more space and unknown in terms of structure and ***,density functional theory(DFT)calculations were performed to explore the influences including cores,shells,caps,and terminal ligands,et *** IVB-Keggin,and analyze the possibility of novel structure *** the perspective of multi-layer onion-like clusters,molecular energy level,host-guest interaction energy,surface charge and covalent bond polarity can be further adjusted to achieve the oriented design of functional *** insights are expected to provide theoretical support for experimental synthesis,opening a new perspective to understand the growth of Keggin.

关键词： Keggin Metal-oxo clusters Group IVB Onion pattern DFT

Spray pyrolysis-derived W-doped MoSe2/rGO paper-like microspheres:optimization of microstructure and mesostructure for enhanced lithium storage

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Rare Metals 2024年第7期43卷 3019-3031页

作者： Wei Wang Jun-Yu Chen Jie Ouyang Hong Yin Ao-Jie Li Liang Chen Jun-Lin Huang Yu-Can Zhu Gang-Yong Li Zhao-Hui Hou Key Laboratory of Hunan Province for Advanced Carbon-based Functional Materials Hunan Institute of Science and Technology School of chemistry and Chemical Engineering Hunan Institute of Science and Technology Hunan Province Key Laboratory of Materials surface & Interface Science and Technology Material Science and Engineering SchoolCentral South University of Forestry and Technology International Iberian Nanotechnology Laboratory (INL)

Two-dimensional MoSe2is a promising candidate for lithium-ion battery ***,its conductivity and lithium storage volumetric effect still need to be *** this work,W-doped MoSe2/rGO paper-like microspheres are successfully prepared through ultrasonic spray pyrolysis,achieving optimization at both the microstructure and mesostructure to enhance the lithium storage performance of the ***,by utilizing the similar two-dimensional structure between MoSe2and rGO,self-assembly is achieved through spray pyrolysis,resulting in a well-defined van der Waals heterostructure at the interface on the microscale,enhancing the electron and ion transfer capability of the ***,the mesoscale paper-like microsphere morphology provides additional volume expansion buffering ***,W-doping not only increases the interlayer spacing of MoSe2（0.73 nm）,thereby reducing the diffusion resistance of Li+,but also allow for the modulation of the energy band structure of the *** functional theory（DFT） calculations confirm that W-doped MoSe2/rGO exhibits the narrowest bandgap（0.892 eV）.Therefore,the composite demonstrates excellent lithium storage performance,maintaining a specific capacity of 732.9 mAh·g-1after 300 cycles at a current density of 1 A·g-1.

关键词： Molybdenum selenide Heterostructure Microspheres Li-ion batteries Kinetics

Modularized viromimetic polymer nanoparticle vaccines(VPNVaxs) to elicit durable and effective humoral immune responses

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National Science Review 2024年第3期11卷 200-214页

作者： Zichao Huang Xinyu Zhuang Liping Liu Jiayu Zhao Sheng Ma Xinghui Si Zhenyi Zhu Fan Wu Ningyi Jin Mingyao Tian Wantong Song Xuesi Chen Key Laboratory of Polymer Ecomaterials Changchun Institute of Applied ChemistryChinese Academy of Sciences School of Applied chemistry and Engineering University of Science and Technology of China Changchun Veterinary Research institute Chinese Academy of Agricultural Sciences Jilin Biomedical Polymers Engineering Laboratory State Key Laboratory of Polymer Physics and chemistry Changchun Institute of Applied Chemistry Chinese Academy of Sciences

Virus-like particle(VLP) vaccines had shown great potential during the COVID-19 pandemic, and was thought to be the next generation of antiviral vaccine technology due to viromimetic structures. However,the time-consuming and complicated processes in establishing a current recombinant-protein–based VLP vaccine has limited its quick launch to the out-bursting pandemic. To simplify and optimize VLP vaccine design, we herein report a kind of viromimetic polymer nanoparticle vaccine(VPNVax), with subunit receptor-binding domain(RBD) proteins conjugated to the surface of polyethylene glycol-b-polylactic acid(PEG-b-PLA) nanoparticles for vaccination against SARS-CoV-2. The preparation of VPNVax based on synthetic polymer particle and chemical post-conjugation makes it possible to rapidly replace the antigens and construct matched vaccines at the emergence of different viruses. Using this modular preparation system, we identified that VPNVax with surface protein coverage of 20%–25% had the best immunostimulatory activity, which could keep high levels of specific antibody titers over 5 months and induce virus neutralizing activity when combined with an aluminum adjuvant. Moreover, the polymer nano-vectors could be armed with more immune-adjuvant functions by loading immunostimulant agents or chemical chirality design. This VPNVax platform provides a novel kind of rapidly producing and efficient vaccine against different variants of SARS-CoV-2 as well as other viral pandemics.

关键词： vaccine polymer nanomaterials SARS-CoV-2

Chronological Study of Coal-seam Water and its Implication on Gas Production in the South Qinshui Basin

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Acta Geologica Sinica(English Edition) 2024年第1期98卷 207-219页

作者： CHEN Biying FANG Lujia LANG Yunchao XU Sheng LIU Congqiang ZHANG Luyuan HOU Xiaolin institute of surface-Earth System Science School of Earth System ScienceTianjin UniversityTianjin 300072China institute of Earth Environments Chinese Academy of SciencesXi’an 710061China

The knowledge of the residence time of formation water is fundamental to understanding the subsurface flow and hydrological *** better identify the origin and evolution of coal seam water and its impact on gas storage and production,this study collected coalbed methane co-produced water in the southeast Qinshui Basin and detected chemical and isotopic compositions,especially 36Cl and 129I *** calculated tracer ages of 129I(5.2–50.6 Ma)and 36Cl(0.13–0.76 Ma)are significantly younger than the age of coal-bearing formation(Pennsylvanian-Cisuralian),indicating freshwater recharge after coal *** model that utilises 129I/I and 36Cl/Cl ratios to constrain the timing of recharge and the proportion of recharge water reveals that over 60%of pre-anthropogenic meteoric water entered coal seams since 10 Ma and mixed with residue initial deposition water,corresponding to the basin inversion in *** spatial distribution of major ion concentrations reveals the primary recharge pathway for meteoric water from coal outcrops at the eastern margin to the basin *** study demonstrates the occurrence of higher gas production rates from wells that accept water recharge in recent times and suggests the possible potential of the non-stagnant zones for high gas production.

关键词： CBM co-produced water iodine-129 chlorine-36 water chemistry Qinshui Basin