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Rapid and controllable in-situ self-assembly of main-group metal nanofilms for highly efficient CO_(2)electroreduction to liquid fuel in flow cells

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Nano research 2024年第6期17卷 5718-5725页

作者： Miao Wang Huaizhu Wang Yaoda Wang Junchuan Liang Mengfei Zhu Jiarui Li Zuoxiu Tie Zhong Jin State Key laboratory of Coordination chemistry MOE Key Laboratory of Mesoscopic ChemistryMOE Key Laboratory of High Performance Polymer Materials and TechnologyJiangsu Key Laboratory of Advanced Organic MaterialsTianchang New Materials and Energy Technology Researc

The electrocatalytic reduction of CO_(2)is a promising pathway to generate renewable fuels and ***,its advancement is impeded by the absence of electrocatalysts with both high selectivity and ***,we present a scalable in-situ thermal evaporation technique for synthesizing series of Bi,In,and Sn nanofilms on carbon felt(CF)substrates with a high-aspect-ratio *** resulting main-group metal nanofilms exhibit a homogeneously distributed and highly exposed catalyst surface with ample active sites,thereby promoting mass transport and ad-/desorption of reaction *** from the unique fractal morphology,the Bi nanofilms deposited on CF exhibit optimal catalytic activities for CO_(2)electroreduction among the designed metal nanofilms electrodes,with the highest Faradaic efficiency of 96.9%for formate production at−1.3 V *** hydrogen electrode(RHE)in *** an industrially relevant current density of 221.4 mA·cm−2 in flow cells,the Bi nanofilms retain a high Faradaic efficiency of 81.7%at−1.1 V(***)and a good long-term stability for formate ***,a techno-economic analysis(TEA)model shows the potential commercial viability of electrocatalytic CO_(2)conversion into formate using the Bi nanofilms *** results offer a green and convenient approach for in-situ fabrication of stable and inexpensive thin-film catalysts with a fractal structure applicable to various industrial settings.

关键词： CO_(2)electroreduction non-noble metal nanofilms flow cells efficiency and selectivity techno-economic analysis

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Probing the interaction between asphaltene-wax and its effects on the crystallization behavior of waxes in heavy oil via molecular dynamics simulation

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Petroleum Science 2024年第4期21卷 2839-2848页

作者： Yong Hu Xi Lu Hai-Bo Wang Ji-Chao Fang Yi-Ning Wu Jian Fang Sun SINOPEC Petroleum Exploration and Production research Institute Shandong Key laboratory of Oilfield chemistry School of Petroleum Engineering China University of Petroleum (East China)

High content of asphaltenes and waxes leads to the high pour point and the poor flowability of heavy oil,which is adverse to its efficient development and its transportation in *** the interaction mechanism between asphaltene-wax is crucial to solve these problems,but it is still *** this paper,molecular dynamics simulation was used to investigate the interaction between asphaltenewax and its effects on the crystallization behavior of waxes in heavy *** show that molecules in pure wax are arranged in a paralleled *** wax molecules in heavy oil,which are close to the surface of asphaltene aggregates,are bent and arranged *** the mass fraction of asphaltenes in asphaltene-wax system(ωasp) is 0-25 wt%,the attraction among wax molecules decreases and the bend degree of wax molecules increases with the increase of ω*** ωaspincreases from 0 to 25 wt%,and the attraction between asphaltene-wax is stronger than that among *** causes that the wax precipitation point changes from 353 to 333 *** the ωaspincreases to 50 wt%,wax molecules are more dispersed owing to the steric hindrance of asphaltene aggregates,and the interaction among wax molecules transforms from attraction to *** causes that the ordered crystal structure of waxes can't be formed at normal ***,the asphaltene,with the higher molecular weight or the more hetero atoms,has more obvious inhibition to the formation of wax ***,resins also have an obvious inhibition on the wax crystal due to the formation of asphalteneresin aggregates with a larger *** results reveal the interaction mechanism between asphaltene-wax,and provide useful guidelines for the development of heavy oil.

关键词： Heavy oil Interaction mechanism Asphaltenes Waxes Molecular dynamics

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Highly selective adsorption of rhenium by amyloid-like protein material

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Science China(Technological Sciences) 2024年第5期67卷 1417-1430页

作者： MUHAMMAD Arif YANG QingMin KANWAL Aisha ZHAO Jian NAWAZ Mohsan REN Hao YANG Peng Key laboratory of Applied Surface and Colloid chemistry Ministry of Education Xi’an Key laboratory of Polymeric Soft Matter International Joint Research Center on Functional Fiber and Soft Smart TextileSchool of Chemistry and Chemical EngineeringShaanxi Normal UniversityXi’an710119China School of chemistry and Chemical Engineering Northwestern Polytechnical UniversityXi’an710072China

Rhenium separation from molybdenum in molybdenite minerals and waste leachate has become an emerging *** this challenge,we prepared a set of protein-based alkylamine/alkylammonium salts complexes as extractants for selective uptake of rhenium from molybdenum,where the protein component turned into the insoluble amyloid-like structure when its internal disulfide bonds were reduced,namely phase-transition *** them,the phase-transited lysozyme and methyletrioctyleammonium chloride complex(PTL-N263)exhibited the most efficient adsorption at the alkaline condition for the electrostatic interaction between negatively charged metal ions with positively charged center(R_(4)N^(+))in N263,where negatively charged protein residues hindered the ion exchange of Cl^(-)in N263 for larger size Mo species(Mo_(7)O_(24)^(6-))than smaller size Re species(ReO^(4-)).The adsorption follows the Freundlich model and pseudo-second-order kinetics,which exhibits toplevel adsorption performance with a maximum adsorption capacity of 124 mg/g and a separation factor(β_(Re/Mo))of 2.78×10^(3)for *** adsorption capacity per unit area(57.2 mg/(g m^(2)))is 1.6–41 times higher than previously reported adsorbents,and the cost for adsorbing 1 g of Re(VII)is$1.07,indicating its industrial *** adsorption strategy can be applied to separating Re from Mo in binary solutions and industrial wastewater with other competing ions.

关键词： amyloid phase-transited lysozyme selective adsorption rhenium waste leachate solution

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Advances of graphdiyne-supported metal catalysts in thermocatalytic reactions

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Nano research 2024年第4期17卷 2223-2233页

作者： Jia Yu Yida Yang Yuliang Li Changyan Cao Weiguo Song Beijing National laboratory for Molecular Sciences CAS Research/Education Center for Excellence in Molecular SciencesLaboratory of Molecular Nanostructures and NanotechnologyInstitute of ChemistryChinese Academy of SciencesBeijing 100190China School of Chemical Sciences University of Chinese Academy of SciencesBeijing 100049China Beijing National laboratory for Molecular Sciences CAS Research/Education Center for Excellence in Molecular SciencesLaboratory of organic solidsInstitute of ChemistryChinese Academy of SciencesBeijing 100190China

Supported metal catalysts are widely used in the modern chemical *** electronic interaction between supports and active components is of great significance for heterogeneous ***(GDY),a new type of carbon allotrope with sp-hybridized carbon atoms,πconjugate structure,and electron transmission capability,is a promising candidate as catalyst *** years have witnessed the rapid progress of GDY-supported metal catalysts for different catalysis *** that most processes in the current chemical industry are thermocatalytic reactions,we herein give an overview about the advances and particular characteristics of GDY-supported catalysts in these *** geometric structure and electronic properties of GDY are first ***,the synthesis methods for GDY-supported metal catalysts and their applications in thermocatalytic reactions are discussed,in which the effect of electronic interaction on catalytic performance is ***,the current challenges and future directions of GDY-supported metal catalysts for thermocatalysis are *** is expected that this review will enrich our understanding of the advances of GDY as a superior support for metal catalysts in thermocatalytic reactions.

关键词： graphdiyne metal catalysts thermocatalytic reactions heterogeneous catalysis

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Polyoxometalate as the assembly material to self-assembled Ni(OH)_(2) nanosheets with electrocatalytic performance

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Nano research 2024年第8期17卷 7061-7067页

作者： Danyang He Tianyang Li Luozhen Jiang Fei Wang Zihao Xing Nan Wang Zhiyu Jia Guo-Yu Yang Key laboratory of Cluster Science Ministry of EducationSchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 100081China Shanghai Advanced research Institute Chinese Academy of ScienceShanghai 201210China Key laboratory of Polyoxometalate and Reticular Material chemistry of Ministry of Education Facluty of ChemistryNortheast Normal UniversityChangchun 130024China

Developing non-noble metal-based electrocatalyst with high catalytic activity is essential for advancing hydrogen energy *** study introduces a hydrothermal method for synthesizing order Ni(OH)_(2) nanosheets,with H_(3)O_(40)PW_(12)(denoted as PW_(12))loaded onto reduced graphene oxide(rGO)coated on nickel foam(referred to as PW_(12)-Ni(OH)_(2)/rGO).This method contrasts with the electrodeposition of Ni(OH)_(2),where PW_(12) is added to the synthetic system to direct the assembly and morphology of the Ni(OH)_(2) through a hydrothermal *** this work,the nickel foam acts dual roles as both the substrate and the source of nickel for the formation of Ni(OH)_(2).The PW_(12)-Ni(OH)_(2)/rGO nanosheets,when successfully prepared and loaded onto the nickel foam(NF),exhibited superior electrocatalytic activity for the hydrogen evolution reaction(HER)in an alkaline electrolyte,achieving a current density of 10 mA·cm^(-2) at an overpotential of 69 ***,we endeavored to expand the application of this material towards the oxygen evolution reaction(OER)by preparing PW_(12)-(Fe/Co)Ni(OH)_(2)/rGO through the addition of metal *** nanocomposite displayed outstanding electrocatalytic activity in alkaline electrolytes,with a current density of 10 mA·cm^(-2)at an overpotential of 211 mV,and demonstrated excellent stability over a 50 h period in a 1 M KOH *** results presented in this paper offer an effective strategy for the preparation of polyoxometalate-based inorganic materials with diverse functionalities,applicable to both HER and OER.

关键词： polyoxometalate Ni(OH)_(2) assembly hydrogen evolution reaction oxygen evolution reaction

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Recent advances in quantifying the inactive lithium and failure mechanism of Li anodes in rechargeable lithium metal batteries

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Journal of Energy chemistry 2024年第9期96卷 226-248页

作者： Mingming Tao Junning Chen Hongxin Lin Yingao Zhou Danhui Zhao Peizhao Shan Yanting Jin Yong Yang State Key laboratory for Physical chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy Materials and Department of ChemistryCollege of Chemistry and Chemical EngineeringTan Kah Kee Innovation Laboratory(IKKEM)Xiamen UniversityXiamen 361005FujianChina School of Engineering Westlake UniversityHangzhou 310024ZhejiangChina School of Energy research Xiamen UniversityXiamen 361005FujianChina

Lithium metal is considered as the ultimate anode material for the next generation of high-energy density ***,non-uniform lithium dendrite growth,serious electrolyte consumption,and significant volume changes during lithium deposition/stripping processes lead to sustained accumulation of inactive lithium and poor cycling *** the formation and evolution of inactive lithium under different conditions and fully evaluating the complex failure modes are the key issues in this challenging *** article comprehensively reviews recent research progress on the quantification of formation and evolution of inactive lithium detected by different quantitative techniques in rechargeable lithium metal *** key research challenges such as failure mechanism,modification strategies and operando characterization of lithium metal anodes are systematically summarized and *** review provides a new angle of view to understand failure mechanism of lithium metal anodes and inspiration and guidance for the future development of rechargeable lithium metal batteries.

关键词： Lithium metal anodes Inactive lithium Quantitative technique Failure mechanism

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Manipulating fast Li_(2)S redox via carbon confinement and oxygen defect engineering of In_(2)O_(3)for lithium-sulfur batteries

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Nano research 2024年第6期17卷 5179-5187页

作者： Jinlei Qin Rui Wang Zilong Yuan Pei Xiao Deli Wang Key laboratory of Material chemistry for Energy Conversion and Storage Ministry of EducationHubei Key Laboratory of Material Chemistry and Service FailureSchool of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan 430074China

Lithium-sulfur(Li-S)batteries have been considered as promising energy storage systems due to the merits of high energy density and low ***,the lithium polysulfides(LiPSs)diffusion and sluggish redox kinetics hamper t... 详细信息

关键词： Li-S batteries nitrogen-doped carbon confinement oxygen vacancies bidirectional Li_(2)S redox

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A highly reduced Mo_(74) polyoxometalate featuring high proton conductivity accessed by building block strategy

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Science China chemistry 2024年第3期67卷 862-868页

作者： Shi-Yi Liu Xue-Xin Li Wei-Chao Chen Kui-Zhan Shao Xin-Long Wang Chao Qin Zhong-Min Su Key laboratory of Polyoxometalate and Reticular Material chemistry of Ministry of Education Department of ChemistryNortheast Normal UniversityChangchun 130024China State Key laboratory of Supramolecular Structure and Materials Institute of Theoretical ChemistryCollege of ChemistryJilin UniversityChangchun 130021China

Highly reduced polyoxometalates(POMs) are predicted to be used as rather high energy density materials;however,it still suffers from the limited cluster species and reduction *** we demonstrate that it is possible to employ the building block strategy to generate a highly reduced polyoxomolybdate(C_(2)H_(8)N)_(14)(NH_(4))_(4)H_(14)[Mo_(48)-ⅤMo_(26)ⅥO_(202)(OH)_(12)(SO_(4))_(6)]·46H_(2)O(Mo_(74)).The fundamental Mo-based{Mo_x}(x=4,5,and 6) building blocks,which are templated by tetra-coordinated anions{MoO_(4)}or{SO_(4)},not only lay foundation for the formation of Mo_(74) featuring an unprecedented reduction ratio of 65%,but also give rise to SBBs-mediated(secondary building blocks) supramolecular dense packing interactions among the isolated Mo_(74) clusters that are favorable for proton ***,high proton conductivity(2.04×10^(-2)S cm^(-1)) had been realized at 50℃ and 90% relative humidity,revealing one of the well-known POMs-based crystalline proton conducting *** result highlights that this building block approach possesses great potential in producing highly reduced POM systems that can achieve controllable reduced ratio and desirable properties.

关键词： polyoxometalate building block molybdenum highly reduced state proton conduction

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Degradation mechanisms and stabilization strategies of ruthenium-based catalysts for OER in the proton exchange membrane water electrolyzer

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Progress in Natural Science:Materials International 2024年第1期34卷 207-222页

作者： Ming Yang Hongxiang Wu Zhaoping Shi Yibo Wang Jiahao Yang Jing Ni Pengbo Wang Yuqing Cheng Ziang Wang Meiling Xiao Changpeng Liu Wei Xing laboratory of Advanced Power Sources Changchun Institute of Applied Chemistry Chinese Academy of Sciences School of Applied chemistry and Engineering University of Science and Technology of China Jilin Province Key laboratory of Low Carbon Chemical Power Sources State Key laboratory of Electroanalytical chemistry Changchun Institute of Applied Chemistry Chinese Academy of Sciences

Designing economical oxygen evolution reaction(OER) electrocatalysts with high activity and long-term stability is essential to promote the scale-up applications of proton exchange membrane water electrolyzer(PEMWE) for hydrogen production. Ruthenium(Ru)-based materials with high intrinsic activity are hailed as the most promising catalysts, but still infeasible for practical application considering their long unresolved poor stability(only dozens of lifespan). Thus, tremendous efforts have been devoted to uncovering the degradation mechanisms and developing stabilization strategies for the Ru-based catalysts. In this review, starting from summarizing the fundamental understanding of deactivation mechanisms, a picture of the stability issue of Ru-based catalysts is proposed, which is followed by a detailed discussion on the recently developed strategies and progress made on enhancing durability. Finally, insights on the prospects for the future development of stable and practical Rubased OER catalysts are provided.

关键词： OER Ru-based catalysts PEMWE Degradation mechanisms Stabilization strategies

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Dimensional reduction enhances photocatalytic carbon dioxide reduction performance of metal-organic frameworks

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Nano research 2024年第5期17卷 3653-3659页

作者： Kaiyue Ma Jixin Li Jinlu Liu Chunguang Li Zhan Shi Shouhua Feng State Key laboratory of Inorganic Synthesis and Preparative chemistry College of ChemistryJilin UniversityChangchun 130012China

Metal-organic frameworks(MOFs)have shown significant potential as *** has been widely assumed that all catalytic active sites within MOFs are functional in photocatalytic reactions but for a three-dimensional MOF,whether the internal catalytic active sites can effectively absorb light and actively contribute to photocatalytic reactions remains to be *** this context,we synthesized a two-dimensional nanosheet MOF(2D-MOF)and a three-dimensional bulk MOF(3D-MOF)composed of Zr^(6) clusters and tetracarboxylic porphyrin(TCPP)by the approach described in the ***(bpy)(CO)^(3)Cl(bpy=2,2’-bipyridine),which has remarkable CO_(2) photoreduction ability,was introduced to the two MOFs to create two new photocatalysts 2D-MOF-Re and 3D-MOF-Re,*** CO_(2) reduction experiments show that based on the equal number of catalytic active sites,the CO turnover number(TON)of 2D-MOF-Re reaches 27.8 in 6 h,which is 50 times that of *** result shows that certain catalytic active sites inside the bulk MOF are inactive due to the inability to absorb *** study illuminates the potential of the dimensional reduction approach in the design of photocatalysts to exploit the capabilities fully.

关键词： photocatalysis CO_(2)reduction metal-organic frameworks(MOFs) nanosheets light absorption

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