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Cu/Mo2C synthesized through Anderson-type polyoxometalates modulate interfacial water structure to achieve hydrogen evolution at high current density

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Nano Research 2024年第4期17卷 2546-2554页

作者： Dunyuan Jin Fen Qiao Yan Zhou Junfeng Wang Kecheng Cao Jing Yang Jikang Zhao Lei Zhou Haitao Li School of Energy and Power Engineering Jiangsu UniversityZhenjiang 212013China School of Physical Science and Technology and Shanghai Key Laboratory of high-{1. electron microscopy ShanghaiTech UniversityShanghai 201210China Institute for Energy Research Jiangsu UniversityZhenjiang 212013China

The development of efficient non-precious metal catalysts is important for the large-scale application of alkaline hydrogen evolution reaction(HER).Here,we synthesized a composite catalyst of Cu and Mo_(2)C(Cu/Mo_(2)C)using Anderson-type polyoxometalates(POMs)synthesized by the facile soaking method as *** electronic interaction between Cu and Mo_(2)C drives the positive charge of Cu,alleviating the strong adsorption of hydrogen at the Mo site by modulating the d-band {1. of Mo_(2)*** studying the interfacial water structure using in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy(ATR-SEIRAS),we determined that the positively charged Cu crystals have the function of activating water molecules and optimizing the interfacial water *** interfacial water of Cu/Mo_(2)C contains a large amount of free water,which could facilitate the transport of reaction *** to activated water molecules and optimized interfacial water structure and hydrogen adsorption energy,the overpotential of Cu/Mo_(2)C is 24 mV at a current density of 1. mA·cm^(-2) and 1.8 mV at a current density of 1.00 mA·cm^(-2).This work improves catalyst performance in terms of interfacial water structure optimization and deepens the understanding of water-mediated catalysis.

关键词： electrocatalytic hydrogen production interfacial water charge transport d band center in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy(ATR-SEIRAS)

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A robust synthesis route of confined carbyne

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Nano Research 2024年第7期17卷 6274-6280页

作者： Yanghao Feng Wendi Zhang Kunpeng Tang Yingzhi Chen Jiou Zhang Kecheng Cao Weili Cui Lei Shi State Key Laboratory of Optoelectronic Materials and Technologies Nanotechnology Research CenterGuangdong Basic Research Center of Excellence for Functional Molecular EngineeringSchool of Materials Science and EngineeringSun Yat-sen UniversityGuangzhou 510275China School of Physical Science and Technology and Shanghai Key Laboratory of high-{1. electron microscopy Shanghai Tech UniversityShanghai 201210China

The unique mechanical,optical,and electrical properties of carbyne,a one-dimensional allotrope of carbon,make it a highly promising material for various *** has been demonstrated that carbon nanotubes(CNTs)can serve as an ideal host for the formation of confined carbyne(CC),with the yield being influenced by the quality of the carbon nanotubes for confinement and the carbon source for carbyne *** this study,a robust synthesis route of CC within CNTs is proposed.C70 was utilized as a precursor to provide an additional carbon source,based on its ability to supply more carbon atoms than C60 at the same filling ***-step transformation processes,including defect creation,were designed to enhance the yield of *** a result,the yield of CC was significantly increased for the C70 encapsulated single-walled CNTs by more than an order of magnitude than the empty counterparts,which also surpasses that of the double-walled CNTs,making it the most effective route for synthesizing *** findings highlight the importance of the additional carbon source and the optimal pathway for CC formation,offering valuable insights for the application of materials with high yield.

关键词： confined carbyne yield enhancement carbon nanotube C70 encapsulation defect introduction Raman spectroscopy

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Hierarchical FeO_(χ)H_(y)@Ni_(3)B hybrid for efficient alkaline oxygen evolution at high current density

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Journal of Energy Chemistry 2024年第7期94卷 599-607页

作者： Fuxi Liu Qing Liang Zhenyu Li Meiqi Liu Nailin Yue Zizhun Wang Xu Zou Wei Zhang Key Laboratory of Automobile Materials Ministry of Education School of Materials Science&EngineeringElectron Microscopy CenterInternational Center of Future ScienceJilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy MaterialsJilin UniversityChangchun 130012JilinChina

Electrocatalysts with high activity and long-term durability are vital toward large-scale hydrogen pro-duction from electrocatalytic water ***,the self-supported electrode(FeO_(χ)H_(y)@Ni_(3)B/NF)with hierarchical heterostructure was simply prepared by using Ni_(3)B chunks grown on nickel foam as sub-strate to in situ form vertical FeO_(χ)H_(y)*** hybrid shows efficient oxygen evolution reaction activity with overpotentials as low as 267 and 249 mV at 1.0 mA cm^(-2)in 1.M KOH solution and 30 wt%KOH solution,***,it also exhibits excellent catalytic stability,sustaining catalysis at 500 mA cm^(-2)in 1.M KOH solution for 200 h,and even for 200 h at 1.00 mA cm^(-2)in 30 wt%KOH *** experimental results reveal that the FeO_(χ)H_(y)@Ni_(3)B/NF is endowed with superhydrophilic and superaerophobic surface properties,which not only provide more mass transport channels,as well as facilitated the diffusion of reaction intermediates and gas ***,it holds faster reaction kinetics,more accessible active sites and accelerated {1. transfer rates due to strong synergistic interactions attheheterogeneous interface.

关键词： FeO_(χ)H_(y)@Ni_(3)B/NF hybrid Heterostructure Oxygen evolution reaction Electrocatalytic

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Optimizing high-coordination shell of Co-based single-atom catalysts for efficient ORR and zinc-air batteries

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Journal of Energy Chemistry 2024年第8期95卷 306-314,I0007页

作者： Yugang Qi Qing Liang Kexin Song Xinyan Zhou Meiqi Liu Wenwen Li Fuxi Liu Zhou Jiang Xu Zou Zhongjun Chen Wei Zhang Weitao Zheng Key Laboratory of Automobile Materials MOE School of Materials Science&Engineering Electron Microscopy Centerand International Center of Future ScienceJilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy MaterialsJilin UniversityChangchun 130012JilinChina Institute of high Energy Physics Chinese Academy of SciencesBeijing 100049China

Atom-level modulation of the coordination environment for single-atom catalysts(SACs)is considered as an effective strategy for elevating the catalytic *** the MNxsite,breaking the symmetrical geometry and charge distribution by introducing relatively weak electronegative atoms into the first/second shell is an efficient way,but it remains challenging for elucidating the underlying mechanism of ***,a practical strategy was reported to rationally design single cobalt atoms coordinated with both phosphorus and nitrogen atoms in a hierarchically porous carbon derived from metal-organic frameworks.X-ray absorption spectrum reveals that atomically dispersed Co sites are coordinated with four N atoms in the first shell and varying numbers of P atoms in the second shell(denoted as Co-N/P-C).The prepared catalyst exhibits excellent oxygen reduction reaction(ORR)activity as well as zinc-air battery *** introduction of P atoms in the Co-SACs weakens the interaction between Co and N,significantly promoting the adsorption process of ^(*)OOH,resulting in the acceleration of reaction kinetics and reduction of thermodynamic barrier,responsible for the increased intrinsic *** discovery provides insights into an ultimate design of single-atom catalysts with adjustable electrocatalytic activities for efficient electrochemical energy conversion.

关键词： Electrocatalytic Oxygen reduction reaction Single atom catalyst Shell coordination optimization

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high-efficiency sodium storage of Co_(0.85)Se/WSe_(2) encapsulated in N-doped carbon polyhedron via vacancy and heterojunction engineering

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Carbon Energy 2024年第1期6卷 94-107页

作者： Ya Ru Pei Hong Yu Zhou Ming Zhao Jian Chen Li Xin Ge Wei Zhang Chun Cheng Yang Qing Jiang Key Laboratory of Automobile Materials(Jilin University) Ministry of EducationSchool of Materials Science and EngineeringJilin UniversityChangchunChina Jilin Provincial International Cooperation Key Laboratory of high-Efficiency Clean Energy Materials Electron Microscopy CenterJilin UniversityChangchunChina

With the advantage of fast charge transfer,heterojunction engineering is identified as a viable method to reinforce the anodes'sodium storage ***,vacancies can effectively strengthen the Na+adsorption ability and provide extra active sites for Na+***,their synchronous engineering is rarely ***,a hybrid of Co_(0.85)Se/WSe_(2) heterostructure with Se vacancies and N-doped carbon polyhedron(CoWSe/NCP)has been fabricated for the first time via a hydrothermal and subsequent selenization *** aberration-corrected transmission electron {1. confirms the phase interface of the Co_(0.85)Se/WSe_(2) heterostructure and the existence of Se *** functional theory simulations reveal the accelerated charge transfer and enhanced Na+adsorption ability,which are contributed by the Co_(0.85)Se/WSe_(2) heterostructure and Se vacancies,*** expected,the CoWSe/NCP anode in sodium-ion battery achieves outstanding rate capability(339.6 mAh g^(−1. at 20 A g^(−1.),outperforming almost all Co/W-based selenides.

关键词： Co_(0.85)Se/WSe_(2)heterostructure density functional theory simulations N-doped carbon polyhedron Se vacancies sodium-ion batteries

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Kinetically and thermodynamically expediting elementary steps via high-valence Cr-incorporated of nickel selenide for water electrolysis

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Nano Research 2024年第3期17卷 1199-1208页

作者： Huafeng Fan Dongxu Jiao Jinchang Fan Dewen Wang Bilal Zaman Wei Zhang Lei Zhang Weitao Zheng Xiaoqiang Cui State Key Laboratory of Automotive Simulation and Control School of Materials Science and EngineeringKey Laboratory of Automobile Materials of MOEJilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy MaterialsElectron Microscopy CenterJilin UniversityChangchun 130012China College of Chemistry Jilin UniversityChangchun 130012China

Designing high-performance electrocatalysts toward hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)is essential to reduce the activation barrier and optimize free adsorption energy of reactive ***,we report that incorporating high-valence Cr into NiSe_(2)(Cr_(x)Ni_(1.x)Se_(2))kinetically and thermodynamically expedites elementary steps of both HER and *** as-prepared Cr_(0.05)Ni_(0.95)Se_(2) catalyst displays excellent HER and OER activities,with low overpotentials of 89 and 272 mV at the current density of 1. mA·cm^(-2)(j1.),respectively,and remains stable during operation for 30 h.A low cell voltage of only 1.59 V is required to drive j1. in alkaline *** situ Raman spectroscopy reveals that Cr incorporation facilitates the formation of NiOOH active species during the OER ***,theoretical explorations demonstrate that high-valence Cr incorporation efficiently accelerates water dissociation kinetics and improves H*adsorption during HER process,lowering the activation barrier of OER and optimizing the adsorption energy of oxygen-based intermediate,thus kinetically and thermodynamically enhancing the intrinsic performance of NiSe_(2) for over water *** strategy provides a new horizon to design transition metal based electrocatalysts in the clean energy field.

关键词： nickel selenide electrocatalytic water splitting high-valence Cr density functional theory(DFT)calculation

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highly-efficient CoRuO_(x)nanocatalysts for acidic oxygen evolution:The merit of optimum ordering degree of carbon nanotube support

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Particuology 2024年第7期90卷 470-477页

作者： Wenwen Li Yanni Wang Zhenzhen Zhao Meiqi Liu Qing Liang Yuhua Liu Fuxi Liu Zhou Jiang Xu Zou Bingsen Zhang Wei Zhang Key Laboratory of Automobile Materials MOE School of Materials Science&EngineeringJilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy MaterialsElectron Microscopy CenterInternational Center of Future ScienceJilin UniversityChangchun 130012China Shenyang National Laboratory for Materials Science Institute of Metal ResearchChinese Academy of Sciences110016ShenyangChina

Hydrogen production from proton exchange membrane water electrolysis is constrained by the sluggish kinetics of the anodic oxygen evolution ***_(2)has attracted considerable attention due to its low reaction overpotential,but its inferior stability remains a major ***,a strategy is proposed to enhance the catalytic activity and stability of CoRuOx nanoparticles by doping Co and regulating the ordering degree of carbon nanotubes(CNTs)by air *** was found that the CoRuOx@CNTs-300 catalyst exhibited the best catalytic activity and stability when the annealing temperature was 300°*** the current density of 1. mA cm−2,the overpotential of this catalyst was only 201.mV,which was nearly 1.0 mV lower than that of commercial RuO_(2)(300 mV).Surprisingly,there was no significant increase in the overpotential when tested at a current density of 1. mA cm−2 for 50 *** density functional theory calculations indicate that the high activity of the catalyst is due to the {1.ic coupling of CoRuOx nanoparticles and CNTs,and that the introduction of Co and CNTs improves the {1.ic structure and solvation energies of the Ru in the active site,dramatically increasing the structural stability.

关键词： Electrocatalysis RuO_(2) CNTs Oxygen evolution reaction

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Dual-Functional Electrode Promoting Dendrite-Free and CO_(2) Utilization Enabled high-Reversible Symmetric Na-CO_(2) Batteries

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Energy & Environmental Materials 2024年第3期7卷 123-132页

作者： Changfan Xu Jiajia Qiu Yulian Dong Yueliang Li Yonglong Shen Huaping Zhao Ute Kaiser Guosheng Shao Yong Lei Fachgebiet Angewandte Nanophysik Institut für Physik&IMN MacroNanoTechnische Universität Ilmenau 98693Ilmenau Germany Central Facility for electron {1. Electron Microscopy Group of Materials ScienceUlm UniversityUlm 89081Germany School of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450001China

Sodium-carbon dioxide(Na-CO_(2))batteries are regarded as promising energy storage technologies because of their impressive theoretical energy density and CO_(2)reutilization,but their practical applications are restricted by uncontrollable sodium dendrite growth and poor electrochemical kinetics of CO_(2)*** suitable multifunctional electrodes for dendritefree anodes and kinetics-enhanced CO_(2)cathodes is considered one of the most important ways to advance the practical application of Na-CO_(2)***,RuO2 nanoparticles encapsulated in carbon paper(RuCP)are rationally designed and employed as both Na anode host and CO_(2)cathode in Na-CO_(2)*** outstanding sodiophilicity and high catalytic activity of RuCP electrodes can simultaneously contribute to homogenous Na+distribution and dendrite-free sodium structure at the anode,as well as strengthen discharge and charge kinetics at the *** morphological evolution confirmed the uniform deposition of Na on RuCP anode with dense and flat interfaces,delivering enhanced Coulombic efficiency of 99.5%and cycling stability near 1.00 ***,Na-CO_(2)batteries with RuCP cathode demonstrated excellent cycling stability(>350 cycles).Significantly,implementation of a dendrite-free RuCP@Na anode and catalytic-site-rich RuCP cathode allowed for the construction of a symmetric Na-CO_(2)battery with long-duration cyclability,offering inspiration for extensive practical uses of Na-CO_(2)batteries.

关键词： CO_(2)cathode dendrite free electrocatalysis Na metal anode symmetric CO_(2)batteries

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Pressure-Tuned Intrinsic Anomalous Hall Conductivity in Kagome Magnets RV_(6)Sn_(6)(R=Gd,Tb)

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Chinese Physics Letters 2024年第4期41卷 139-151页

作者：孔祥明陶咨成张蕊夏威陈旭裴翠颖应天平齐彦鹏郭艳峰杨小帆李世燕 State Key Laboratory of Surface Physics Department of PhysicsFudan UniversityShanghai 200438China Shanghai Research center for Quantum Sciences Shanghai 201315China School of Physical Science and Technology ShanghaiTech UniversityShanghai 201210China ShanghaiTech Laboratory for Topological Physics Shanghai 201210China Northwest Institute for Non-Ferrous Metal Research Xi'an 710016China Beijing National Laboratory for Condensed Matter Physics and Institute of PhysicsChinese Academy of SciencesBeijing 100190China Shanghai Key Laboratory of high-{1. electron microscopy Shanghai 201210China Collaborative Innovation center of Advanced Microstructures Nanjing 210093China

Exploration of exotic phenomena in magnetic topological systems is at the frontier of condensed matter physics,holding a significant promise for applications in topological ***,complex magnetic structures carrying nontrivial topological properties hinder its ***,we investigate the pressure effect on the novel topological kagome magnets GdV_(6)Sn_(6) and TbV_(6)Sn_(6) to dig out the interplay between magnetic Gd/Tb layers and nonmagnetic V-based kagome *** pressure-tuned magnetic transition temperature Tm in both the compounds exhibit a turning point at the critical pressure P_(c),accompanied with a sign reversal in anomalous Hall effect(AHE).The separation of intrinsic and extrinsic contributions using the Tian-Ye-Jin scaling model suggests that the intrinsic mechanism originating from the electronic Berry curvature holds the priority in the competition with extrinsic mechanism in *** above-mentioned findings can be attributed to the combined effect of pressure-tuned band topology and magnetic interaction in segregated *** results provide a practical route to design and manipulate the intrinsic AHE in magnetic topological materials.

关键词： holds frontier hinder

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Efficient optimization of electron transfer pathway by constructing phosphide/ceria interface boosts seawater hydrogen production

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Journal of Energy Chemistry 2024年第8期95卷 490-498,I0011页

作者： Yifan Zhao Lingfeng Yang Youyu Long Min Xi Anran Chen Hua Zhang School of Materials and Energy Yunnan UniversityKunming 650091YunnanChina electron {1. Centre of Yunnan University Yunnan UniversityKunming 650091YunnanChina

Developing efficient and durable hydrogen evolution reaction(HER)electrocatalysts is one of the most important issues for the commercialization of seawater electrolysis,but it remains ***,we report a CeO_(2)-CoP nanoneedle array catalyst loaded on Ti mesh(CeO_(2)-CoP/TM)with workfunction-induced directional charge transport *** CeO_(2)-CoP/TM catalyst showed superior HER catalytic activity and stability,with over potentials of 41.and 60 mV to attain 1. mA cm^(-2),in 1.M KOH and 1.M KOH+seawater electrolyte,*** results and theoretical calculations reveal that the work function drives the charge transfer from CeO_(2)to CoP,which effectively balances the electronic density of CoP and CeO_(2),optimizes the d-band {1.,and accelerates the water activation kinetics,thus enhancing the HER *** solar-driven water electrolysis device displays a high and stable solar-to-hydrogen conversion efficiency of 1..6%.This study offers a work function-induced directional charge transport strategy to design efficient and durable catalysts for hydrogen production.

关键词： Work function Heterostructure Charge transport Seawater splitting Solar-to-hydrogen

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