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Tailoring d-band center over electron traversing effect of Ni M@C-cop(M=Zn,Mo,Ni,Co)for high-performance electrocatalysis hydrogen evolution

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Journal of Materials Science & Technology 2023年第35期166卷 164-172页

作者： Hao Luo Xudong Zhang Hui Zhu Kexin Zhang Fan Yang Kewei Xu Sen Yu Dagang Guo State Key Laboratory for Mechanical Behavior of Materials School of Materials Science and EngineeringXi’an Jiaotong UniversityXi’an710049China Center for High Performance Computing Network Information CenterXi’an Jiaotong UniversityXi’an710049China State Key Laboratory for Manufacturing Systems Engineering Xi’an Jiaotong UniversityXi’an710049China Shaanxi Key Laboratory of Biomedical Metal Materials Northwest Institute for Non-ferrous Metal ResearchXi’an710016China

Attaining a highly efficient and inexpensive electrocatalyst is significant for the hydrogen evolution reaction(HER)but still challenging nowadays.The transition-metal phosphides(TMPs)catalysts with platinum-like electronic structures are a potential candidate for the HER,but those are prone to be strongly bound with hydrogen intermediates(H∗),resulting in sluggish HER kinetics.Herein we report a unique hybrid structure of cop anchored on graphene nanoscrolls@carbon nano tubes(CNTs)scaffold(Ni M@C-cop)encapsulating various Ni M(M=Zn,Mo,Ni,Co)bimetal nanoalloy via chemical vapor deposi-tion(CVD)growth of CNT on graphene nanoscrolls followed by the impregnation of cobalt precursors and phosphorization for efficiently electrocatalytic hydrogen evolution.cop nanoparticles mainly scattered at the tip of CNT branches which exhibited the analogical“Three-layer core-shell”structures.Experiments and density functional theory(DFT)calculations consistently disclose that the encapsulated various NiMs can offer different numbers of electrons to weaken the interactions of outmost cop with H∗and push the downshift of the d-band center to different degrees as well as stabilize the outmost cop nanopar-ticles to gain catalytic stability via the electron traversing effect.The electrocatalytic HER activity can be maximumly enhanced with low overpotentials of 78 mV(alkaline)and 89 mV(acidic)at a current density of 10 mA/cm^(2) and sustained at least 24 h especially for NiZn@C-cop catalyst.This novel system is distinct from conventional three-layer heterostructure,providing a specially thought of d-band center control engineering strategy for the design of heterogeneous catalysts and expanding to other electrocat-alysts,energy storage,sensing,and other applications.

关键词： Electron traversing effect 3D graphene/CNT cop nanoparticle d-band center Hydrogen evolution

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Full reaction mechanism of hydrogen peroxide catalyzed by reductive cop nanoparticles:the enzyme-like activity

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Science China Chemistry 2023年第4期66卷 1221-1227页

作者： Kaiwei Wan Chang Long Bing Jiang Minmin Liang Zhiyong Tang Hui Wang Xinghua Shi Laboratory of Theoretical and Computational Nanoscience CAS Key Laboratory of Nanosystem and Hierarchical FabricationCAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China Molecular Electrochemistry Laboratory Institute of Fundamental and Frontier SciencesUniversity of Electronic Science and Technology of ChinaChengdu 610054China Experimental Center of Advanced Materials School of Materials Science&EngineeringBeijing Institute of TechnologyBeijing 100081China

The hydrogen peroxide(H2O2)catalyzed by nanoparticles(NPs)demonstrates potential broad applications in the field of biomedicine and environmental protection.However,a systematic understanding of the catalytic mechanism severely limited the rational design of NPs with better enzyme-like activity and selectivity.Here,compared with the widely concerned Fe3O4NPs,the decomposition process of H_(2)O_(2) on reductive Co P NPs and p H-regulated peroxidase-and catalase-like activities with 3,3′,5,5′-tetramethylbenzidine(TMB)as reductive substrates were explored.All results show that OH·radical intermediates generated from the decomposition of H2O2*/OOH*at acidic conditions and complexed with TMB via H-bonds(complexed OH·)are the principal oxidant of TMB rather than free OH·as reported.Besides,the produced O*/OH*on Co P NPs shows negligible oxidation activity due to the strong reducibility of catalysts.The high coverage of O*/OH*from the dissociation of H2O2(H2O)at neutral(alkaline)p H conditions on Co P NPs enhances the dehydrogenation of H_(2)O_(2) to O2,leading to the transition between peroxidase-and catalase-like activities.

关键词： cop nanoparticle peroxidase,catalase DFT calculations heterogeneous catalysis

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Molten Salts Strategy for the Synthesis of cop nanoparticles Entrapped,N,P co-Doped Mesoporous Carbons as Electrocatalysts for Hydrogen Evolution

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Chemical Research in Chinese Universities 2022年第1期38卷 237-242页

作者： XU Jing MIAO Sijia TANG Duihai ZHANG Wenting ZHAO Zhen QIAO Zhen-An Institute of Catalysis for Energy and Environment College of Chemistry and Chemical EngineeringShenyang Normal UniversityShenyang 110034P.R.China State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of ChemistryJilin UniversityChangchun 130012P.R.China

Amolten salt process was developed to prepare cop nanoparticles(NPs) embedded, N,P co-doped carbons with the combination of hand milling and high temperature carbonization. The characterization results implied that the as-prepared samples possessed mesoporous structures. Moreover, the mass ratios of the precursors affected the crystalline structures and the porosities of the final electrocatalysts. The as-prepared catalysts exhibited excellent electrocatalytic performances towards hydrogen evolution reaction(HER) under acidic and alkaline conditions. The as-prepared samples were designed as GxMyCoz, where x, y and z meant the amounts of glucose, melamine and CoCl2, respectively. The optimum sample of G6.0M2.0Co5.0 showed the best HER property with a low onset overpotential and a small Tafel slope, as well as excellent electrocatalytic stability.

关键词： cop nanoparticle Mesopore N P co-doped carbon Hydrogen evolution reaction Molten salt

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