首页|Reversed charge transfer induced by nickel in Fe-Ni/Mo2C@nitrogen-doped carbon nanobox for promoted reversible oxygen electrocatalysis

Reversed charge transfer induced by nickel in Fe-Ni/Mo2C@nitrogen-doped carbon nanobox for promoted reversible oxygen electrocatalysis

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The interaction between metal and support is critical in oxygen catalysis as it governs the charge transfer between these two entities,influences the electronic structures of the supported metal,affects the adsorption energies of reaction intermediates,and ultimately impacts the catalytic performance.In this study,we discovered a unique charge transfer reversal phenomenon in a metal/carbon nanohybrid sys-tem.Specifically,electrons were transferred from the metal-based species to N-doped carbon,while the carbon support reciprocally donated electrons to the metal domain upon the introduction of nickel.This led to the exceptional electrocatalytic performances of the resulting Ni-Fe/Mo2C@nitrogen-doped carbon catalyst,with a half-wave potential of 0.91 V towards oxygen reduction reaction(ORR)and a low over-potential of 290 mV at 10 mA cm-2 towards oxygen evolution reaction(OER)under alkaline conditions.Additionally,the Fe-Ni/Mo2C@carbon heterojunction catalyst demonstrated high specific capacity(794 mA h gZn-1)and excellent cycling stability(200 h)in a Zn-air battery.Theoretical calculations revealed that Mo2C effectively inhibited charge transfer from Fe to the support,while secondary doping of Ni induced a charge transfer reversal,resulting in electron accumulation in the Fe-Ni alloy region.This local electronic structure modulation significantly reduced energy barriers in the oxygen catalysis process,enhancing the catalytic efficiency of both ORR and OER.Consequently,our findings underscore the poten-tial of manipulating charge transfer reversal between the metal and support as a promising strategy for developing highly-active and durable bi-functional oxygen electrodes.

Metal-support interactionCharge transfer reversalOxygen reduction reactionOxygen evolution reactionZinc-air battery

Zhicheng Nie、Lei Zhang、Qiliang Zhu、Zhifan Ke、Yingtang Zhou、Thomas W?gberg、Guangzhi Hu

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School of Materials Science and Engineering,Anhui University of Science and Technology,Huainan 232001,Anhui,China

National Engineering Research Center for Marine Aquaculture,Marine Science and Technology College,Zhejiang Ocean University,Zhoushan 316004,Zhejiang,China

Department of Physics,Umeå University,Umeå S-901 87,Sweden

Institute for Ecological Research and Pollution Control of Plateau Lakes,School of Ecology and Environmental Science,Yunnan University,Kunming 650504,Yunnan,China

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Outstanding Youth Scientific Research Project for Colleges and Universities of Anhui Province of ChinaAnhui Provincial Natural Science FoundationNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaSupport Program of Excellent Young Talents in Anhui Provincial Colleges and UniversitiesDouble Tops Joint Fund of the Yunnan Science and Technology Bureau and Yunnan University

2022AH0200542208085Y0621975001U2002213gxyqZD20220342019FY003025

2024

10.1016/j.jechem.2023.09.009

能源化学
中国科学院大连化学物理研究所 中国科学院成都有机化学研究所

能源化学

CSTPCDEI
影响因子：0.654
ISSN：2095-4956
年,卷(期)：2024.88(1)
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