首页|Engineering asymmetric electronic structure of cobalt coordination on CoN3S active sites for high performance oxygen reduction reaction

Engineering asymmetric electronic structure of cobalt coordination on CoN3S active sites for high performance oxygen reduction reaction

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The efficacy of the oxygen reduction reaction(ORR)in fuel cells can be significantly enhanced by optimiz-ing cobalt-based catalysts,which provide a more stable alternative to iron-based catalysts.However,their performance is often impeded by weak adsorption of oxygen species,leading to a 2e-pathway that negatively affects fuel cell discharge efficiency.Here,we engineered a high-density cobalt active center catalyst,coordinated with nitrogen and sulfur atoms on a porous carbon substrate.Both experimental and theoretical analyses highlighted the role of sulfur atoms as electron donors,disrupting the charge symmetry of the original Co active center and promoting enhanced interaction with Co 3d orbitals.This modification improves the adsorption of oxygen and reaction intermediates during ORR,signifi-cantly reducing the production of hydrogen peroxide(H2O2).Remarkably,the optimized catalyst demon-strated superior fuel cell performance,with peak power densities of 1.32 W cm-2 in oxygen and 0.61 W cm-2 in air environments,respectively.A significant decrease in H2O2 by-product accumulation was observed during the reaction process,reducing catalyst and membrane damage and consequently improving fuel cell durability.This study emphasizes the critical role of coordination symmetry in Co/N/C catalysts and proposes an effective strategy to enhance fuel cell performance.

Fuel cellsOxygen reduction reactionCoordination symmetryCoN3SH2O2 selectivity

Long Chen、Shuhu Yin、Hongbin Zeng、Jia Liu、Xiaofeng Xiao、Xiaoyang Cheng、Huan Huang、Rui Huang、Jian Yang、Wen-Feng Lin、Yan-Xia Jiang、Shi-Gang Sun

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State Key Laboratory of Physical Chemistry of Solid Surfaces,Engineering Research Center of Electrochemical Technologies of Ministry of Education,College of Chemistry and Chemical Engineering,and Discipline of Intelligent Instrument and Equipment,Xiamen University,Xiamen 361005,Fujian,China

Key Laboratory of Urban Pollutant Conversion,Institute of Urban Environment,Chinese Academy of Sciences,Xiamen 361005,Fujian,China

Beijing Synchrotron Radiation Facility,Institute of High Energy Physics,Chinese Academy of Sciences,Beijing 100049,China

Center of Advanced Electrochemical Energy,Institute of Advanced Interdisciplinary Studies,School of Chemistry and Chemical Engineering,Chongqing University,Chongqing 400044,China

Department of Chemical Engineering Loughborough University,Loughborough,Leicestershire LE11 3TU,UK

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2024

10.1016/j.jechem.2024.07.011

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)：2024.98(11)