物理化学学报2023，Vol.39Issue(1)：67-76,10.DOI:10.3866/PKU.WHXB202207007
原子尺度钴基氮碳催化剂对析氧反应的构效关系的研究
Structure-Activity Relationship of Atomic-Scale Cobalt-Based N-C Catalysts in the Oxygen Evolution Reaction
摘要
Abstract
Understanding the origin of the active site activity in the oxygen evolution reaction(OER)electrocatalysts is key for developing efficient electrocatalysts.However,crucial challenges remain due to the complexity of catalyst structure-activity relationships.Herein,various Co-N-C configurations,including single atoms,diatoms,and clusters,were designed to establish structure-activity relationships by first-principles calculations.It was revealed that the Co-N4 exhibited the best reactivity due to the high coordination number of the metal center and moderate adsorption energies for all reaction intermediates.The diatom and cluster activities originate from the highly coordinated structures formed with reaction intermediates,which serve as coordination ligands.Furthermore,other factors influencing the OER activity based on the Co-N4 configuration are discussed.For example,the weak metal-metal interaction can further optimize the adsorption of oxygen-containing intermediates by tuning antibonding energy levels of Co-O.Subsequently,an ultralow overpotential of 0.23 V for the OER in CoNi-type4 systems can be obtained by extrapolation of the volcano plot derived from the established structure-adsorption-activity relationships.This work uncovers the underlying OER activity mechanisms of Co-N-C catalysts,which helps to further understanding of high-performance of M-N-C base catalysts and will aid in the future design of high-efficiency OER catalysts.关键词
电催化/析氧反应/第一性原理计算/构效关系/弱金属相互作用Key words
Electrocatalysis/Oxygen evolution reaction/First-principles calculations/Structure-activity relationship/Weak metal-metal interaction分类
化学化工引用本文复制引用
吴明亮,章烨晖,付战照,吕之阳,李强,王金兰..原子尺度钴基氮碳催化剂对析氧反应的构效关系的研究[J].物理化学学报,2023,39(1):67-76,10.基金项目
This work is supported by the National Key Research and Development Program of China(2021YFA1500700),National Natural Science Foundation of China(22033002,22173018),and Fundamental Research Funds for the Central Universities.国家重点研发计划项目(2021YFA1500700),国家自然科学基金项目(22033002,22173018),中央高校基本科研专项资金资助 （2021YFA1500700）
