材料科学
催化作用
金属有机骨架
析氧
氧气
金属
纳米技术
化学工程
无机化学
化学物理
物理化学
冶金
有机化学
化学
物理
吸附
电极
工程类
电化学
作者
Tengjia Ni,Xianbiao Hou,Jian Zhou,Canhui Zhang,Shuixing Dai,Lei Chu,Huanlei Wang,Heqing Jiang,Minghua Huang
标识
DOI:10.1002/adfm.202413856
摘要
Abstract Asymmetric coordination has emerged as a promising approach to enhance the oxygen evolution reaction (OER) activity, yet achieving a controlled synthesis of asymmetric structures to comprehensively understand the structure‐activity relationship remains challenging. In this study, a facile and effective symmetry‐breaking strategy is reported for tailoring the asymmetric MO 5 S 1 ‐type metal–organic frameworks (MOFs) catalyst, establishing the correlation between the sulfur (S)‐mediated electron rearrangement and the adsorption/desorption dynamics of oxygen‐related intermediates in OER. Experimental and theoretical calculations reveal that a well‐designed asymmetric structure can effectively lower the d‐band center, optimizing the adsorption behavior of OH * and significantly decreasing the reaction energy barrier for the rate‐determining step (OH * → O * ) with enhanced O–H bond cleavage process. The S‐NiFe‐MOF/CFP catalyst demonstrates a remarkable OER performance in an alkaline electrolyte environment. More importantly, the self‐assembled anion exchange membrane water electrolysis cell showcases a low voltage of 1.84 V to deliver the current density of 1 A cm −2 , maintaining long‐term stability for over 100 h. This study unveils a precise asymmetric synthesis strategy employing S, highlighting the critical role of manipulating electron redistribution through asymmetric coordination to promote catalytic activity and develop advanced MOF‐based catalysts.
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