催化作用
钴
原位
氧还原反应
Atom(片上系统)
氧气
还原(数学)
氧原子
化学
材料科学
无机化学
物理化学
计算机科学
分子
生物化学
电极
电化学
有机化学
几何学
数学
嵌入式系统
作者
Meihuan Liu,Jing Zhang,Hui Su,Yaling Jiang,Wanlin Zhou,Chenyu Yang,Shuowen Bo,Jun Pan,Qinghua Liu
标识
DOI:10.1038/s41467-024-45990-w
摘要
Abstract Single-atom catalysts, especially those with metal−N 4 moieties, hold great promise for facilitating the oxygen reduction reaction. However, the symmetrical distribution of electrons within the metal−N 4 moiety results in unsatisfactory adsorption strength of intermediates, thereby limiting their performance improvements. Herein, we present atomically coordination-regulated Co single-atom catalysts that comprise a symmetry-broken Cl−Co−N 4 moiety, which serves to break the symmetrical electron distribution. In situ characterizations reveal the dynamic evolution of the symmetry-broken Cl−Co−N 4 moiety into a coordination-reduced Cl−Co−N 2 structure, effectively optimizing the 3 d electron filling of Co sites toward a reduced d -band electron occupancy ( d 5.8 → d 5.28 ) under reaction conditions for a fast four-electron oxygen reduction reaction process. As a result, the coordination-regulated Co single-atom catalysts deliver a large half-potential of 0.93 V and a mass activity of 5480 A g metal −1 . Importantly, a Zn-air battery using the coordination-regulated Co single-atom catalysts as the cathode also exhibits a large power density and excellent stability.
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