Atomically Dispersed Dual‑Metal Sites Showing Unique Reactivity and Dynamism for Electrocatalysis  

作　　者：Jun‑Xi Wu Wen‑Xing Chen Chun‑Ting He Kai Zheng Lin‑Ling Zhuo Zhen‑Hua Zhao Jie‑Peng Zhang 

机构地区：[1]MOE Key Laboratory of Bioinorganic and Synthetic Chemistry,School of Chemistry,Sun Yat-Sen University,Guangzhou 510275,People’s Republic of China [2]Key Lab of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of Education,College of Chemistry and Chemical Engineering,Jiangxi Normal University,Nanchang 330022,People’s Republic of China [3]Energy&Catalysis Center,School of Materials Science and Engineering,Beijing Institute of Technology,Beijing 100081,People’s Republic of China

出　　处：《Nano-Micro Letters》2023年第8期192-204,共13页纳微快报（英文版）

基　　金：supported by the National Key Research and Development Program of China(2021YFA1500401);the National Natural Science Foundation of China(21890380,21975290,21901089,and 21821003);the Foundation of Basic and Applied Basic Research of Guangdong Province(2020B1515120024);C.-T.H.acknowledges the Jiangxi Province(20202ZDB01004 and jxsq2018106041).

摘　　要：The real structure and in situ evolution of catalysts under working conditions are of paramount importance,especially for bifunctional electrocatalysis.Here,we report asymmetric structural evolution and dynamic hydrogen-bonding promotion mechanism of an atomically dispersed electrocatalyst.Pyrolysis of Co/Ni-doped MAF-4/ZIF-8 yielded nitrogen-doped porous carbons functionalized by atomically dispersed Co–Ni dual-metal sites with an unprecedented N8V4 structure,which can serve as an efficient bifunctional electrocatalyst for overall water splitting.More importantly,the electrocatalyst showed remarkable activation behavior due to the in situ oxidation of the carbon substrate to form C–OH groups.Density functional theory calculations suggested that the flexible C–OH groups can form reversible hydrogen bonds with the oxygen evolution reaction intermediates,giving a bridge between elementary reactions to break the conventional scaling relationship.

关 键 词：Metal-organic frameworks Atomically dispersed catalyst Hydrogen bond Overall water splitting 

分 类 号：TQ116.2[化学工程—无机化工] TQ426