Issue

Vol. 15 (2023)

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

https://doi.org/10.1007/s40820-023-01080-y
Jun‑Xi Wu
MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry, Sun Yat-Sen University, Guangzhou 510275, People’s Republic of China
Wen‑Xing Chen
Energy & Catalysis Center, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, People’s Republic of China
Chun‑Ting He
MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry, Sun Yat-Sen University, Guangzhou 510275, People’s Republic of China
Kai Zheng
MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry, Sun Yat-Sen University, Guangzhou 510275, People’s Republic of China
Lin‑Ling Zhuo
MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry, Sun Yat-Sen University, Guangzhou 510275, People’s Republic of China
Zhen‑Hua Zhao
MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry, Sun Yat-Sen University, Guangzhou 510275, People’s Republic of China
Jie‑Peng Zhang
MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry, Sun Yat-Sen University, Guangzhou 510275, People’s Republic of China

Corresponding Author: Jie‑Peng Zhang

zhangjp7@mail.sysu.edu.cn

Nano-Micro Letters, Vol. 15 (2023), Article Number: 120

Abstract

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.


Highlights:


1 An atomically dispersed catalyst with unprecedented N8V4 Co-Ni dual-metal sites is synthesized, which shows interesting asymmetric in situ structural evolution and serves as a quasi-bifunctional catalyst for water splitting.
2 The flexible C–OH groups generated by in situ oxidation can reversibly turn on/off the hydrogen-bonding interaction with the oxygen evolution reaction intermediates to break the conventional scaling relationship.

Keywords

Metal–organic frameworks Atomically dispersed catalyst Hydrogen bond Overall water splitting
Wu, Jun‑Xi, Wen‑Xing Chen, Chun‑Ting He, Kai Zheng, Lin‑Ling Zhuo, Zhen‑Hua Zhao, and Jie‑Peng Zhang. 2023. “Atomically Dispersed Dual-Metal Sites Showing Unique Reactivity and Dynamism for Electrocatalysis”. Nano-Micro Letters 15 (May):120. https://doi.org/10.1007/s40820-023-01080-y.
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