用于增强析氧的异质单原子与团簇之间的远程协同作用。

Remote Synergy between Heterogeneous Single Atoms and Clusters for Enhanced Oxygen Evolution.

作者信息

Ding Xilan, Jia Chuanyi, Ma Peiyu, Chen Huihuang, Xue Jiawei, Wang Dongdi, Wang Ruyang, Cao Heng, Zuo Ming, Zhou Shiming, Zhang Zhirong, Zeng Jie, Bao Jun

机构信息

National Synchrotron Radiation Laboratory, Key Laboratory of Precision and Intelligent Chemistry, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), University of Science and Technology of China, Hefei, Anhui 230026, P.R. China.

Guizhou Provincial Key Laboratory of Computational Nano-Material Science, Institute of Applied Physics, Guizhou Education University, Guiyang, Guizhou 550018, P.R. China.

出版信息

Nano Lett. 2023 Apr 26;23(8):3309-3316. doi: 10.1021/acs.nanolett.3c00228. Epub 2023 Mar 22.

DOI:10.1021/acs.nanolett.3c00228

PMID:36946560

Abstract

Integrating single atoms and clusters into one system is a novel strategy to achieve desired catalytic performances. Compared with homogeneous single-atom cluster catalysts, heterogeneous ones combine the merits of different species and therefore show greater potential. However, it is still challenging to construct single-atom cluster systems of heterogeneous species, and the underlying mechanism for activity improvement remains unclear. In this work, we developed a heterogeneous single-atom cluster catalyst (CoIr/N-C) for efficient oxygen evolution. The Ir single atoms worked in synergy with the Co clusters at a distance of about 8 Å, which optimized the configuration of the key intermediates. Consequently, the oxygen evolution activity was significantly improved on CoIr/N-C relative to the Co cluster catalyst (Co/N-C), exhibiting an overpotential lower by 107 mV than that of Co/N-C at 10 mA cm and a turnover frequency 50.9 times as much as that of Co/N-C at an overpotential of 300 mV.

摘要

将单原子和团簇整合到一个系统中是实现所需催化性能的一种新策略。与均相单原子团簇催化剂相比，非均相催化剂结合了不同物种的优点，因此显示出更大的潜力。然而，构建非均相物种的单原子团簇系统仍然具有挑战性，活性提高的潜在机制仍不清楚。在这项工作中，我们开发了一种用于高效析氧的非均相单原子团簇催化剂（CoIr/N-C）。Ir单原子与Co团簇在约8 Å的距离上协同作用，优化了关键中间体的构型。因此，相对于Co团簇催化剂（Co/N-C），CoIr/N-C上的析氧活性显著提高，在10 mA cm时的过电位比Co/N-C低107 mV，在300 mV过电位下的周转频率是Co/N-C的50.9倍。