Canhui Zhang, Xu Liu, Cheng Zhen, Hanxu Yao, Liangliang Xu, Haibing Ye, Yue Wang, Xingkun Wang, M. Danny Gu, Minghua Huang, Heqing Jiang
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引用次数: 0
Abstract
A self-driven seawater splitting system could efficiently produce hydrogen from abundant seawater. However, high Cl− concentrations in seawater lead to catalyst corrosion and deactivation, impairing performance in the oxygen reduction reaction (ORR), oxygen evolution reaction (OER), and hydrogen evolution reaction (HER). Here, we adopted single-atom Co-N-C-based catalysts, in which the electronic structure around the central Co site can be controlled and adjusted at an atomic level. Experimentally, the target N and S co-doped hollow carbon sphere (Co-N/S-HCS) catalyst, featuring asymmetric Co-N3S1 sites, shows excellent ORR/OER/HER performance. By employing density functional theory and molecular dynamics simulations of real-time simulations, we reveal that the S doped in the asymmetric Co-N3S1 model leads to a customized electronic structure around the central Co site, enabling weakened adsorption of the corrosive Cl− and excellent ORR/OER/HER activities. Moreover, the seawater-based Zn-air batteries (S-ZABs) assembled by the Co-N/S-HCS deliver a cycling performance exceeding 650 h, and the overall seawater splitting system can run continuously for 1,100 h.
期刊介绍:
Chem Catalysis is a monthly journal that publishes innovative research on fundamental and applied catalysis, providing a platform for researchers across chemistry, chemical engineering, and related fields. It serves as a premier resource for scientists and engineers in academia and industry, covering heterogeneous, homogeneous, and biocatalysis. Emphasizing transformative methods and technologies, the journal aims to advance understanding, introduce novel catalysts, and connect fundamental insights to real-world applications for societal benefit.