Sulfur-bridge ligands altering the microenvironment of single-atom CoN3S sites to boost the oxygen reduction reaction

Feng Liu; Yingchun Guo; Yan Zhong; Jingsha Li; Heng Zhang; Lei Shi; Xuanni Lin; Fenghui Ye; Kai Ge; Shuai Yuan; Chuangang Hu; Chunxian Guo

doi:10.1039/d4cc00854e

Sulfur-bridge ligands altering the microenvironment of single-atom CoN₃S sites to boost the oxygen reduction reaction

Chem Commun (Camb). 2024 Apr 9;60(30):4064-4067. doi: 10.1039/d4cc00854e.

Authors

Feng Liu¹, Yingchun Guo², Yan Zhong¹, Jingsha Li¹, Heng Zhang¹, Lei Shi³, Xuanni Lin⁴, Fenghui Ye⁴, Kai Ge⁵, Shuai Yuan⁶, Chuangang Hu⁴, Chunxian Guo¹

Affiliations

¹ Institute of Materials Science and Devices, School of Materials Science and Engineering, Suzhou University of Science and Technology, Suzhou 215009, China. cxguo@usts.edu.cn.
² Department of Materials Engineering, Huzhou University, Huzhou 313000, China. ycguo@zjhu.edu.cn.
³ CAS Key Laboratory of Nanosystem and Hierarchical Fabrication, CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology, Beijing 100190, China.
⁴ State Key Laboratory of Organic - Inorganic Composites, College of Chemical Engineering, Beijing University of Chemical Technology, Beijing 100029, China. chuangang.hu@mail.buct.edu.cn.
⁵ Institute of Polymer Science and Engineering, Hebei Key Laboratory of Functional Polymers, Hebei University of Technology, Tianjin 300130, China.
⁶ School of Software and Microelectronics, Peking University, Beijing 102600, China.

PMID: 38502568
DOI: 10.1039/d4cc00854e

Abstract

We report here an asymmetric N,S-coordinated cobalt-based single-atom catalyst with sulfur (S)-bridge ligands (Co-N/S-C) for the oxygen reduction reaction (ORR). The Co-N/S-C exhibits a half-wave potential (E_1/2) of 0.908 V versus RHE, outperforming most state-of-the-art ORR catalysts. Theoretical calculations indicate that the CoN₃SC₁₀-S moiety facilitates the ORR kinetics by optimizing the adsorption of intermediates. This work provides new insights into the design of single-atom catalysts for electrocatalysis through heteroatom-bridge ligand engineering.