Dopant triggered atomic configuration activates water splitting to hydrogen

Rui Wu; Jie Xu; Chuan-Lin Zhao; Xiao-Zhi Su; Xiao-Long Zhang; Ya-Rong Zheng; Feng-Yi Yang; Xu-Sheng Zheng; Jun-Fa Zhu; Jun Luo; Wei-Xue Li; Min-Rui Gao; Shu-Hong Yu

doi:10.1038/s41467-023-37641-3

Dopant triggered atomic configuration activates water splitting to hydrogen

Nat Commun. 2023 Apr 21;14(1):2306. doi: 10.1038/s41467-023-37641-3.

Authors

Rui Wu^#¹, Jie Xu^#², Chuan-Lin Zhao^#³, Xiao-Zhi Su^#⁴, Xiao-Long Zhang¹, Ya-Rong Zheng¹, Feng-Yi Yang¹, Xu-Sheng Zheng⁵, Jun-Fa Zhu⁵, Jun Luo⁶, Wei-Xue Li³, Min-Rui Gao⁷, Shu-Hong Yu⁸

Affiliations

¹ Division of Nanomaterials & Chemistry, Hefei National Research Center for Physical Sciences at the Microscale, New Cornerstone Science Laboratory, Department of Chemistry, Institute of Biomimetic Materials & Chemistry, Anhui Engineering Laboratory of Biomimetic Materials, University of Science and Technology of China, Hefei, 230026, Anhui, P. R. China.
² Institute of Functional Nano and Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, 215123, Suzhou, P. R. China.
³ Department of Chemical Physics, School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, 230026, Anhui, P. R. China.
⁴ Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, CAS, 201210, Shanghai, P. R. China.
⁵ National Synchrotron Radiation Laboratory, University of Science and Technology of China, 230029, Hefei, P. R. China.
⁶ School of Materials Science and Engineering, Tianjin University of Technology, 300384, Tianjin, P. R. China.
⁷ Division of Nanomaterials & Chemistry, Hefei National Research Center for Physical Sciences at the Microscale, New Cornerstone Science Laboratory, Department of Chemistry, Institute of Biomimetic Materials & Chemistry, Anhui Engineering Laboratory of Biomimetic Materials, University of Science and Technology of China, Hefei, 230026, Anhui, P. R. China. mgao@ustc.edu.cn.
⁸ Division of Nanomaterials & Chemistry, Hefei National Research Center for Physical Sciences at the Microscale, New Cornerstone Science Laboratory, Department of Chemistry, Institute of Biomimetic Materials & Chemistry, Anhui Engineering Laboratory of Biomimetic Materials, University of Science and Technology of China, Hefei, 230026, Anhui, P. R. China. shyu@ustc.edu.cn.

^# Contributed equally.

Abstract

Finding highly efficient hydrogen evolution reaction (HER) catalysts is pertinent to the ultimate goal of transformation into a net-zero carbon emission society. The design principles for such HER catalysts lie in the well-known structure-property relationship, which guides the synthesis procedure that creates catalyst with target properties such as catalytic activity. Here we report a general strategy to synthesize 10 kinds of single-atom-doped CoSe₂-DETA (DETA = diethylenetriamine) nanobelts. By systematically analyzing these products, we demonstrate a volcano-shape correlation between HER activity and Co atomic configuration (ratio of Co-N bonds to Co-Se bonds). Specifically, Pb-CoSe₂-DETA catalyst reaches current density of 10 mA cm^-2 at 74 mV in acidic electrolyte (0.5 M H₂SO₄, pH ~0.35). This striking catalytic performance can be attributed to its optimized Co atomic configuration induced by single-atom doping.