Engineering single-atomic ruthenium catalytic sites on defective nickel-iron layered double hydroxide for overall water splitting

Panlong Zhai; Mingyue Xia; Yunzhen Wu; Guanghui Zhang; Junfeng Gao; Bo Zhang; Shuyan Cao; Yanting Zhang; Zhuwei Li; Zhaozhong Fan; Chen Wang; Xiaomeng Zhang; Jeffrey T Miller; Licheng Sun; Jungang Hou

doi:10.1038/s41467-021-24828-9

Engineering single-atomic ruthenium catalytic sites on defective nickel-iron layered double hydroxide for overall water splitting

Nat Commun. 2021 Jul 28;12(1):4587. doi: 10.1038/s41467-021-24828-9.

Authors

Panlong Zhai^#¹, Mingyue Xia^#², Yunzhen Wu^#¹, Guanghui Zhang¹, Junfeng Gao², Bo Zhang¹, Shuyan Cao¹, Yanting Zhang¹, Zhuwei Li¹, Zhaozhong Fan¹, Chen Wang¹, Xiaomeng Zhang¹, Jeffrey T Miller³, Licheng Sun^{1

4

5}, Jungang Hou⁶

Affiliations

¹ State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, Dalian, China.
² Laboratory of Materials Modification by Laser Ion and Electron Beams (Dalian University of Technology), Ministry of Education, Dalian, China.
³ Davidson School of Chemical Engineering, Purdue University, West Lafayette, IN, USA.
⁴ Center of Artificial Photosynthesis for Solar Fuels, School of Science, Westlake University, Hangzhou, China.
⁵ Department of Chemistry, School of Engineering Sciences in Chemistry, Biotechnology and Health, KTH Royal Institute of Technology, Stockholm, Sweden.
⁶ State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, Dalian, China. jhou@dlut.edu.cn.

^# Contributed equally.

Abstract

Rational design of single atom catalyst is critical for efficient sustainable energy conversion. However, the atomic-level control of active sites is essential for electrocatalytic materials in alkaline electrolyte. Moreover, well-defined surface structures lead to in-depth understanding of catalytic mechanisms. Herein, we report a single-atomic-site ruthenium stabilized on defective nickel-iron layered double hydroxide nanosheets (Ru₁/D-NiFe LDH). Under precise regulation of local coordination environments of catalytically active sites and the existence of the defects, Ru₁/D-NiFe LDH delivers an ultralow overpotential of 18 mV at 10 mA cm^-2 for hydrogen evolution reaction, surpassing the commercial Pt/C catalyst. Density functional theory calculations reveal that Ru₁/D-NiFe LDH optimizes the adsorption energies of intermediates for hydrogen evolution reaction and promotes the O-O coupling at a Ru-O active site for oxygen evolution reaction. The Ru₁/D-NiFe LDH as an ideal model reveals superior water splitting performance with potential for the development of promising water-alkali electrocatalysts.