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

Nature Communications

Jeffrey T. Miller¹  Junfeng Gao²  Mingyue Xia²  Shuyan Cao³  Yanting Zhang³  Jungang Hou³  Bo Zhang³  Zhuwei Li³  Guanghui Zhang³  Panlong Zhai³  Yunzhen Wu³  Xiaomeng Zhang³  Chen Wang³  Zhaozhong Fan³  Licheng Sun⁴ 

[1] Davidson School of Chemical Engineering, Purdue University, West Lafayette, IN, USA;Laboratory of Materials Modification by Laser Ion and Electron Beams (Dalian University of Technology), Ministry of Education, Dalian, China;State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, Dalian, China;State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, Dalian, China;Center of Artificial Photosynthesis for Solar Fuels, School of Science, Westlake University, Hangzhou, China;Department of Chemistry, School of Engineering Sciences in Chemistry, Biotechnology and Health, KTH Royal Institute of Technology, Stockholm, Sweden;

DOI  :  10.1038/s41467-021-24828-9

来源: Springer

【 摘 要 】

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.

【 授权许可】

CC BY