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

• Published in: Nature communications Vol. 12; no. 1; pp. 4587 - 11
• Main Authors: Zhai, Panlong, Xia, Mingyue, Wu, Yunzhen, Zhang, Guanghui, Gao, Junfeng, Zhang, Bo, Cao, Shuyan, Zhang, Yanting, Li, Zhuwei, Fan, Zhaozhong, Wang, Chen, Zhang, Xiaomeng, Miller, Jeffrey T., Sun, Licheng, Hou, Jungang
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 28.07.2021; Nature Publishing Group; Nature Portfolio
• Subjects: 140/133; 140/146; 147/137; 147/143; 639/301/299/886; 639/638/161/886; 639/925/357; Active control; Active sites; Catalysts; Chemical engineering; Chemistry; Defects; Density functional theory; Design defects; Electrocatalysts; Electrolytes; Energy conversion; Etching; Evolution; Humanities and Social Sciences; Hydrogen; Hydrogen evolution reactions; Hydroxides; Intermediates; Intermetallic compounds; Iron; Iron compounds; Laboratories; Morphology; multidisciplinary; Nanostructure; Nickel; Nickel compounds; Nickel iron; Oxygen evolution reactions; Renewable energy; Ruthenium; Scanning electron microscopy; Science; Science (multidisciplinary); Single atom catalysts; Sustainable energy; Transmission electron microscopy; Water splitting
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-021-24828-9

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 (Ru 1 /D-NiFe LDH). Under precise regulation of local coordination environments of catalytically active sites and the existence of the defects, Ru 1 /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 Ru 1 /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 Ru 1 /D-NiFe LDH as an ideal model reveals superior water splitting performance with potential for the development of promising water-alkali electrocatalysts. Rational design of single atom catalyst is critical for efficient sustainable energy conversion. Single-atomic-site ruthenium stabilized on defective nickel-iron layered double hydroxide nanosheets achieve superior HER and OER performance in alkaline media.