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 and Jungang Hou ()
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Panlong Zhai: Dalian University of Technology
Mingyue Xia: Ministry of Education
Yunzhen Wu: Dalian University of Technology
Guanghui Zhang: Dalian University of Technology
Junfeng Gao: Ministry of Education
Bo Zhang: Dalian University of Technology
Shuyan Cao: Dalian University of Technology
Yanting Zhang: Dalian University of Technology
Zhuwei Li: Dalian University of Technology
Zhaozhong Fan: Dalian University of Technology
Chen Wang: Dalian University of Technology
Xiaomeng Zhang: Dalian University of Technology
Jeffrey T. Miller: Purdue University
Licheng Sun: Dalian University of Technology
Jungang Hou: Dalian University of Technology

Nature Communications, 2021, vol. 12, issue 1, 1-11

Abstract: 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.

Date: 2021
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DOI: 10.1038/s41467-021-24828-9

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