Coordination modulation of iridium single-atom catalyst maximizing water oxidation activity

Zhanwu Lei, Wenbin Cai, Yifei Rao, Kuan Wang, Yuyuan Jiang, Yang Liu, Xu Jin, Jianming Li, Zhengxing Lv, Shuhong Jiao (), Wenhua Zhang (), Pengfei Yan, Shuo Zhang and Ruiguo Cao ()
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Zhanwu Lei: University of Science and Technology of China
Wenbin Cai: University of Science and Technology of China
Yifei Rao: University of Science and Technology of China
Kuan Wang: Beijing University of Technology
Yuyuan Jiang: Beijing University of Technology
Yang Liu: University of Science and Technology of China
Xu Jin: Research Center of New Energy, Research Institute of Petroleum Exploration and Development (RIPED), PetroChina
Jianming Li: Research Center of New Energy, Research Institute of Petroleum Exploration and Development (RIPED), PetroChina
Zhengxing Lv: Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences
Shuhong Jiao: University of Science and Technology of China
Wenhua Zhang: University of Science and Technology of China
Pengfei Yan: Beijing University of Technology
Shuo Zhang: Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences
Ruiguo Cao: University of Science and Technology of China

Nature Communications, 2022, vol. 13, issue 1, 1-10

Abstract: Abstract Single-atom catalysts (SACs) have attracted tremendous research interests in various energy-related fields because of their high activity, selectivity and 100% atom utilization. However, it is still a challenge to enhance the intrinsic and specific activity of SACs. Herein, we present an approach to fabricate a high surface distribution density of iridium (Ir) SAC on nickel-iron sulfide nanosheet arrays substrate (Ir1/NFS), which delivers a high water oxidation activity. The Ir1/NFS catalyst offers a low overpotential of ~170 mV at a current density of 10 mA cm−2 and a high turnover frequency of 9.85 s−1 at an overpotential of 300 mV in 1.0 M KOH solution. At the same time, the Ir1/NFS catalyst exhibits a high stability performance, reaching a lifespan up to 350 hours at a current density of 100 mA cm−2. First-principles calculations reveal that the electronic structures of Ir atoms are significantly regulated by the sulfide substrate, endowing an energetically favorable reaction pathway. This work represents a promising strategy to fabricate high surface distribution density single-atom catalysts with high activity and durability for electrochemical water splitting.

Date: 2022
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DOI: 10.1038/s41467-021-27664-z

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