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; Ruiguo Cao

doi:10.1038/s41467-021-27664-z

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

Nat Commun. 2022 Jan 10;13(1):24. doi: 10.1038/s41467-021-27664-z.

Authors

Zhanwu Lei^#¹, Wenbin Cai^#¹, Yifei Rao^#¹, Kuan Wang², Yuyuan Jiang², Yang Liu¹, Xu Jin³, Jianming Li³, Zhengxing Lv⁴, Shuhong Jiao⁵, Wenhua Zhang⁶, Pengfei Yan², Shuo Zhang⁴, Ruiguo Cao⁷

Affiliations

¹ Hefei National Laboratory for Physical Sciences at the Microscale, CAS Key Laboratory of Materials for Energy Conversion, Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, Anhui, 230026, China.
² Beijing Key Laboratory of Microstructure and Properties of Solids, Beijing University of Technology, Beijing, 100124, China.
³ Research Center of New Energy, Research Institute of Petroleum Exploration and Development (RIPED), PetroChina, Beijing, 100083, China.
⁴ Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai, 201204, China.
⁵ Hefei National Laboratory for Physical Sciences at the Microscale, CAS Key Laboratory of Materials for Energy Conversion, Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, Anhui, 230026, China. jiaosh@ustc.edu.cn.
⁶ Hefei National Laboratory for Physical Sciences at the Microscale, CAS Key Laboratory of Materials for Energy Conversion, Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, Anhui, 230026, China. whhzhang@ustc.edu.cn.
⁷ Hefei National Laboratory for Physical Sciences at the Microscale, CAS Key Laboratory of Materials for Energy Conversion, Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, Anhui, 230026, China. rgcao@ustc.edu.cn.

^# Contributed equally.

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.

Abstract

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