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

作者：Zhanwu Lei, Wenbin Cai, Yifei Rao, Kuan Wang, Yuyuan Jiang, Yang Liu, Jin Xu, Jianming Li, Zhengxing Lv, Shuhong Jiao, Wenhua Zhang, Pengfei Yan, Shuo Zhang, Ruiguo Cao · 发表于：Nature Communications · 年份：2022 · DOI：10.1038/s41467-021-27664-z · 被引用次数：184 · 研究领域：Electrocatalysts for Energy Conversion、Advanced Photocatalysis Techniques、Catalytic Processes in Materials Science

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 (Ir 1 /NFS), which delivers a high water oxidation activity. The Ir 1 /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 Ir 1 /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.