Lei Zhanwu, Cai Wenbin, Rao Yifei, Wang Kuan, Jiang Yuyuan, Liu Yang, Jin Xu, Li Jianming, Lv Zhengxing, Jiao Shuhong, Zhang Wenhua, Yan Pengfei, Zhang Shuo, Cao Ruiguo
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.
Beijing Key Laboratory of Microstructure and Properties of Solids, Beijing University of Technology, Beijing, 100124, China.
Nat Commun. 2022 Jan 10;13(1):24. doi: 10.1038/s41467-021-27664-z.
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/NFS), which delivers a high water oxidation activity. The Ir/NFS catalyst offers a low overpotential of ~170 mV at a current density of 10 mA cm and a high turnover frequency of 9.85 s at an overpotential of 300 mV in 1.0 M KOH solution. At the same time, the Ir/NFS catalyst exhibits a high stability performance, reaching a lifespan up to 350 hours at a current density of 100 mA cm. 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.
单原子催化剂（SACs）因其高活性、选择性和100%的原子利用率，在各种能源相关领域引起了巨大的研究兴趣。然而，提高SACs的本征活性和比活性仍然是一个挑战。在此，我们提出了一种在硫化镍铁纳米片阵列基底（Ir/NFS）上制备高表面分布密度铱（Ir）单原子催化剂的方法，该催化剂具有高析氧活性。在1.0 M KOH溶液中，Ir/NFS催化剂在电流密度为10 mA cm时提供约170 mV的低过电位，在过电位为300 mV时具有9.85 s的高周转频率。同时，Ir/NFS催化剂表现出高稳定性，在电流密度为100 mA cm时寿命长达350小时。第一性原理计算表明，Ir原子的电子结构受到硫化物基底的显著调节，从而赋予了一条能量有利的反应途径。这项工作代表了一种很有前景的策略，用于制备具有高活性和耐久性的高表面分布密度单原子催化剂，用于电化学水分解。
