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用于酸性析氧催化的铱金属烯氧化物

Iridium metallene oxide for acidic oxygen evolution catalysis.

作者信息

Dang Qian, Lin Haiping, Fan Zhenglong, Ma Lu, Shao Qi, Ji Yujin, Zheng Fangfang, Geng Shize, Yang Shi-Ze, Kong Ningning, Zhu Wenxiang, Li Youyong, Liao Fan, Huang Xiaoqing, Shao Mingwang

机构信息

College of Chemistry, Chemical Engineering and Materials Science, Soochow University, 215123, Jiangsu, P. R. China.

Institute of Functional Nano & Soft Materials (FUNSOM), Soochow University, 215123, Jiangsu, P. R. China.

出版信息

Nat Commun. 2021 Oct 14;12(1):6007. doi: 10.1038/s41467-021-26336-2.

Abstract

Exploring new materials is essential in the field of material science. Especially, searching for optimal materials with utmost atomic utilization, ideal activities and desirable stability for catalytic applications requires smart design of materials' structures. Herein, we report iridium metallene oxide: 1 T phase-iridium dioxide (IrO) by a synthetic strategy combining mechanochemistry and thermal treatment in a strong alkaline medium. This material demonstrates high activity for oxygen evolution reaction with a low overpotential of 197 millivolt in acidic electrolyte at 10 milliamperes per geometric square centimeter (mA cm). Together, it achieves high turnover frequencies of 4.2 s (3.0 s) at 1.50 V vs. reversible hydrogen electrode. Furthermore, 1T-IrO also shows little degradation after 126 hours chronopotentiometry measurement under the high current density of 250 mA cm in proton exchange membrane device. Theoretical calculations reveal that the active site of Ir in 1T-IrO provides an optimal free energy uphill in *OH formation, leading to the enhanced performance. The discovery of this 1T-metallene oxide material will provide new opportunities for catalysis and other applications.

摘要

探索新型材料在材料科学领域至关重要。特别是,为催化应用寻找具有最高原子利用率、理想活性和良好稳定性的最佳材料需要对材料结构进行巧妙设计。在此,我们报告了一种铱金属氧化物:通过在强碱性介质中结合机械化学和热处理的合成策略制备的1T相二氧化铱(IrO)。这种材料在酸性电解质中,在每几何平方厘米10毫安(mA cm)的电流密度下,对析氧反应表现出高活性,过电位低至197毫伏。同时,相对于可逆氢电极,在1.50 V时它实现了4.2 s(3.0 s)的高周转频率。此外,在质子交换膜装置中,在250 mA cm的高电流密度下进行126小时计时电位测量后,1T-IrO也几乎没有降解。理论计算表明,1T-IrO中Ir的活性位点在*OH形成过程中提供了最佳的自由能上升,从而提高了性能。这种1T金属氧化物材料的发现将为催化及其他应用提供新的机遇。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4f1d/8516950/9edc2a1830e4/41467_2021_26336_Fig1_HTML.jpg

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