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原子工程界面诱导桥氧介导的去质子化以增强酸性条件下的析氧反应

Atomically engineered interfaces inducing bridging oxygen-mediated deprotonation for enhanced oxygen evolution in acidic conditions.

作者信息

Wu Han, Chang Jiangwei, Yu Jingkun, Wang Siyang, Hu Zhiang, Waterhouse Geoffrey I N, Yong Xue, Tang Zhiyong, Chang Junbiao, Lu Siyu

机构信息

College of Chemistry and Pingyuan Laboratory, Zhengzhou University, Zhengzhou, P.R. China.

School of Chemical Sciences, The University of Auckland, Auckland, New Zealand.

出版信息

Nat Commun. 2024 Nov 28;15(1):10315. doi: 10.1038/s41467-024-54798-7.

DOI:10.1038/s41467-024-54798-7
PMID:39609455
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11605066/
Abstract

The development of efficient and stable electrocatalysts for water oxidation in acidic media is vital for the commercialization of the proton exchange membrane electrolyzers. In this work, we successfully construct Ru-O-Ir atomic interfaces for acidic oxygen evolution reaction (OER). The catalysts achieve overpotentials as low as 167, 300, and 390 mV at 10, 500, and 1500 mA cm in 0.5 M HSO, respectively, with the electrocatalyst showing robust stability for >1000 h of operation at 10 mA cm and negligible degradation after 200,000 cyclic voltammetry cycles. Operando spectroelectrochemical measurements together with theoretical investigations reveal that the OER pathway over the Ru-O-Ir active site is near-optimal, where the bridging oxygen site of Ir-O serves as the proton acceptor to accelerate proton transfer on an adjacent Ru centre, breaking the typical adsorption-dissociation linear scaling relationship on a single Ru site and thus enhancing OER activity. Here, we show that rational design of multiple active sites can break the activity/stability trade-off commonly encountered for OER catalysts, offering good approaches towards high-performance acidic OER catalysts.

摘要

开发用于酸性介质中析氧反应的高效稳定电催化剂对于质子交换膜电解槽的商业化至关重要。在这项工作中,我们成功构建了用于酸性析氧反应(OER)的Ru-O-Ir原子界面。这些催化剂在0.5 M HSO中,在10、500和1500 mA cm时的过电位分别低至167、300和390 mV,该电催化剂在10 mA cm下运行>1000 h表现出强大的稳定性,并且在200,000次循环伏安循环后降解可忽略不计。原位光谱电化学测量与理论研究表明,Ru-O-Ir活性位点上的OER途径接近最优,其中Ir-O的桥连氧位点作为质子受体,加速相邻Ru中心上的质子转移,打破了单个Ru位点上典型的吸附-解离线性标度关系,从而提高了OER活性。在此,我们表明合理设计多个活性位点可以打破OER催化剂常见的活性/稳定性权衡,为高性能酸性OER催化剂提供了良好的方法。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f938/11605066/b17948bb9750/41467_2024_54798_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f938/11605066/89237a6557bc/41467_2024_54798_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f938/11605066/898ae2019a93/41467_2024_54798_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f938/11605066/79c7d4753b8f/41467_2024_54798_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f938/11605066/b17948bb9750/41467_2024_54798_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f938/11605066/89237a6557bc/41467_2024_54798_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f938/11605066/898ae2019a93/41467_2024_54798_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f938/11605066/79c7d4753b8f/41467_2024_54798_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f938/11605066/b17948bb9750/41467_2024_54798_Fig4_HTML.jpg

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