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

IF 14.7 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES Nature Communications Pub Date : 2024-11-28 DOI:10.1038/s41467-024-54798-7
Han Wu, Jiangwei Chang, Jingkun Yu, Siyang Wang, Zhiang Hu, Geoffrey I. N. Waterhouse, Xue Yong, Zhiyong Tang, Junbiao Chang, Siyu Lu
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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−2 in 0.5 M H2SO4, respectively, with the electrocatalyst showing robust stability for >1000 h of operation at 10 mA cm−2 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–OBRI 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.

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通过原子工程界面诱导桥氧介导的去质子化作用,提高酸性条件下的氧进化能力
在酸性介质中开发高效稳定的水氧化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氧进化反应(OER)的 Ru-O-Ir 原子界面。在 0.5 M H2SO4 中,催化剂在 10、500 和 1500 mA cm-2 条件下的过电位分别低至 167、300 和 390 mV。操作光谱电化学测量和理论研究表明,Ru-O-Ir 活性位点上的 OER 途径接近最佳,其中 Ir-OBRI 的桥接氧位点可作为质子受体,加速相邻 Ru 中心上的质子转移,打破了单一 Ru 位点上典型的吸附-解离线性比例关系,从而提高了 OER 活性。我们在此表明,合理设计多个活性位点可以打破 OER 催化剂通常遇到的活性/稳定性权衡问题,为开发高性能酸性 OER 催化剂提供了良好的方法。
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来源期刊
Nature Communications
Nature Communications Biological Science Disciplines-
CiteScore
24.90
自引率
2.40%
发文量
6928
审稿时长
3.7 months
期刊介绍: Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.
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