Iridium-Free High-Entropy Alloy for Acidic Water Oxidation at High Current Densities

IF 16.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Jinghao Chen, Jiale Ma, Tao Huang, Qichen Liu, Xiaokang Liu, Ruihao Luo, Jingwen Xu, Xiaoyang Wang, Taoli Jiang, Hongxu Liu, Zhenshan Lv, Tao Yao, Gongming Wang, Xusheng Zheng, Zhenyu Li, Wei Chen
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Abstract

Designing active and cost-effective catalysts for acidic oxygen evolution reaction (OER) is critically important for improving proton exchange membrane water electrolyzers (PEMWEs) used in hydrogen production. In this study, we introduce a rapid and straightforward method to synthesize a quinary high-entropy ruthenium-based alloy (RuMnFeMoCo) for acidic OER. This iridium-free catalyst demonstrates a low overpotential of 170 mV and exceptional stability, enduring a 1000-hour durability test at 10 mA cm−2 in 0.5 M H2SO4. Microstructural analyses and density functional theory (DFT) calculations reveal that the incorporation of corrosion-resistant elements such as Ru, Mo, and Co enhances the overall stability of the catalyst under acidic conditions. Concurrently, the presence of Mn, Fe, and Co significantly reduces the energy barrier of the rate-determining step in the OER process, thus accelerating the OER kinetics and lowering the overpotential. The PEMWE employing the RuMnFeMoCo catalyst operates stably at high current densities of 500 and 1000 mA cm−2 for over 300 hours with negligible performance degradation. This work illustrates a strategy for designing high-performance OER electrocatalysts by synergistically integrating the benefits of multiple elements, potentially overcoming the activity-stability trade-off typically encountered in the catalyst development.

Abstract Image

用于高电流密度酸性水氧化的无铱高熵合金
为酸性析氧反应(OER)设计高效、经济的催化剂对于优化质子交换膜制氢水电解槽至关重要。在这项研究中,我们介绍了一种简单、快速的方法来合成一种用于酸性OER的五高熵钌基合金(RuMnFeMoCo)。这种不含铱的催化剂具有170 mV的低过电位和优异的稳定性,在0.5 M H2SO4中,在10 mA cm-2条件下进行了1000小时的耐久性测试。微观结构分析和密度泛函理论(DFT)计算表明,Ru、Mo和Co等耐腐蚀元素的加入提高了催化剂在酸性条件下的整体稳定性。同时,Mn、Fe和Co的存在显著降低了OER过程中速率决定步骤的能量势垒,从而加速了OER动力学并降低了过电位。采用RuMnFeMoCo催化剂的PEMWE在500 mA cm-2和1000 mA cm-2的高电流密度下稳定工作超过300小时,性能下降可以忽略不计。这项工作阐明了一种设计高性能OER电催化剂的策略,通过协同整合多种元素的优势,有可能克服催化剂开发中通常遇到的活性-稳定性权衡。
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来源期刊
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
期刊介绍: Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
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