Durable Anion Exchange Membrane Water Electrolysis in Low-Alkaline Concentration Electrolyte

IF 14.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Haifeng Shen, Fei-Yue Gao, Haobo Li, Jun Xu, Mietek Jaroniec, Yao Zheng, Shi-Zhang Qiao
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Abstract

Anion-exchange-membrane water electrolysis (AEMWE) is a promising technology for scalable green hydrogen production. However, the conventional use of high-alkalinity conditions accelerates membrane degradation, emphasizing the need for low-alkalinity operation to ensure long-term stability. For a low-alkalinity electrolyte with a high water-dissociation energy barrier, Ru serves as an ideal cathodic catalyst owing to its strong Ru–H bond, which provides distinguished water dissociation ability. However, the trade-off is high *H coverage, causing sluggish kinetics and limited durability during high-current operation. Herein, we developed an Ir–Ru solid solution catalyst, which enables rapid hydrogen transfer kinetics through a hydrogen spillover mechanism at high current. As a result, AEMWE with the Ir–Ru solid solution achieved a cell voltage of 1.75 V at 1 A cm–2 in 0.05 M KOH. Notably, the low-alkalinity AEMWE cell exhibited exceptional durability for over 1000 h, surpassing most of the previously reported data under similar operating conditions. Isotope labeling and in situ characterizations confirmed that dissociated *H spills from efficient water-dissociation sites on Ru to favorable hydrogen-desorption sites on Ir with lower *H coverage, significantly improving activity and stability at high current densities.

Abstract Image

低碱性电解液中耐久阴离子交换膜电解
阴离子交换膜水电解(AEMWE)是一种很有前途的大规模绿色制氢技术。然而,常规使用的高碱度条件加速了膜的降解,强调需要低碱度操作以确保长期稳定性。对于具有高水解能势垒的低碱度电解质,Ru具有较强的Ru - h键,具有优异的水解能,是理想的阴极催化剂。然而,代价是高*H覆盖率,导致大电流操作时动力学缓慢,耐久性有限。在此,我们开发了一种Ir-Ru固溶体催化剂,该催化剂通过大电流下的氢溢出机制实现了快速的氢转移动力学。结果表明,采用Ir-Ru固溶体的AEMWE在0.05 M KOH条件下,在1 a cm-2条件下获得了1.75 V的电池电压。值得注意的是,低碱度AEMWE电池表现出超过1000小时的耐久性,超过了之前报道的大多数类似操作条件下的数据。同位素标记和原位表征证实,解离的*H从Ru上有效的水解离位点溢出到*H覆盖率较低的Ir上有利的氢解吸位点,显著提高了高电流密度下的活性和稳定性。
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来源期刊
CiteScore
24.40
自引率
6.00%
发文量
2398
审稿时长
1.6 months
期刊介绍: The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.
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