Ultralow Ru Loading on Spinel Oxide Enhances Oxygen Coupling for Efficient Acidic Water Oxidation

IF 15.6 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Mingxin Cai, Guopu Cai, Ke Liu, Degao Wang, Hongbin Zhao, Peilei He
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Abstract

The development of proton-exchange membrane water electrolysis (PEMWE) technologies urgently demands electrocatalytic systems capable of maintaining exceptional activity and durability under harsh acidic oxygen evolution reaction (OER) conditions. Here, we present ultralow Ru loading on cobalt–manganese oxides (Ru–Co2MnO4.5) through a facile synthetic strategy. Ru and Co sites facilitate the direct coupling of the oxygen radicals, thereby exceeding the limitations of the scaling relation and triggering the oxide pathway mechanism. Structural characterizations and theoretical calculations demonstrate that the incorporation of Ru single atoms suppresses both lattice oxygen and metal dissolution while maintaining good coordination environments and crystal structures. Furthermore, Ru single-atom loading enhances the hydroxyl adsorption on the catalyst surface and promotes the OER kinetics. Consequently, the Ru–Co2MnO4.5 catalyst achieves an optimal trade-off between catalytic efficiency and structural durability. In 0.5 M H2SO4, the Ru–Co2MnO4.5 demonstrates a minimal overpotential of 176 mV at 10 mA cm–2 and exhibits excellent stability during 600 h. In the PEMWE device, the Ru–Co2MnO4.5 catalyst requires merely a voltage of 1.638 V to achieve 1 A cm–2, with an ultralow Ru loading of 20 μg cm–2. The system can operate for over 100 h under a high current density of 1 A cm–2, showcasing its potential in a practical hydrogen production device. This work presents an innovative strategy for advancing the development of high-efficiency and large-scale green hydrogen production systems while elucidating the underlying reaction mechanisms.

Abstract Image

尖晶石氧化物的超低负载钌增强氧偶联以实现高效的酸性水氧化
质子交换膜水电解(PEMWE)技术的发展迫切需要电催化系统能够在恶劣的酸性析氧反应(OER)条件下保持优异的活性和耐久性。在这里,我们通过一种简单的合成策略提出了钴锰氧化物(Ru - co2mno4.5)的超低Ru负载。Ru和Co位点促进了氧自由基的直接偶联,从而突破了标度关系的限制,触发了氧化途径机制。结构表征和理论计算表明,Ru单原子的掺入抑制了晶格氧和金属的溶解,同时保持了良好的配位环境和晶体结构。此外,钌单原子负载增强了羟基在催化剂表面的吸附,促进了OER动力学。因此,Ru-Co2MnO4.5催化剂实现了催化效率和结构耐久性之间的最佳权衡。在0.5 M H2SO4中,Ru - co2mno4.5在10 mA cm-2时的过电位最低为176 mV,在600 h内表现出优异的稳定性。在PEMWE装置中,Ru - co2mno4.5催化剂只需1.638 V电压即可达到1 a cm-2,超低Ru负载为20 μg cm-2。该系统可以在1 a cm-2的高电流密度下运行超过100小时,显示了其在实际制氢装置中的潜力。这项工作提出了一个创新的战略,推进高效和大规模的绿色制氢系统的发展,同时阐明了潜在的反应机制。
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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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