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动态循环锌位点促进氧化钌用于亚安培级电化学水氧化

Dynamic-Cycling Zinc Sites Promote Ruthenium Oxide for Sub-Ampere Electrochemical Water Oxidation.

作者信息

Liu Meihuan, Chen Xiaoxia, Li Shiyu, Ni Chudi, Chen Yiwen, Su Hui

机构信息

Key Laboratory of Light Energy Conversion Materials of Hunan Province College, College of Chemistry and Chemical Engineering, Hunan Normal University, Changsha 410081, Hunan, China.

State Key Laboratory for Powder Metallurgy, Central South University, Changsha 410083, Hunan, China.

出版信息

Nano Lett. 2024 Dec 18;24(50):16055-16063. doi: 10.1021/acs.nanolett.4c04485. Epub 2024 Dec 6.

DOI:10.1021/acs.nanolett.4c04485
PMID:39641405
Abstract

Although iridium-based electrocatalysts are commonly regarded as the sole stable operating acidic oxygen evolution reaction (OER) catalysts in proton-exchange membrane water electrolysis (PEMWE) devices, their exorbitant cost and scarcity severely restrict their widespread application. Herein, we introduce a promising alternative to iridium: zinc-doped ruthenium dioxide (TE-Zn/RuO), which exhibits remarkable and enduring activity for acidic OER. characterizations elucidate that the dynamic cycling of zinc dopants serves as both electron acceptors and donors, facilitating the activation of Ru sites at low overpotentials while thwarting peroxidation at high overpotentials, thus concurrently achieving heightened activity and robust stability. Additionally, the incorporation of zinc induces weakened Ru-O covalency, thereby stabling *OOH intermediates and instigating a sustained adsorbate evolution mechanism, dramatically stabilizing the RuO lattice. Importantly, the TE-Zn/RuO catalyst as an anode exhibits good stability over 300 h at a water-splitting current of 500 mA cm in the PEMWE device, underscoring its considerable promise for practical applications.

摘要

尽管基于铱的电催化剂通常被认为是质子交换膜水电解(PEMWE)装置中唯一稳定运行的酸性析氧反应(OER)催化剂,但其高昂的成本和稀缺性严重限制了它们的广泛应用。在此,我们引入了一种有前景的铱替代物:锌掺杂二氧化钌(TE-Zn/RuO),它对酸性OER表现出显著且持久的活性。表征结果表明,锌掺杂剂的动态循环既作为电子受体又作为电子供体,在低过电位下促进Ru位点的活化,同时在高过电位下阻止过氧化,从而同时实现了更高的活性和强大的稳定性。此外,锌的掺入导致Ru-O共价性减弱,从而稳定了*OOH中间体并引发了持续的吸附质演化机制,极大地稳定了RuO晶格。重要的是,TE-Zn/RuO催化剂作为阳极在PEMWE装置中于500 mA cm的析氢电流下300 h以上表现出良好的稳定性,突出了其在实际应用中的巨大潜力。

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