Qi Menghui, Du Xiangbowen, Shi Xiaoyun, Wang Suwen, Lu Bing, Chen Jiadong, Mao Shanjun, Zhang Hao, Wang Yong
Advanced Materials and Catalysis Group, Center of Chemistry for Frontier Technologies, State Key Laboratory of Clean Energy Utilization, Institute of Catalysis, Department of Chemistry, Zhejiang University, Hangzhou 310058, P. R. China.
Department of Chemical Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, United States.
J Am Chem Soc. 2025 May 28;147(21):18295-18306. doi: 10.1021/jacs.5c05752. Epub 2025 May 15.
Activating the oxygen anionic redox presents a promising avenue for developing highly active oxygen evolution reaction (OER) electrocatalysts for proton-exchange membrane water electrolyzers (PEMWE). Here, we engineered a lattice-confined Ru single atom dispersed on a lamellar manganese oxide (MnO) cation site. The strong Ru-O bond induced an upward shift in the O 2 band, enhancing metal-oxygen covalency and reshaping the OER mechanism toward lattice oxygen oxidation pathway with increased activity. spectral characterization combined with density functional theory (DFT) calculations revealed that electron transfer from Mn to Ru alleviates the Jahn-Teller effect within the MnO octahedral structure, stabilizing the lattice. The layered Ru/MnO architecture also promotes the rapid replenishment of oxygen vacancies, preventing structural collapse. As a result, the optimized Ru/MnO electrocatalyst achieves an OER overpotential of only 179 mV at 10 mA cm in 0.5 M HSO, along with exceptional durability over 1000 h at 100 mA cm. Moreover, the Ru/MnO-based PEM device requires only 1.71 V to reach 1 A cm and shows a durability of 500 h at 500 mA cm.
激活氧阴离子氧化还原为开发用于质子交换膜水电解槽（PEMWE）的高活性析氧反应（OER）电催化剂提供了一条有前景的途径。在此，我们设计了一种晶格限制的钌单原子分散在层状氧化锰（MnO）阳离子位点上。强Ru-O键导致O 2带向上移动，增强了金属-氧共价性，并将OER机制重塑为具有更高活性的晶格氧氧化途径。光谱表征结合密度泛函理论（DFT）计算表明，电子从Mn转移到Ru减轻了MnO八面体结构内的 Jahn-Teller 效应，稳定了晶格。层状Ru/MnO结构还促进了氧空位的快速补充，防止结构坍塌。结果，优化后的Ru/MnO电催化剂在0.5 M HSO中10 mA cm时的OER过电位仅为179 mV，在100 mA cm下具有超过1000 h的出色耐久性。此外，基于Ru/MnO的PEM装置在1 A cm时仅需1.71 V，并在500 mA cm下表现出500 h的耐久性。
