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Accelerated Proton Transfer in Asymmetric Active Units for Sustainable Acidic Oxygen Evolution Reaction

journal contribution
posted on 2024-11-17, 14:52 authored by Liming Deng, Sung Fu Hung, Shuyi Liu, Sheng Zhao, Zih Yi Lin, Chenchen Zhang, Ying Zhang, Ai Yin Wang, Han Yi Chen, Jian Peng, Rongpeng Ma, Lifang Jiao, Feng Hu, Linlin Li, Shengjie Peng
The poor durability of Ru-based catalysts limits the practical application in proton exchange membrane water electrolysis (PEMWE). Here, we report that the asymmetric active units in Ru1-xMxO2 (M = Sb, In, and Sn) binary solid solution oxides are constructed by introducing acid-resistant p-block metal sites, breaking the activity and stability limitations of RuO2 in acidic oxygen evolution reaction (OER). Constructing highly asymmetric Ru-O-Sb units with a strong electron delocalization effect significantly shortens the spatial distance between Ru and Sb sites, improving the bonding strength of the overall structure. The unique two-electron redox couples at Sb sites in asymmetric active units trigger additional chemical steps at different OER stages, facilitating continuous proton transfer. The optimized Ru0.8Sb0.2O2 solid solution requires a superlow overpotential of 160 mV at 10 mA cm-2 and a record-breaking stability of 1100 h in an acidic electrolyte. Notably, the scale-prepared Ru0.8Sb0.2O2 achieves efficient PEMWE performance under industrial conditions. General mechanism analysis shows that the enhanced proton transport in the asymmetric Ru-O-M unit provides a new working pathway for acidic OER, breaking the scaling relationship without sacrificing stability.

Funding

Shanghai Key Laboratory of Materials Laser Processing and Modification, Shanghai Jiao Tong University (2021T140319)

History

Journal title

Journal of the American Chemical Society

Language

English

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