Lanthanide-regulating Ru-O covalency optimizes acidic oxygen evolution electrocatalysis

Lu Li, Gengwei Zhang, Chenhui Zhou, Fan Lv, Yingjun Tan, Ying Han, Heng Luo, Dawei Wang, Youxing Liu, Changshuai Shang, Lingyou Zeng, Qizheng Huang, Ruijin Zeng, Na Ye, Mingchuan Luo and Shaojun Guo ()
Additional contact information
Lu Li: Peking University
Gengwei Zhang: Kunming University of Science and Technology
Chenhui Zhou: Peking University
Fan Lv: Peking University
Yingjun Tan: Peking University
Ying Han: Peking University
Heng Luo: Peking University
Dawei Wang: Peking University
Youxing Liu: Peking University
Changshuai Shang: Peking University
Lingyou Zeng: Peking University
Qizheng Huang: Peking University
Ruijin Zeng: Peking University
Na Ye: Peking University
Mingchuan Luo: Peking University
Shaojun Guo: Peking University

Nature Communications, 2024, vol. 15, issue 1, 1-9

Abstract: Abstract Precisely modulating the Ru-O covalency in RuOx for enhanced stability in proton exchange membrane water electrolysis is highly desired. However, transition metals with d-valence electrons, which were doped into or alloyed with RuOx, are inherently susceptible to the influence of coordination environment, making it challenging to modulate the Ru-O covalency in a precise and continuous manner. Here, we first deduce that the introduction of lanthanide with gradually changing electronic configurations can continuously modulate the Ru-O covalency owing to the shielding effect of 5s/5p orbitals. Theoretical calculations confirm that the durability of Ln-RuOx following a volcanic trend as a function of Ru-O covalency. Among various Ln-RuOx, Er-RuOx is identified as the optimal catalyst and possesses a stability 35.5 times higher than that of RuO2. Particularly, the Er-RuOx-based device requires only 1.837 V to reach 3 A cm−2 and shows a long-term stability at 500 mA cm−2 for 100 h with a degradation rate of mere 37 μV h−1.

Date: 2024
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DOI: 10.1038/s41467-024-49281-2

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