1. Lanthanide-regulating Ru-O covalency optimizes acidic oxygen evolution electrocatalysis.
- Author
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Li, Lu, Zhang, Gengwei, Zhou, Chenhui, Lv, Fan, Tan, Yingjun, Han, Ying, Luo, Heng, Wang, Dawei, Liu, Youxing, Shang, Changshuai, Zeng, Lingyou, Huang, Qizheng, Zeng, Ruijin, Ye, Na, Luo, Mingchuan, and Guo, Shaojun
- Subjects
ELECTROCATALYSIS ,OXYGEN evolution reactions ,GREEN fuels ,WATER electrolysis ,ELECTRON configuration ,HYDROGEN production ,RARE earth metals - Abstract
Precisely modulating the Ru-O covalency in RuO
x 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 . Lack of stability in RuO2 -based catalysts at industrial currents impedes their use in green hydrogen production. Here, the authors show that incorporating lanthanide elements into RuOx shields against external factors, enabling fine-tuned Ru-O covalency for durable oxygen evolution reaction electrocatalysis. [ABSTRACT FROM AUTHOR]- Published
- 2024
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