4f-modified Ru-O polarity as a descriptor for efficient electrocatalytic acidic oxygen evolution

Xiuxiu Zhang, Yuhao Zhang, Bogdan O. Protsenko, Mikhail A. Soldatov, Jing Zhang, Chenyu Yang, Shuowen Bo, Huijuan Wang, Xin Chen (), Chao Wang (), Weiren Cheng () and Qinghua Liu ()
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Xiuxiu Zhang: University of Science and Technology of China
Yuhao Zhang: University of Science and Technology of China
Bogdan O. Protsenko: Southern Federal University
Mikhail A. Soldatov: Southern Federal University
Jing Zhang: University of Science and Technology of China
Chenyu Yang: University of Science and Technology of China
Shuowen Bo: University of Science and Technology of China
Huijuan Wang: University of Science and Technology of China
Xin Chen: Southwest Petroleum University
Chao Wang: University of Science and Technology of China
Weiren Cheng: University of Science and Technology of China
Qinghua Liu: University of Science and Technology of China

Nature Communications, 2025, vol. 16, issue 1, 1-11

Abstract: Abstract The development of non-iridium-based oxygen evolution reaction (OER) catalysts is crucial for proton exchange membrane water electrolysis (PEMWE), but hydrogen production remains a great challenge because of sluggish OER kinetics and severe catalyst dissolution. Here, we present a 4f-induced covalent polarity modulation strategy for the construction of 4f-orbital-modified RuO2 (4f-RuO2) nanocatalysts with tunable Ru–O polarity. We find that the OER activity of 4f-RuO2 shows a volcano shape as a function of the polarity of Ru–O bond. Consequently, the best 4f-Nd-RuO2 catalyst possesses an ultra-low overpotential of 214 mV at 10 mA cm−2 and robust electrochemical stability in 0.1 M HClO4. Theoretical calculations coupled with in situ synchrotron infrared and X-ray absorption spectroscopy analyses reveal that the modulation of Ru–O polarity in RuO2 by the valence f−p−d gradient orbital coupling can modify the adsorption energy of the reaction intermediates and suppress the participation of lattice oxygen to avoid over-oxidation of Ru, which can thus serve as an effective descriptor for fine tuning the activity and durability of acidic OER nanocatalysts.

Date: 2025
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DOI: 10.1038/s41467-025-62258-z

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