4f-modified Ru-O polarity as a descriptor for efficient electrocatalytic acidic oxygen evolution.
basic_science · Level V
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- Record sourced from PubMed, PMID 40721408.
- Also identified by DOI 10.1038/s41467-025-62258-z and PMC identifier 12304141.
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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 RuO<sub>2</sub> (4f-RuO<sub>2</sub>) nanocatalysts with tunable Ru-O polarity. We find that the OER activity of 4f-RuO<sub>2</sub> shows a volcano shape as a function of the polarity of Ru-O bond. Consequently, the best 4f-Nd-RuO<sub>2</sub> catalyst possesses an ultra-low overpotential of 214 mV at 10 mA cm<sup>-2</sup> and robust electrochemical stability in 0.1 M HClO<sub>4</sub>. Theoretical calculations coupled with in situ synchrotron infrared and X-ray absorption spectroscopy analyses reveal that the modulation of Ru-O polarity in RuO<sub>2</sub> 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.