Synergy-optimized spin support for reinforced intermediate supply in ultrafast water splitting

Meng, C, Kong, D, Zhou, Y, Wang, B, Hojamberdiev, M, Zhang, J, Ji, J, Wang, N, Wang, Y, Huang, M, Li, L, Fielding, AJ ORCID: 0000-0002-4437-9791, Li, H, Hu, H and Wu, M (2025) Synergy-optimized spin support for reinforced intermediate supply in ultrafast water splitting. Science Bulletin. ISSN 2095-9273

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Abstract

Engineering the spin state of catalyst supports is crucial for enhancing OH* adsorption in (hydr)oxide-supported Ru single-atom catalysts, thereby improving intermediate supply for efficient water electrolysis. However, at low Ru loadings, conventional approaches such as element substitution and interfacial charge transfer fail to effectively modulate support spin states, limiting water-splitting performance. Here, we design a single-atom Ru-doped Co₃O₄ catalyst enriched with high-spin Co³⁺ (a-Ru-Co₃O₄) via strong atomic and electronic synergy. The high-spin Co³⁺ acts as a robust OH* adsorption site, enhancing water dissociation and H* intermediate supply to Ru sites, facilitating a faster Volmer−Tafel pathway for the hydrogen evolution reaction (HER). Simultaneously, it promotes the formation and stabilization of O*–Ru–O–Co–OH* intermediates, enabling a more kinetically favourable oxide path mechanism (OPM) for the oxygen evolution reaction (OER). As a result, a-Ru-Co₃O₄ exhibits exceptional bifunctional activity, with mass and cost-normalised activities ~30 times higher than commercial Ru/C in both HER and OER. When integrated into an anion-exchange membrane (AEM) electrolyser, a-Ru-Co₃O₄ achieves industrial-level current densities of 1.46 A cm⁻² at 2.0 V for water splitting and 0.51 A cm⁻² at 1.71 V for seawater splitting, demonstrating outstanding durability.

Item Type:	Article
Subjects:	Q Science > QD Chemistry R Medicine > RS Pharmacy and materia medica
Divisions:	Pharmacy and Biomolecular Sciences
Publisher:	Elsevier
Date of acceptance:	7 July 2025
Date Deposited:	01 Sep 2025 09:43
Last Modified:	01 Sep 2025 09:45
DOI or ID number:	10.1016/j.scib.2025.07.022
URI:	https://researchonline.ljmu.ac.uk/id/eprint/27063

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