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- E-mail： tzhang2009@sinano.ac.cn
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Hierarchical heterojunction construction and interaction mechanism of Ru1-LaOx-NiMnOx nanocomposite for alkaline hydrogen evolution, Journal of Alloys and Compounds, 2025, 1017, 179115.
Qianzuo Liu; Yunping Ma; Nan Ma; Yingyi Wang; Sifan Sun; Binqi He; Ting Zhang*; Xuehua Yan*; Tie Li*;
Abstract
Ruthenium-based catalysts have demonstrated the rapid water dissociation kinetics in the alkaline hydrogen evolution reaction (HER). However, the inappropriate adsorption of hydrogenous intermediates at Ru active sites can restrict its catalytic activity for HER. Here, we successfully synthesize a novel hierarchical nanocomposite catalyst (Ru1-LaOx-NiMnOx) by an availably strategy of engineering a hierarchical heterostructure coupling between the lanthanide metal oxides (LnO) and the transition metal oxides (TMO) to support single-atom Ru, which can optimize the adsorption strength for the hydrogenous intermediates compared to the direct loading of Ru on the TMO matrix, significantly displaying the ultra-high catalytic behavior of mass activity (5182 mA mgRu−1 at −0.1 V) under an ultra-low density of Ru sites (only 9 µg cm−2) in the alkaline media. Specifically, the in-situ electrochemical Raman spectroscopy and Density Functional Theory calculations indicate that the strategy alters the Ru-O-Metals pattern and regulates the electronic status of Ru sites, promoting water dissociation and mitigating the strong adsorption of *H, which enhances the reaction kinetics of catalytic progress. Briefly, utilizing the heterostructure coupling effect of LnO and TMO to modulate the electronic structure of single-atoms can effectively control the adsorption and formation of the intermediates, offering the valuable insights for catalytic reactions.
URL: https://www.sciencedirect.com/science/article/pii/S0925838825006735?ref=pdf_download&fr=RR-9&rr=916e063f9b1a5df0