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Ingeniería de interfaces a nivel atómico para una hidrogenación ácida eficiente y duradera de osmio a altas
Qianyi Lin1, Jun Yu1, Mansheng Liao1
1College of Chemistry and Environmental Engineering, Shenzhen University Shenzhen 518071 China yujun@szu.edu.cn lei.zhang@szu.edu.cn.
Abstract:
Osmium (Os), the least expensive member of the platinum-group metals, has emerged as a promising alternative to Pt-based catalysts for the hydrogen evolution reaction (HER). However, Os-based electrocatalysts still suffer from poor stability under acidic conditions, despite recent efforts to mitigate H* over-adsorption for improved intrinsic activity. Here, we design a porous CeO2 support that enables the atomic dispersion of Os, forming an Os single-atom catalyst (OsSA-CeO2). Unlike traditional flat-film supports, the porous CeO2 architecture prevents Os aggregation and achieves 100% interfacial anchoring of Os atoms. The resulting strong electronic coupling enables tight anchoring of Os and activates the CeO2 matrix with abundant oxygen vacancies, which facilitate H2O dissociation to sustainably supply protons for rapid consumption at large current densities. Also, the generated OH* species are adsorbed by the oxygen vacancies, thus preventing the Os sites from oxidative dissolution. As a result, OsSA-CeO2 exhibits over 500 h of durability at 100 mA cm-2 without performance decay-surpassing all previously reported Os-based HER catalysts. This work provides a general strategy for achieving complete interfacial anchoring of active metal atoms to enhance catalytic stability without sacrificing activity through support activation.
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