Abstract
Catalysts with excellent performances for methanol oxidation reaction (MOR) are supposed to equip with a weaker *CO adsorption but a stronger *OH adsorption. Herein, light incorporation of Cu is implemented into surface-uneven Pt3Sn intermetallic nanocubes to manipulate crucial CO*/OH* intermediates adsorptions for boosting MOR electrocatalysis. The generated ternary Cu0.2Pt3Sn/CNTs intermetallic preserves the uneven cubic shape of non-doped Pt3Sn/CNTs, providing a defect-rich surface structure for affording abundant available active sites. More importantly, the incorporated Cu induces a strong Pt 5d-Sn 5p-Cu 3d orbital hybridization, which upgrades the electron density of Pt but reversely downgrades that of Sn. Such delicately tailored local coordination environments of Pt and Sn result in an intrinsically attenuated CO* adsorption on Pt sites but a promoted OH* adsorption on Sn sites, remarkably diminishing the energy barrier of CO* oxidation. The elaborately customized dual-intermediates adsorptions combined with the defect-rich cubic architecture superiorities consequently contribute to highly elevated MOR performance.
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