Abstract
Simultaneously realizing ternary-component integration and compositional profile engineering are of great significance to promote the efficiency and service life of Pt-based eletrtocatalysts for methanol oxidation reaction (MOR). Herein, a porous ternary alloy consisting of PtRu shell and PtRuCo core (PtRuCo@PtRu) is designed via a facile in-situ alloying strategy. Experimental and theoretical outcomes reveal that the incorporated Co atoms induce a strong Pt 5d-Ru 4d-Co 3d orbital coupling, significantly downshifting the d-band center of Pt and thereby reducing the chemisorption strength toward toxic COads. Moreover, the d-orbital electronic configurations of Pt and Ru are tuned be more electron-rich by the electron donation from Co, endowing the catalyst with more strengthened dissolution resistance. Additionally, the continuously leaching out of Co itself is largely inhibited thanks to the finely engineered composition profile in which less-noble Co is protected by the robust PtRu shell. Profiting by the electronic, compositional and architectural superiorities, the PtRuCo@PtRu exhibits significantly enhanced activity and superior long-term stability with respect to benchmark PtRu binary, holding great prospects in practical DMFCs devices.
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