Composition-Tuned Pt-Skinned PtNi Bimetallic Clusters as Highly Efficient Methanol Dehydrogenation Catalysts

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Volume Title
A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä
Date
2019
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Language
en
Pages
10040-10048
Series
Chemistry of Materials, Volume 31
Abstract
Platinum is the most active anode and cathode catalyst in next-generation fuel cells using methanol as liquid source of hydrogen. Its catalytic activity can be significantly improved by alloying with 3d metals, although a precise tuning of its surface architecture is still required. Herein, we report the design of a highly active low-temperature (below 0 °C) methanol dehydrogenation anode catalyst with reduced CO poisoning based on ultralow amount of precisely defined PtxNi1-x (x = 0 to 1) bimetallic clusters (BCs) deposited on inert flat oxides by cluster beam deposition. These BCs feature clear composition-dependent atomic arrangements and electronic structures stemming from their nucleation mechanism, which are responsible for a volcano-type activity trend peaking at the Pt0.7Ni0.3 composition. Our calculations reveal that at this composition, a cluster skin of Pt atoms with d-band centers downshifted by subsurface Ni atoms weakens the CO interaction that in turn triggers a significant increase in the methanol dehydrogenation activity.
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| openaire: EC/H2020/686053/EU//CritCat
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Citation
Liao , T W , Yadav , A , Ferrari , P , Niu , Y , Wei , X K , Vernieres , J , Hu , K J , Heggen , M , Dunin-Borkowski , R E , Palmer , R E , Laasonen , K , Grandjean , D , Janssens , E & Lievens , P 2019 , ' Composition-Tuned Pt-Skinned PtNi Bimetallic Clusters as Highly Efficient Methanol Dehydrogenation Catalysts ' , Chemistry of Materials , vol. 31 , pp. 10040-10048 . https://doi.org/10.1021/acs.chemmater.9b02824