Composition-Tuned Pt-Skinned PtNi Bimetallic Clusters as Highly Efficient Methanol Dehydrogenation Catalysts
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A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä
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en
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Chemistry of Materials, Volume 31, pp. 10040-10048
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.Description
| openaire: EC/H2020/686053/EU//CritCat
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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