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024 7 _ |a 10.1021/acs.chemmater.9b02824
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100 1 _ |a Liao, Ting-Wei
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245 _ _ |a Composition-Tuned Pt-Skinned PtNi Bimetallic Clusters as Highly Efficient Methanol Dehydrogenation Catalysts
260 _ _ |a Washington, DC
|c 2019
|b American Chemical Society
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520 _ _ |a 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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700 1 _ |a Ferrari, Piero
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700 1 _ |a Niu, Yubiao
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700 1 _ |a Wei, Xian-Kui
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700 1 _ |a Vernieres, Jerome
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700 1 _ |a Hu, Kuo-Juei
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700 1 _ |a Heggen, Marc
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700 1 _ |a Palmer, Richard E.
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700 1 _ |a Laasonen, Kari
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700 1 _ |a Lievens, Peter
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773 _ _ |a 10.1021/acs.chemmater.9b02824
|g Vol. 31, no. 24, p. 10040 - 10048
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|t Chemistry of materials
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