%0 Journal Article
%A Liao, Ting-Wei
%A Yadav, Anupam
%A Ferrari, Piero
%A Niu, Yubiao
%A Wei, Xian-Kui
%A Vernieres, Jerome
%A Hu, Kuo-Juei
%A Heggen, Marc
%A Dunin-Borkowski, Rafal E.
%A Palmer, Richard E.
%A Laasonen, Kari
%A Grandjean, Didier
%A Janssens, Ewald
%A Lievens, Peter
%T Composition-Tuned Pt-Skinned PtNi Bimetallic Clusters as Highly Efficient Methanol Dehydrogenation Catalysts
%J Chemistry of materials
%V 31
%N 24
%@ 1520-5002
%C Washington, DC
%I American Chemical Society
%M FZJ-2020-02801
%P 10040 - 10048
%D 2019
%X 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.
%F PUB:(DE-HGF)16
%9 Journal Article
%U <Go to ISI:>//WOS:000505628000012
%R 10.1021/acs.chemmater.9b02824
%U https://juser.fz-juelich.de/record/878354