TY  - JOUR
AU  - Liao, Ting-Wei
AU  - Yadav, Anupam
AU  - Ferrari, Piero
AU  - Niu, Yubiao
AU  - Wei, Xian-Kui
AU  - Vernieres, Jerome
AU  - Hu, Kuo-Juei
AU  - Heggen, Marc
AU  - Dunin-Borkowski, Rafal E.
AU  - Palmer, Richard E.
AU  - Laasonen, Kari
AU  - Grandjean, Didier
AU  - Janssens, Ewald
AU  - Lievens, Peter
TI  - Composition-Tuned Pt-Skinned PtNi Bimetallic Clusters as Highly Efficient Methanol Dehydrogenation Catalysts
JO  - Chemistry of materials
VL  - 31
IS  - 24
SN  - 1520-5002
CY  - Washington, DC
PB  - American Chemical Society
M1  - FZJ-2020-02801
SP  - 10040 - 10048
PY  - 2019
AB  - 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.
LB  - PUB:(DE-HGF)16
UR  - <Go to ISI:>//WOS:000505628000012
DO  - DOI:10.1021/acs.chemmater.9b02824
UR  - https://juser.fz-juelich.de/record/878354
ER  -