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

Ting Wei Liao*, Anupam Yadav, Piero Ferrari, Yubiao Niu, Xian Kui Wei, Jerome Vernieres, Kuo Juei Hu, Marc Heggen, Rafal E. Dunin-Borkowski, Richard E. Palmer, Kari Laasonen, Didier Grandjean, Ewald Janssens, Peter Lievens

*Tämän työn vastaava kirjoittaja

Tutkimustuotos: LehtiartikkeliArticleScientificvertaisarvioitu

4 Sitaatiot (Scopus)

Abstrakti

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.

AlkuperäiskieliEnglanti
Sivut10040-10048
JulkaisuChemistry of Materials
Vuosikerta31
DOI - pysyväislinkit
TilaJulkaistu - 2019
OKM-julkaisutyyppiA1 Julkaistu artikkeli, soviteltu

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  • Siteeraa tätä

    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, 31, 10040-10048. https://doi.org/10.1021/acs.chemmater.9b02824