Oxidative Decomposition of Methanol on Subnanometer Palladium Clusters: The Effect of Catalyst Size and Support Composition

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• 作者：Sungsik Lee ; Byeongdu Lee ; Faisal Mehmood ; Sö ; nke Seifert ; Joseph A. Libera ; Jeffrey W. Elam ; Jeffrey Greeley ; Peter Zapol ; Larry A. Curtiss ; Michael J. Pellin ; Peter C. Stair ; Randall E. Winans ; S
• 刊名：Journal of Physical Chemistry C
• 出版年：2010
• 出版时间：June 17, 2010
• 年：2010
• 卷：114
• 期：23
• 页码：10342-10348
• 全文大小：242K
• 年卷期：v.114,no.23(June 17, 2010)
• ISSN：1932-7455

文摘

Size and support effects in the oxidative decomposition of methanol on amorphous alumina supported subnanometer palladium clusters were studied under realistic reaction conditions of pressure and temperature. The smaller Pd₈₋₁₂ clusters were found to promote the decomposition channel to CO and hydrogen, however with mediocre activity due to poisoning. The larger Pd₁₅₋₁₈ clusters preferentially produce dimethyl ether and formaldehyde, without signs of posioning. A thin titania overcoat applied on the Pd₁₅₋₁₈ improves the sintering-resistance of the catalyst. Accompanying density functional calculations confirm the posioning of small Pd clusters by CO.