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• W2078133345 endingPage "044306" @default.
• W2078133345 startingPage "044306" @default.
• W2078133345 abstract "Reactions of neutral Vn, Nbn, and Tan metal clusters (n⩽11) with CO+H2 mixed gases and CH3OH in a flow tube reactor (1–50Torr) are studied by time of flight mass spectroscopy and density functional theory calculations. Metal clusters are generated by laser ablation, and reactants and products are ionized by low fluence (∼200μJ∕cm2) 193nm excimer laser light. Nbn clusters exhibit strong size dependent reactivity in reactions both with CO+H2 and CH3OH compared with Vn and Tan clusters. A “magic number” (relatively intense) mass peak at Nb8COH4 is observed in the reaction of Nbn clusters with CO+H2, and CH3OH is suggested to be formed. This feature at Nb8COH4 remains the most intense peak independent of the relative concentrations of CO and H2 in the flow tube reactor. No other Nbn, Tan, or Vn feature behaves in this manner. In reactions of CH3OH with metal clusters Mn (M=V, Nb, and Ta, n=3–11), nondehydrogenated products MnCOH4∕MnCH3OH are only observed on Nb8 and Nb10, whereas dehydrogenated products MnCO∕CMnO are observed for all other clusters. These observations support the suggestion that CH3OH can be formed on Nb8 in the reaction of Nbn with CO+H2. A reaction mechanism is suggested based on the experimental results and theoretical calculations of this work and of those in the literature. Methanol formation from CO+H2 on Nb8 is overall barrierless and thermodynamically and kinetically favorable." @default.
• W2078133345 created "2016-06-24" @default.
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• W2078133345 date "2008-01-28" @default.
• W2078133345 modified "2023-10-14" @default.
• W2078133345 title "Reaction of carbon monoxide and hydrogen on neutral Nb8 clusters in the gas phase" @default.
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• W2078133345 doi "https://doi.org/10.1063/1.2813348" @default.
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