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We report gas-phase reactions of free Co_n(CO)_m^+ (n = 3–11, m = 0–2) with H_2, expecting a catalytic reaction of coadsorbed CO and H2_ on Co_n^+. Preadsorption of CO molecules is found to promote H_...2 adsorption, in particular, on Co_n(CO)^+ (n = 5, 8–10). Density functional theory (DFT) calculations reveal that the reactivity is governed by the molecular-orbital energy of Co_n^+, which is tuned by preadsorbed CO molecules. Collision-induced-dissociation experiments performed on Co_nCOH_2^+ (n = 8–10) imply that at least some of the CO and H_2 molecules are bound together on Co_n^+.続きを見る
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