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We report gas-phase reactions of free Co n (CO) m + (n = 3-11, m = 0-2) with H2, expecting a catalytic reaction of coadsorbed CO and H2 on Co n +. Preadsorption of CO molecules is found to promote H2 adsorption, in particular, on Co n (CO)+ (n = 5, 8-1. 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 n COH2+ (n = 8-1 imply that at least some of the CO an
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