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Studies in heterogeneous catalysis have long speculated on or have provided indirect evidence for the role of hydrogen embedded in the catalyst bulk as a primary reactant. This report describes experiments carried out under single-collision conditions that document the distinctive reactivity of hydrogen embedded in the bulk of the metal catalyst. Specifically, the bulk H atom is shown to be the reactive species in the hydrogenation of CH(3) adsorbed on Ni(111) to form CH(4), while the H atoms bound to the surface were unreactive. These results unambiguously demonstrate the importance of bulk species to heterogeneous catalytic chemistry.
Johnson et al. (Fri,) studied this question.