Evidence for Ambient-Temperature Reversible Catalytic Hydrogenation in Pt-doped Carbons

In situ high-pressure Raman spectroscopy, with corroborating density functional calculations, is used to probe C–H chemical bonds formed when dissociated hydrogen diffuses from a platinum nanocatalyst to three distinct graphenic surfaces. At ambient temperature, hydrogenation and dehydrogenation are reversible in the combined presence of an active catalyst and oxygen heteroatoms. Hydrogenation apparently occurs through surface diffusion in a chemisorbed state, while dehydrogenation requires diffusion of the chemisorbed species back to an active catalyst.