Edge‐Confined Pt1/MoS2 Single‐Atom Catalyst Promoting the Selective Activation of Carbon‐Oxygen Bond

Abstract Selective activation of carbon‐oxygen bonds (like C−O and C=O) represents an essential part of the biomass conversion, but it is difficult to selectively activating the inert carbon‐oxygen bonds. We report 2D MoS 2 edges confined single Pt atoms efficiently catalyze biomass‐derived crotonaldehyde to crotyl alcohol with selectivity from 90 to 100 %. The Pt 1 /MoS 2 single‐atom catalysts have a unique HO−Mo−S−Pt 1 −S−Mo−OH configuration, reminiscent of an enzyme pocket‐like active site, which restricts the adsorption configuration of crotonaldehyde by a steric hindrance effect. The Pt 1 atoms possess unique electronic structures due to the Pt 1 ‐S 4 configuration, which easily dissociates H 2 to H species and boosts the activity. The activated H species spillover and react with O atoms on edges, forming OH and creating the HO−Mo−S−Pt 1 −S−Mo−OH configuration, which restricts the adsorption configuration of crotonaldehyde and yields high selectivity. The tactics of fabricating pocket‐like active sites with metal single atoms and 2D nanosheet edges shed a light on developing highly selective catalysts for biomass conversion reactions.