Promoted Glycerol Oxidation Reaction in an Interface-Confined Hierarchically Structured Catalyst

Confined catalysis in a 2D system is of particular interest owing to the facet control of the catalysts and the anisotropic kinetics of reactants, which suppress side reactions and improve selectivity. Here, a 2D-confined system consisting of intercalated Pt nanosheets within few-layered graphene is demonstrated. The strong metal-substrate interaction between the Pt nanosheets and the graphene leads to the quasi-2D growth of Pt with a unique (100)/(111)/(100) faceted structure, thus providing excellent catalytic activity and selectivity toward one-carbon (C1) products for the glycerol oxidation reaction. A hierarchically porous graphene architecture, grown on carbon cloth, is used to fabricate the confined catalyst bed in order to enhance the mass-diffusion limitation in interface-confined reactions. Owing to its unique 3D porous structure, this graphene-confined Pt catalyst exhibits an extraordinary mass activity of 2910 mA mg_Pt ^-1 together with a formate selectivity of 79% at 60 °C. This paves the way toward rational designs of heterogeneous catalysts for energy-related applications.