Construction of a permeable metal-support interface for glycerol oxidation by the topological transformation of 2D precursor

Abstract

Aiming at achieving a trade-off of electronic-interacted and permeable metal-support interfaces, we developed a feasible approach for constructing semi-continuous TiOx/Pt structure through the topological transformation of ultrathin PtCl62−/TiMgAl-layered double hydroxides (LDHs) to limit the migration degree of metal ions perpendicular to the lamellar direction. Structural characterization revealed that most Pt sites are permeable to the reactants in the ultrathin TiOx/Pt/TiMgAlOx-U catalyst. Despite that, there is still electron transfer to form abundant Pt0-oxygen vacancy(Vo)-Ti3+sites in the interfacial structure. In the glycerol oxidation reaction, the TiOx/Pt/TiMgAlOx-U exhibited a much higher reaction rate(289 molglycrol·molPt−1·h−1), which is 1.7 times of the bulk TiOx/Pt/TiMgAlOx-B and 5.2 times of the TiOx/Pt/TiO2 reference, and simultaneously maintained a decent glyceric acid selectivity. Mechanism study revealed that the Pt0-Vo-Ti3+interfacial structure could promote the activation and fluxion of active oxygen species, and was favorable for the activation of primary hydroxyl groups of glycerol and the aldehyde intermediate.