Boosting the electrocatalytic glycerol oxidation performance with highly-dispersed Pt nanoclusters loaded on 3D graphene-like microporous carbon

Abstract

Preparing Pt nanostructure catalysts with better support materials is an efficient catalyst design strategy to develop high performance Pt-based electrocatalysts. Here we report for the first time a method to synthesize highly-dispersed Pt nanoclusters supported on microporous three-dimensional (3D) graphene-like carbon (3D-GLC) for use in the electrochemical oxidation reaction. The Pt nanoclusters loaded on 3D graphene-like carbon (Pt/3D-GLC) are synthesized by Ca2+-exchanged beta zeolite template based carbon synthesis and subsequent Pt impregnation methods. Highly-dispersed Pt nanoclusters (ca. 1.25 ± 0.30 nm) loaded on the 3D-GLC having a large surface area (ca. 2910 m2/g) demonstrate superior electrocatalytic performance for electrochemical glycerol oxidation reaction (GOR) over that of a commercial Pt/C catalyst. We hypothesize in this work that the improved GOR performance of Pt/3D-GLC is related to the increase of Pt active sites by decreasing Pt cluster size and the change in the physicochemical properties of the Pt by interaction between the Pt cluster and 3D-GLC. In addition, first-principle density functional theory (DFT) and ab-initio molecular dynamics (MD) simulations are performed to demonstrate that the finely-dispersed Pt nanoclusters on 3D-GLC support can give rise to excellent GOR activity in accordance with the enhanced adsorption behavior of glycerol on its Pt crystal surfaces.