Self-reconstruction mediates isolated Pt tailored nanoframes for highly efficient catalysis†
Abstract
Surface reconstruction of nanocatalysts is an inevitable process during heterogeneous catalysis, resulting in dynamic changes of active sites. It remains a grand challenge to identify the evolution of active sites due to the small size and complex surrounding systems. Here we adopt the PtPdCu heterostructure with many Pt crystals on the surface (h-PdCu&Pt) as a model to investigate surface reconstruction during the ethylene glycol electrocatalytic oxidation. The mismatch between the surface free energy and Gibbs free energy drives the structure reconstruction from h-PdCu&Pt to single Pt active site-tailored PdPtCu nanoframes (SAPt-PdCu NFs) during catalysis. Density functional theory calculation results reveal that the adsorption energy of ethylene glycol on h-PdCu&Pt gradually improves with the surface evolution. Moreover, SAPt-PdCu NFs show better hydrogen evolution reaction activity than h-PdCu&Pt. This discovery promotes the recognition of active sites and facilitates the design of stable catalysts with high activity for heterogeneous catalysis.
Please wait while we load your content...
