High-Performance and Long-Lived Pd Nanocatalyst Directed by Shape Effect for CO Oxidative Coupling to Dimethyl Oxalate

Abstract

We synthesized monodisperse Pd nanocrystals with exposed (111) and (100) facets through preferentially oriented facet growth technology. We then supported them on α-Al2O3 as catalysts for application in CO oxidative coupling to dimethyl oxalate (DMO) and find, for the first time, that the (111) facets of Pd nanocrystals are active planes for CO oxidative coupling to DMO. This conclusion is based on experiment results, reaction mechanism, and density functional theory calculation. Directed by this shape effect, a high-performance and long-lived nanocatalyst with much lower Pd load for CO oxidative coupling to DMO was successfully prepared by a new wet impregnation–solution chemical reduction method, which can well control the exposure of (111) facets and sizes of Pd nanocrystals.