Harnessing Reaction-Driven Structural Evolution of Zeolite-Supported Gold Catalyst for Selective Oxidation Reactions

Abstract

Zeolite-supported gold catalysts exhibit exceptional performance across a range of industrially relevant reactions. While previous research has predominantly focused on optimizing catalyst structures through static synthesis parameters, the dynamic structural transformations of Au species under reaction conditions and their subsequent catalytic implications remain largely unexplored. Herein, we utilize advanced electron microscopy and spectroscopy to track the reaction-driven structural evolution of Au nanoclusters supported on hierarchical TS-1 zeolite during the direct epoxidation of propylene with H2 and O2. Comprehensive catalytic and characterization analyses reveal that these structural transformations are actively driven by complex interactions among the Au nanoclusters, the Na promoter, and the in situ-formed oxygenate products. Remarkably, using this direct epoxidation reaction feed as a targeted pretreatment enhances the catalytic performance of the Au-zeolite catalysts by 2- to 4-fold across a broad range of oxidation reactions, including CO oxidation, the selective oxidation of ethanol to acetaldehyde, the selective oxidation of methane to acetic acid, and the oxidation of silane to silanol. These findings establish that exposure to a reactive atmosphere can serve as a powerful, generalized strategy to intentionally modulate the structural features and amplify the catalytic properties of zeolite-supported metal catalysts.