Tailoring the Electronic Metal-Support Interactions in Supported Atomically Dispersed Gold Catalysts for Efficient Fenton-like Reaction

Angew Chem Int Ed Engl. 2021 Jun 21;60(26):14370-14375. doi: 10.1002/anie.202103652. Epub 2021 May 17.

Abstract

The atomically dispersed metal is expected as one of the most promising Fenton-like catalysts for the degradation of recalcitrant organic pollutants (ROPs) by the strong "electronic metal-support interactions" (EMSIs). Here, we develop an atomically dispersed metal-atom alloy made by guest Au atoms substitute host V atoms in the two-dimensional VO2 (B) nanobelt support (Au/VO2 ) to activate Fenton-like oxidation for elimination of ROPs. The 2D nanobelt structure enlarges the exposure of atomically Au thus increasing the number of active sites to absorb more S2 O8 2- ions. And the EMSIs regulate the charge density in Au atoms to present positive charge Au+ , lowering the energy barrier of S2 O8 2- decomposition to produce SO4 .- . The Au/VO2 catalyst possesses excellent durable and reliable characteristics and exhibits record-breaking efficiency with TOF as high as 21.42 min-1 , 16.19 min-1 , and 80.89 min-1 for rhodamine, phenol, and bisphenol A degradation, respectively.

Keywords: active sites; atomically dispersed; electronic metal-support interactions; one-pot strategy; substitutional solid solution.