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

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 S2O82− ions. And the EMSIs regulate the charge density in Au atoms to present positive charge Au+, lowering the energy barrier of S2O82− 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.

Metal–support interactions for heterogeneous catalysis: mechanisms, characterization techniques and applications

“…Xie et al synthesized an atomically spread gold catalyst supported on VO 2 (B) nanovolt for a solvothermal-assisted exfoliation technique, which may degrade ROPs expeditiously and stably. 187 The significant inclination between Au and V drives electron transfer from V to Au. Sturdy EMSIs were established between the Au atoms and VO 2 (B) nanovolt scaffolds, which may speedily activate PDS to get sulfate-radicals to remove different ROPs (usually RhB, phenol, and BPA).…”

Improved Electronic Structure from Spin-State Reconstruction of a Heteronuclear Fe–Co Diatomic Pair to Boost the Fenton-like Reaction

“…Single-atom catalysts (SACs) have been extensively applied in various fields, including chemical synthesis, energy conversion, and environmental remediation. − In the Fenton-like reaction using persulfate as the oxidant, transition metal-nitrogen-carbon (M–N/C) materials are emerging as a representative class of SACs due to their well-defined M–N x coordination moieties with a unique electronic structure that is key to determine the adsorption energy of oxygen-containing intermediates and intrinsic catalytic activity. − Thus far, substantial efforts have been devoted to regulating the electronic structure and enhancing the catalytic performance of M–N/C by, for example, coordination adjustment, heteroatom doping, and metal–support interactions. − However, this persulfate-based Fenton-like process is usually involved in the multistep reactions, including activation, stabilization, and accumulation, making it difficult to break the inherent scaling relationship of adsorption energy on the single-atom site, which results in sluggish reaction kinetics and inferior catalytic activity …”

Fe Single-Atom Catalyst for Cost-Effective yet Highly Efficient Heterogeneous Fenton Catalysis

“…Recently, single-atom catalysts (SACs) have attracted great interest in heterogeneous Fenton-like reactions because of their ultimate atom utilization efficiency, maximal exposed active sites, adjustable electronic structure, synergy between adsorption and catalysis, and so on. Many transition-metal atoms, such as Cu (or Co, Fe, , and Au), etc., were incorporated in nitrogen-doped carbon-based supports to activate H 2 O 2 (or persulfate), which exhibits a high catalytic performance for organic pollutant degradation. Some nonmetal atoms, including B and O atoms, were doped in supports to further adjust the electronic configuration of metal sites for improving the Fenton-like activity.…”