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.

Overturned Loading of Inert CeO2to Active Co3O4for Unusually Improved Catalytic Activity in Fenton‐Like Reactions

“…The reaction is initiated by the adsorption of PMS onto the surface, followed by the decomposition of PMS to generate free radicals, and finally, the desorption of radicals to the solution to oxidize the pollutants, where the desorption of generated sulfate radicals from the surface of the catalyst is the rate-limiting step for the entire reaction. [35] To simulate our samples, we built two different model surfaces, both exposing the representative (110) facets of Co 3 O 4 , because it is one of the most exposed and stable facets as determined by its Wulff structure [36] The adsorption of PMS on the two substrates is shown in Figure 5a. The free energy for the adsorption of PMS (ΔE ads ) by the two substrates was calculated to be À 3.45 eV and À 3.28 eV (Table S11), indicating favored PMS adsorption onto both substrates.…”

Signal Amplification Strategy Using Atomically Gold-Supported VO2 Nanobelts as a Co-reaction Accelerator for Ultrasensitive Electrochemiluminescent Sensor Construction Based on the Resonance Energy Transfer Platform

“…17 nanobelt (Au/VO 2 ) with excellent catalytic performance. 18 However, using Au/VO 2 as a catalyst in ECL applications has not yet been reported. Glutathione (GSH) is a tripeptide with an active sulfhydryl group, which is an important regulatory metabolite in cells.…”

Electronic Metal–Support Interactions for Electrochemiluminescence Signal Amplification

“…Meanwhile, a similar enhanced tendency of Co 3+ in Co 2p spectra was observed, indicating the generation of O v -Co 3+ sites. In the Au 4f spectra (Figure 3C), the characteristic peaks at 84.84 eV for 4f 7/2 and 87.42 eV for 4f 5/2 were observed in Au/LDH/ITO, 19 while relatively lower binding energy peaks at 83.49 and 87.27 eV were given in Au/LDH-O v /ITO, revealing the enrichment of electron of Au atom (Au δ− ). The formation of electron-rich Au atoms in this work strongly demonstrated the occurrence of EMSI between Au atoms and LDH-O v at the Au/LDH-O v interface for the electron excursion from LDH-O v to Au nanoparticles and the generation of Au δ− -O v -Co 3+ interface sites.…”

“…Metal–support interactions play an important role in the improvement of the catalytic activity of supported metal catalysts. , In 2012, a new type of metal–support interaction, electronic metal–support interaction (EMSI), had attached increasing attention since it was first proposed by Campbell . Recently, much attention has been paid to the fabrication of novel catalysts by the EMSI effect. − For example, Lu and his co-workers developed an atomical Au on two-dimensional VO 2 nanobelt catalysts for the efficient Fenton-like reaction . They concluded that the strong EMSI between Au atoms and VO 2 nanobelt supports could rapidly activate S 2 O 8 2– to generate SO 4 •– radicals to remove various recalcitrant organic pollutants; Datta et al realized the tuning of the EMSI between Ru nanoparticles and CuO nanowire supports by increasing multiple twinned Ru nanoparticle population, and they demonstrated that the defect-assisted EMSI could improve the catalyst activity and stability for oxygen evolution reaction at neutral condition; Wei’s group reported that EMSI from Co­(OH) 2 to Pt nanoparticles could form electron-rich Pt nanoparticles, leading to the improvement of the catalytic activity toward CO oxidation .…”

“…18−29 For example, Lu and his co-workers developed an atomical Au on two-dimensional VO 2 nanobelt catalysts for the efficient Fenton-like reaction. 19 They concluded that the strong EMSI between Au atoms and VO 2 nanobelt supports could rapidly activate S 2 O 8 2− to generate SO 4…”