Structural tuning of multishelled hollow microspheres for boosted peroxymonosulfate activation and selectivity: Role of surface superoxide radical

Li, Wenqian; He, Xu; Li, Boda; Zhang, Bin; Liu, Ting; Hu, Ying

doi:10.1016/j.apcatb.2021.121019

Cited by 62 publications

(27 citation statements)

References 42 publications

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“… TEMP- 1 O 2 is detected in all systems since it can be generated via the recombination or disproportion of O 2 •– , hydrolysis of SO 5 •– , and self-decomposition of PMS in water (Figure S34). By virtue of in situ Raman, the role of PMS* in ZnMn 2 O 4 /PMS and ZnCoMnO 4 /PMS systems is identified. From Figure S35, the peak of PMS* at ∼838 cm –1 appeared upon PMS addition and disappeared after 2-CP addition, indicative of the direct oxidation of 2-CP by PMS*.…”

Section: Resultsmentioning

confidence: 99%

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e_g Orbital Occupancy-Dependent Intrinsic Catalytic Activity of Zn–Co–Mn Spinel Oxides in Fenton-like Reactions

Xia

Wang

et al. 2023

ACS EST Water

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Transition-metal (TM)-based spinel oxides have demonstrated excellent efficacy in Fenton-like reactions, but the key mechanism behind peroxymonosulfate (PMS) adsorption, decomposition, and pollutant degradation is still unclear. Here, a crucial role of eg orbital occupancy in manipulating the interaction between PMS and Zn–Co–Mn ternary spinel catalysts and the resulting pollutant degradation is first discovered. The introduction of Co into the ZnMn2O4 network lowers the magnetic momentum and eg occupancy and favors the overlap between TM eg and O 2p orbitals. Experimental results demonstrate that the eg occupancy-dependent catalytic activity and pathway originate from its cascade effect on PMS binding, decomposition, and radical desorption. Zn–Co–Mn with optimized eg occupancy exhibits favorable PMS binding strength, interaction capability, radical desorption, and pollutant degradation. Cyclic voltammetry (CV) and density functional theory (DFT) corroborate the critical role of eg in PMS affinity. In addition, the ZnCoMnO4/PMS system shows high selectivity for carbamazepine (CBZ, 0.275 min–1) and environmental robustness. The surface active complex PMS*, the peroxymonosulfate radical, and the sulfate radical are identified as reactive species. This work provides an intrinsic mechanism behind pollutant degradation and offers guidance for performance enhancement in a water environment.

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Section: Resultsmentioning

confidence: 99%

“…•− , and selfdecomposition of PMS in water (Figure S34). 38 •− quencher). In the ZnCoMnO 4 /PMS system, the degradation efficiency was inhibited to 38.6% with the addition of methyl alcohol (MeOH, • OH, and SO 4…”

Section: Acs Esandt Watermentioning

confidence: 99%

e_g Orbital Occupancy-Dependent Intrinsic Catalytic Activity of Zn–Co–Mn Spinel Oxides in Fenton-like Reactions

Xia

Wang

et al. 2023

ACS EST Water

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“…138 In another example, Co 3 O 4 with OVs promotes the adsorption and reduction of O 2 , and O 2 c À can be detected over the surface of Co 3 O 4 . 139 In the case of Ni-Fe layered double hydroxide (NiFe-LDH), OVs facilitate the charge carrier transfer of NiFe-LDH, and activate O 2 into O 2 c À for the selective oxidation of NO into nitrate (Fig. 6).…”

Section: àmentioning

confidence: 99%

Reactive oxygen species on transition metal-based catalysts for sustainable environmental applications

et al. 2022

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“…Hollow microspheres have been promising functional materials for their excellent chemical and physical characteristics conferred by the spherical form of a hollow shell structure 1 . Owing to the distinct morphology involving favorable surface property and large internal space, hollow microspheres possess a surprising‐specific surface area, low bulk density as well as low thermal conductivity, which enable them to be applied as storage and controllable releasing materials, adsorbents and catalysts, lightweight materials and thermal insulation materials 2–8 .…”

Section: Introductionmentioning

confidence: 99%

Submicron mullite hollow spheres synthesized via UV polymerization of Pickering emulsions

Yang

Zhang

et al. 2023

J Am Ceram Soc.

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We here propose a simple, facile, and effective method to prepare submicron mullite hollow spheres templated from Pickering emulsions. Dual-phase sol consisted of boehmite and silica nanoparticles decorated by pentanoate ion could assemble at water/oil interface irreversibly to form photosensitive Pickering emulsions. The droplets of emulsions could be separated by dilution and formed by photopolymerization to gain hybrid microspheres, which could completely transform to mullite hollow microspheres via binder removal and sintering. It is found that the prepared hollow microspheres possess intact morphology, favorable sphericity, large cavity volume, and bulk density of 0.356 g/cm 3 . Importantly, the average diameter of mullite hollow spheres obtained via this method could be as low as 0.33-2.31 μm. This steady method is efficient and suitable for various types of inorganic particles, providing an innovative perspective for preparing fine hollow spheres applicable for filtration, drug loading as well as energy storage areas.

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Structural tuning of multishelled hollow microspheres for boosted peroxymonosulfate activation and selectivity: Role of surface superoxide radical

Cited by 62 publications

References 42 publications

e_g Orbital Occupancy-Dependent Intrinsic Catalytic Activity of Zn–Co–Mn Spinel Oxides in Fenton-like Reactions

e_g Orbital Occupancy-Dependent Intrinsic Catalytic Activity of Zn–Co–Mn Spinel Oxides in Fenton-like Reactions

Reactive oxygen species on transition metal-based catalysts for sustainable environmental applications

Submicron mullite hollow spheres synthesized via UV polymerization of Pickering emulsions

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Structural tuning of multishelled hollow microspheres for boosted peroxymonosulfate activation and selectivity: Role of surface superoxide radical

Cited by 62 publications

References 42 publications

eg Orbital Occupancy-Dependent Intrinsic Catalytic Activity of Zn–Co–Mn Spinel Oxides in Fenton-like Reactions

eg Orbital Occupancy-Dependent Intrinsic Catalytic Activity of Zn–Co–Mn Spinel Oxides in Fenton-like Reactions

Reactive oxygen species on transition metal-based catalysts for sustainable environmental applications

Submicron mullite hollow spheres synthesized via UV polymerization of Pickering emulsions

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Product

Resources

About

e_g Orbital Occupancy-Dependent Intrinsic Catalytic Activity of Zn–Co–Mn Spinel Oxides in Fenton-like Reactions

e_g Orbital Occupancy-Dependent Intrinsic Catalytic Activity of Zn–Co–Mn Spinel Oxides in Fenton-like Reactions