Degradation of organic pollutants by peroxymonosulfate activated by MnO2 with different crystalline structures: Catalytic performances and mechanisms

Zhou, Zhigang; Du, Hong-Mei; Dai, Zhenhua; Mu, Yi; Tong, L.; Xing, Qiu‐Ju; Liu, Shanshan; Ao, Zhimin; Zou, Jian‐Ping

doi:10.1016/j.cej.2019.05.170

Cited by 164 publications

(27 citation statements)

References 60 publications

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“…degradation (Zhou et al 2019). In conclusion, sulfate radicals (SO4 • − ), hydroxyl radicals ( • OH) and the non-radical degradation pathway exist in the Mn-catalytic membrane/PMS system, and no superoxide radicals (O2 •− ) produced.…”

Section: Catalytic Oxidation Of Hbamentioning

confidence: 90%

Manganese oxide integrated catalytic ceramic membrane for degradation of organic pollutants using sulfate radicals

Shi

et al. 2019

Water Research

179

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Membrane separation and advanced oxidation processes (AOPs) have been respectively demonstrated to be effective for a variety of water and/or wastewater treatments. Innovative integration of membrane with catalytic oxidation is thus expected to be more competing for more versatile applications. In this study, ceramic membranes (CMs) integrated with manganese oxide (MnO2) were designed and fabricated via a simple one-step ball-milling method with a high temperature sintering. Functional membranes with different loadings of MnO2 (1.67%, 3.33% and 6.67% of the total membrane mass) were then fabricated. The microstructures and compositions of the catalytic membranes were investigated by a number of advanced characterisations. It was found that the MnO2 nanocatalysts (10-20 nm) were distributed uniformly around the Al2O3 particles (500 nm) of the membrane basal material, and can provide a large amount of active sites for the peroxymonosulfate (PMS) activation which can be facilitated within the pores of the catalytic membrane. The catalytic degradation of 4hydroxylbenzoic acid (HBA), which is induced by the sulfate radicals via PMS activation, was investigated in a cross-flow membrane unit. The degradation efficiency slightly increased with a higher MnO2 loading. Moreover, even with the lowest loading of MnO2 (1.67%), the effectiveness of HBA degradation was still prominent, shown by that a 98.9 % HBA degradation was achieved at the permeated side within 30 min when the initial HBA concentration was 80 ppm. The stability and leaching tests revealed a good stability of the catalytic membrane even after the 6 th run. Electron paramagnetic resonance (EPR) and quenching tests were used to investigate the mechanism of PMS activation and HBA degradation. Both sulfate radicals (SO4˙−) and hydroxyl radicals (˙OH) were generated in the catalytic membrane process. Moreover, the contribution from non-radical process was also observed. This study provides a novel strategy for preparing a ceramic membrane with the 3 function of catalytic degradation of organic pollutants, as well as outlining into future integration of separation and AOPs.

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Section: Catalytic Oxidation Of Hbamentioning

confidence: 90%

Manganese oxide integrated catalytic ceramic membrane for degradation of organic pollutants using sulfate radicals

Shi

et al. 2019

Water Research

179

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“…Efficient degradation of phenol was achieved in β-MnO 2 /PDS system through the generation of singlet oxygen ( 1

) [ 41 ]. Zhou et al indicated the higher catalytic property of α-MnO 2 than δ-MnO 2 in PMS activation for 4-nitrophenol degradation because α-MnO 2 owns more active sites, larger Brunauer–Emmett–Teller (BET) area, faster electron transfer rate, and better adsorption performance [ 42 ]. Furthermore, the activation of PMS by MnO 2 with different crystal phases (i.e., α-, β-, γ-, and δ-MnO 2 ) was reported by Huang et al [ 43 ].…”

Section: Introductionmentioning

confidence: 99%

A Review of Manganese(III) (Oxyhydr)Oxides Use in Advanced Oxidation Processes

et al. 2021

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The key role of trivalent manganese (Mn(III)) species in promoting sulfate radical-based advanced oxidation processes (SR-AOPs) has recently attracted increasing attention. This review provides a comprehensive summary of Mn(III) (oxyhydr)oxide-based catalysts used to activate peroxymonosulfate (PMS) and peroxydisulfate (PDS) in water. The crystal structures of different Mn(III) (oxyhydr)oxides (such as α-Mn2O3, γ-MnOOH, and Mn3O4) are first introduced. Then the impact of the catalyst structure and composition on the activation mechanisms are discussed, as well as the effects of solution pH and inorganic ions. In the Mn(III) (oxyhydr)oxide activated SR-AOPs systems, the activation mechanisms of PMS and PDS are different. For example, both radical (such as sulfate and hydroxyl radical) and non-radical (singlet oxygen) were generated by Mn(III) (oxyhydr)oxide activated PMS. In comparison, the activation of PDS by α-Mn2O3 and γ-MnOOH preferred to form the singlet oxygen and catalyst surface activated complex to remove the organic pollutants. Finally, research gaps are discussed to suggest future directions in context of applying radical-based advanced oxidation in wastewater treatment processes.

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“…hydrogen peroxide, ozone, and persulfates) exhibit promising advantages. 16,17 By combining AOPs with rapid adsorption, a synergistic effect is usually uncovered and the overall performance will be significantly improved, especially when the oxidation occurred on the surface of the adsorbents/ catalysts. 18−21 Consequently, the catalytic behavior of biochar in AOPs was tentatively explored in recent studies.…”

Section: Introductionmentioning

confidence: 99%

“…Specifically, heterogeneous advanced oxidation processes (AOPs) consisting of solid catalysts and chemical oxidants ( i.e. hydrogen peroxide, ozone, and persulfates) exhibit promising advantages. , By combining AOPs with rapid adsorption, a synergistic effect is usually uncovered and the overall performance will be significantly improved, especially when the oxidation occurred on the surface of the adsorbents/catalysts. − Consequently, the catalytic behavior of biochar in AOPs was tentatively explored in recent studies. − For example, persulfates, including peroxymonosulfate (PMS) and peroxydisulfate (PS), can be decomposed to radicals (SO 4 ·– , O 2 ·– ) and nonradical ( 1 O 2 ) reactive oxidative species (ROS) with the assistance of biochars derived from rice straw, , alga (Enteromorpha), wetland plant (reed), and pine needle . Despite numerous attempts, the inherent roles of adsorption between the contaminant, oxidant, and catalyst in heterogeneous AOPs remain ambiguous.…”

Section: Introductionmentioning

confidence: 99%

Synergistic Adsorption and Oxidation of Ciprofloxacin by Biochar Derived from Metal-Enriched Phytoremediation Plants: Experimental and Computational Insights

Ding

Zhou

Kang

et al. 2020

ACS Appl. Mater. Interfaces

105

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Biochar is a promising candidate for the adsorptive removal of organic/inorganic pollutants, yet its role in metal-free catalyzed advanced oxidation processes still remains ambiguous. In this work, five biochar samples (PPBKx, where x represents the pyrolysis temperature) were prepared by using metal-enriched phytoremediation plant residue as the feedstock. Notably, PPBK exhibited a high specific surface area (as high as 1090.7 m2 g–1) and outstanding adsorption capacity toward ciprofloxacin (CIP, as much as 1.51 ± 0.19 mmol g–1). By introducing peroxymonosulfate (PMS, 5 mM) as the chemical oxidant, over 2 mmol g–1 CIP was synergistically adsorbed and oxidized within 30 min although PMS itself could not oxidize CIP efficiently, suggesting the formation of reactive oxidative species. Theoretical calculations revealed that PMS anions preferentially adsorbed on the activated C atoms adjacent to the graphitic N dopant, where the carbon matrix served as the electron donor, instead of as an electron mediator. The adsorbed PMS possessed a smaller molecular orbital energy gap, indicating that it was much easier to be activated than free PMS anions. Surface-bound reactive species were elucidated to be the dominant contributor through chemical quenching experiments and electrochemical characterizations. The catalytic activity of PPBK700 could be greatly retained in repeated oxidations because of the stable N species, which serve as the active catalytic sites, while the CIP adsorption was greatly deteriorated because of the diminishing active adsorption sites (carbon matrix edge) caused by the partial oxidation of PMS. This work not only provides a facile and low-cost approach for the synthesis of functional biochar toward environmental remediation but also deepens the understanding of biochar-catalyzed PMS activation and nonradical oxidation.

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Degradation of organic pollutants by peroxymonosulfate activated by MnO2 with different crystalline structures: Catalytic performances and mechanisms

Cited by 164 publications

References 60 publications

Manganese oxide integrated catalytic ceramic membrane for degradation of organic pollutants using sulfate radicals

Manganese oxide integrated catalytic ceramic membrane for degradation of organic pollutants using sulfate radicals

A Review of Manganese(III) (Oxyhydr)Oxides Use in Advanced Oxidation Processes

Synergistic Adsorption and Oxidation of Ciprofloxacin by Biochar Derived from Metal-Enriched Phytoremediation Plants: Experimental and Computational Insights

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