Merits and Limitations of Radical vs. Nonradical Pathways in Persulfate-Based Advanced Oxidation Processes

Environmental Science & Technology, Год журнала: 2023, Номер 57(33), С. 12153 - 12179

Опубликована: Авг. 3, 2023

Urbanization and industrialization have exerted significant adverse effects on water quality, resulting in a growing need for reliable eco-friendly treatment technologies. Persulfate (PS)-based advanced oxidation processes (AOPs) are emerging as viable technologies to treat challenging industrial wastewaters or remediate groundwater impacted by hazardous wastes. While the generated reactive species can degrade variety of priority organic contaminants through radical nonradical pathways, there is lack systematic in-depth comparison these pathways practical implementation different scenarios. Our comparative analysis reaction rate constants vs. indicates that radical-based AOPs may achieve high removal efficiency with relatively short contact time. Nonradical feature advantages minimal matrix interference complex wastewater treatments. (e.g., singlet oxygen, high-valent metals, surface activated PS) preferentially react bearing electron-donating groups, allowing enhancement degradation known target contaminants. For byproduct formation, analytical limitations computational chemistry applications also considered. Finally, we propose holistically estimated electrical energy per order (EE/O) parameter show significantly higher requirements pathways. Overall, critical comparisons help prioritize basic research PS-based inform merits system-specific applications.

Язык: Английский

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Activation of peroxymonosulfate via mediated electron transfer mechanism on single-atom Fe catalyst for effective organic pollutants removal

Applied Catalysis B Environment and Energy, Год журнала: 2021, Номер 299, С. 120714 - 120714

Опубликована: Сен. 14, 2021

Язык: Английский

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Persulfate Oxidation of Sulfamethoxazole by Magnetic Iron-Char Composites via Nonradical Pathways: Fe(IV) Versus Surface-Mediated Electron Transfer

Environmental Science & Technology, Год журнала: 2021, Номер 55(14), С. 10077 - 10086

Опубликована: Июль 2, 2021

Despite the vital roles of reactive radical species in coupled iron–carbon composite/persulfate (PS) system for eliminating pollutants, nonradical contributions are typically overlooked. Herein, we developed two efficient magnetic iron–char composites via low-temperature (BCFe-400) and high-temperature (BCFe-700) pyrolysis. The activated PS through pathways sulfamethoxazole (SMX) degradation. In BCFe-400/PS system, high-valent iron Fe(IV) was dominant active oxidation, evidenced by methyl phenyl sulfoxide-based probe tests, Mössbauer spectroscopy, situ Raman analyses with kinetic evaluation. BCFe-700/PS surface-mediated electron transfer dominated regime probed electrochemical test analysis. Furthermore, maintained high efficiency continuous degradation SMX due to feasible Fe2+generation toward formation. stability limited hindered between surface complex (i.e., BCFe-700–PS*) SMX, thermal treatment would help recover reactivity. Both systems exhibited performances removal presence chloride humic acid real water matrixes (e.g., seawater, piggery wastewater, landfill leachate), exhibiting great merits system. Overall, study provide new insights into activation iron-loaded catalysts efficiently degrade pollutants pathways.

Язык: Английский

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Effect of phosphate on peroxymonosulfate activation: Accelerating generation of sulfate radical and underlying mechanism

Applied Catalysis B Environment and Energy, Год журнала: 2021, Номер 298, С. 120532 - 120532

Опубликована: Июль 13, 2021

Язык: Английский

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Ultrafast degradation of emerging organic pollutants via activation of peroxymonosulfate over Fe3C/Fe@N-C-x: Singlet oxygen evolution and electron-transfer mechanisms

Applied Catalysis B Environment and Energy, Год журнала: 2022, Номер 321, С. 122034 - 122034

Опубликована: Окт. 10, 2022

Язык: Английский

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Single Mn atom anchored on N-doped porous carbon as highly efficient Fenton-like catalyst for the degradation of organic contaminants

Applied Catalysis B Environment and Energy, Год журнала: 2020, Номер 279, С. 119363 - 119363

Опубликована: Июль 23, 2020

Язык: Английский

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New notion of biochar: A review on the mechanism of biochar applications in advannced oxidation processes

Chemical Engineering Journal, Год журнала: 2021, Номер 416, С. 129027 - 129027

Опубликована: Фев. 26, 2021

Язык: Английский

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Toward Selective Oxidation of Contaminants in Aqueous Systems

Environmental Science & Technology, Год журнала: 2021, Номер 55(21), С. 14494 - 14514

Опубликована: Окт. 20, 2021

The presence of diverse pollutants in water has been threating human health and aquatic ecosystems on a global scale. For more than century, chemical oxidation using strongly oxidizing species was one the most effective technologies to destruct ensure safe clean supply. However, removal increasing amount with higher structural complexity, especially emerging micropollutants trace concentrations complicated matrix, requires excessive dosage oxidant and/or energy input, resulting low cost-effectiveness possible secondary pollution. Consequently, it is practical significance but scientifically challenging achieve selective interest for decontamination. Currently, there are variety examples concerning aqueous systems. systematic understanding relationship between origin selectivity its applicable treatment scenarios, as well rational design catalyst catalytic oxidation, still lacking. In this critical review, we summarize state-of-the-art strategies decontamination probe origins selectivity, that is, from reactivity either oxidants or target pollutants, arising accessibility via adsorption size exclusion, due interfacial electron transfer process enzymatic oxidation. Finally, challenges perspectives briefly outlined stimulate future discussion decontamination, particularly toward application real scenarios.

Язык: Английский

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Recent advances in persulfate-based advanced oxidation processes for organic wastewater treatment

Chinese Chemical Letters, Год журнала: 2021, Номер 33(10), С. 4461 - 4477

Опубликована: Дек. 23, 2021

Язык: Английский

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Electron delocalization triggers nonradical Fenton-like catalysis over spinel oxides

Proceedings of the National Academy of Sciences, Год журнала: 2022, Номер 119(31)

Опубликована: Июль 25, 2022

Nonradical Fenton-like catalysis offers opportunities to overcome the low efficiency and secondary pollution limitations of existing advanced oxidation decontamination technologies, but realizing this on transition metal spinel oxide catalysts remains challenging due insufficient understanding their catalytic mechanisms. Here, we explore origins selectivity Fe-Mn identify electron delocalization surface active site as key driver its nonradical catalysis. Through fine-tuning crystal geometry trigger superexchange interaction at octahedra, ZnFeMnO4 with high-degree Mn-O unit was created enable near 100% activation peroxymonosulfate (PMS) unprecedented utilization efficiency. The resulting surface-bound PMS* complex can efficiently oxidize electron-rich pollutants extraordinary degradation activity, selectivity, good environmental robustness favor water applications. Our work provides a molecule-level bimetallic interactions oxides, which may guide design low-cost oxides for more selective efficient

Язык: Английский

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