Efficient decomposition of perfluorooctane sulfonate by electrochemical activation of peroxymonosulfate in aqueous solution: Efficacy, reaction mechanism, active sites, and application potential

Li, Meng; Jin, Yu-Ting; Cao, Dan-Yang; Yang, Ling-Ling; Yan, Jian-Fang; Zhang, Zhao-Xin; Liu, Zhang; Huang, Long-Wei; Zhou, Shaoqi; Cheng, Jiliang; Zhao, Qinglan; Zhao, Hai-Ming; Feng, Nai-Xian; Chen, Mo

doi:10.1016/j.watres.2022.118778

Cited by 23 publications

(5 citation statements)

References 39 publications

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“…It is widely accepted that the liquid-phase oxidation of cyclohexane proceeds through a radical-involved autoxidation process. EPR analysis was conducted to identify ChemCatChem radical species by using 5,5-dimethyl-1-pyrroline N-oxide (DMPO) as the spin trap agent for the capture of free radicals, [30][31][32] and the electrolyte containing radicals is extracted from the electrode/electrolyte interface. The EPR spectra of seven oxidation systems are shown in Figure 4a.…”

Section: Resultsmentioning

confidence: 99%

Selective Radical Oxidation of Cyclohexane to Adipic Acid at Electrochemical Interfaces

Tian

Zhang

et al. 2022

ChemCatChem

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Direct conversion of cyclohexane to adipic acid (AA) under mild conditions is an attractive technology in response to the increasing industrial demand of chemical intermediate AA. Exploring advanced free radical oxidation systems is the key to converting cyclohexane in a direct and mild manner. This study demonstrates that electrocatalytic water oxidation can quantitatively generate hydroxyl radicals (⋅OH) to selectively oxidize cyclohexane to AA by a vanadium oxide (VOx)‐platinum (Pt) composite catalyst coupled with persulfate (PS) redox mediator at the electrode/electrolyte interface under ambient temperature and pressure. The three active components of VOx, Pt, and PS can produce different concentrations of ⋅OH radicals alone or in combination, resulting in different AA selectivity and cyclohexane conversion, and the activity increased with the increase of free radical concentration before AA peroxidation. The optimized ternary oxidation system of VOx‐Pt‐PS achieved a cyclohexane conversion of 85 % with 95 % AA selectivity and the corresponding yield was 81 %, better than most traditional oxidation systems. Electrochemical interfaces‐driven radical oxidation provides opportunities to oxidatively convert many other inexpensive hydrocarbons to value‐added chemicals.

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Section: Resultsmentioning

confidence: 99%

Selective Radical Oxidation of Cyclohexane to Adipic Acid at Electrochemical Interfaces

Tian

Zhang

et al. 2022

ChemCatChem

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“…PFOA is bioaccumulative, and chronic exposure to PFOA is closely linked to genotoxicity, developmental toxicity, immunotoxicity, and hepatotoxicity. − The high persistence and bioaccumulating capabilities of PFASs necessitate the development of future treatment technologies in real-world implications . In this work, we propose a cathode-mediated electrochemical process for PFOA degradation with controllable SO 4 •– and HO • .…”

Section: Discussionmentioning

confidence: 99%

Controllable Generation of Sulfate and Hydroxyl Radicals to Efficiently Degrade Perfluorooctanoic Acid in Cathode-Dominated Electrochemical Process

Lei,

Liu,

Yang

et al. 2023

ACS EST Water

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Sulfate radical-based advanced oxidation process (SO 4•− -AOP) has been considered as a potential PFOA treatment option. The synergistic effect of SO 4•− and hydroxyl radicals (HO • ) favors the mineralization of PFOA. However, research regarding the optimal PFOA degradation pathway with controllable SO 4•− and HO • is limited. Here, we proposed a cathodemediated electrochemical process for efficiently removing PFOA through the in situ generation of SO 4•− and HO • . Iron−nickel codoped carbon aerogel (Fe x NiC) were designed as cathode for synergistically activating peroxymonosulfonate (PMS) and oxygen (O 2 ). Fe 0.6 NiC with optimized C SO4•-(0.385 mM) and C HO• (0.175 mM) exhibited high PFOA degradation efficiency (83.8%), TOC removal (75.9%), and defluorination rate (63.6%). DFT calculations and experimental studies confirmed that SO 4•− -involved steps promote one-electron transfer from ionic C 7 F 15 COO − to SO 4 •−, and HO • -involved steps yield short-chain PFCAs. The actual application for pretreatment and deep-treatment of fluorochemical wastewater in the conventional treatment systems promoted the PFOA mineralization efficiency. It can be preferable to optimize the ratio of C SO4•-and C HO• in this cathode-mediated electrochemical process to rapidly and economically mineralize PFOA.

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“…The DD value (Δ f A ) per atom A in the OTC molecule is given as the following:Δ f A = f + A − f − A = 2 q A N − 2 q A N +1 − q A N −1 where q A N is the atom A's electron population number in the OTC molecule, and f + A and f − A are obtained when the system undergoes nucleophilic and electrophilic attack, respectively. Furthermore, the OTC geometry optimization and DFT calculations of q A N , q A N +1 , and q A N −1 , were conducted in Gaussian 09 using the b3lyp/6-31 g(d) approach 39,40 combined with Multiwfn. 41,42 Table S1 in the ESI† shows the calculated DD values.…”

Section: Methodsmentioning

confidence: 99%

Dual metal Co-anchored nanosheets to catalyze advanced oxidation processes for highly efficient oxytetracycline degradation

Yan

Zhang

et al. 2022

Environ. Sci.: Nano

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Efficient decomposition of perfluorooctane sulfonate by electrochemical activation of peroxymonosulfate in aqueous solution: Efficacy, reaction mechanism, active sites, and application potential

Cited by 23 publications

References 39 publications

Selective Radical Oxidation of Cyclohexane to Adipic Acid at Electrochemical Interfaces

Selective Radical Oxidation of Cyclohexane to Adipic Acid at Electrochemical Interfaces

Controllable Generation of Sulfate and Hydroxyl Radicals to Efficiently Degrade Perfluorooctanoic Acid in Cathode-Dominated Electrochemical Process

Dual metal Co-anchored nanosheets to catalyze advanced oxidation processes for highly efficient oxytetracycline degradation

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