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• W4308469655 endingPage "140207" @default.
• W4308469655 startingPage "140207" @default.
• W4308469655 abstract "• CSIA was effective to in situ analyze radical contributions on ATZ degradation by heat-activated PS. • ATZ can be degraded by heat-activated PS with high removal efficiency at pH 4-10. • Changes of δ 13 C and δ 2 H during ATZ degradation followed Rayleigh equation well. • The ε C values were 1.58‰ at pH 4 and 0.65‰ at pH 7 for SO 4 •– -dominated oxidation. • Contributions of SO 4 ·- by heat-activated PS were ∼100% and 83.9% at pH 4 and 7. SO 4 •– -assisted oxidation was of great concern and the accurate interpretation of reaction pathway was crucial. Innovatively, this study introduced compound-specific isotope fractionation analysis (CSIA) into atrazine (ATZ) degradation by heat-activated persulfate (PS), in order to provide “in-situ” and “fingerprinted” analysis of reaction contribution and bond cleavage process based on isotope fractionation. As results, radical oxidants including SO 4 ·- and ·OH were generated through thermal activation of PS, and proved to play dominate roles in ATZ degradation. Inconceivably, the isotope fractionation by single SO 4 ·- dominated reaction showed weak and positive C isotope fractionation, with ε C of 1.58‰ at pH 4 and 0.65‰ at pH 7, respectively. Reactions by single SO 4 ·- and ·OH can be distinguished resulting from their significantly different ε and Ʌ C/H values. Changes of δ 13 C and δ 2 H values during ATZ degradation by heat-activated PS followed Rayleigh equation well, with the ε C , ε H and Ʌ C/H values of -1.5‰, -21.1‰, 6.60 at pH 4 and -2.7‰, -36.6‰, 10.02 at pH 7 respectively. The relative contribution of SO 4 ·- radical to ATZ degradation was ca.100% at pH 4 and 83.9% at pH 7. The isotope fractionation study and DFT calculations suggested that single electron transfer with the cleavage of C-Cl bond was dominated and displayed inverse C isotope fractionation for SO 4 ·- oxidation, which was different from that of ·OH oxidation and more selective to dehalogenate reaction. This research emphasized the promising technology of CSIA, which can achieve accurate identification of reaction contribution and pathways in advanced oxidation process." @default.
• W4308469655 created "2022-11-12" @default.
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• W4308469655 date "2023-02-01" @default.
• W4308469655 modified "2023-10-15" @default.
• W4308469655 title "Insights into atrazine degradation by thermally activated persulfate: Evidence from dual C–H isotope analysis and DFT simulations" @default.
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• W4308469655 doi "https://doi.org/10.1016/j.cej.2022.140207" @default.
• W4308469655 hasPublicationYear "2023" @default.
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