Ru(III) catalyzed permanganate oxidation of aniline at environmentally relevant pH

来源 :Journal of Environmental Sciences | 被引量 : 0次 | 上传用户:huoxingtan22
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Ru(III) was employed as catalyst for aniline oxidation by permanganate at environmentally relevant pH for the first time. Ru(III) could significantly improve the oxidation rate of aniline by5–24 times with its concentration increasing from 2.5 to 15 μmol/L. The reaction of Ru(III)catalyzed permanganate oxidation of aniline was first-order with respect to aniline,permanganate and Ru(III), respectively. Thus the oxidation kinetics can be described by a third-order rate law. Aniline degradation by Ru(III) catalyzed permanganate oxidation was markedly influenced by pH, and the second-order rate constant(ktapp) decreased from 643.20 to 2.67(mol/L)-1sec-1with increasing pH from 4.0 to 9.0, which was possibly due to the decrease of permanganate oxidation potential with increasing pH. In both the uncatalytic and catalytic permanganate oxidation, six byproducts of aniline were identified in UPLC–MS/MS analysis. Ru(III), as an electron shuttle, was oxidized by permanganate to Ru(VI) and Ru(VII),which acted the co-oxidants for decomposition of aniline. Although Ru(III) could catalyze permanganate oxidation of aniline effectively, dosing homogeneous Ru(III) into water would lead to a second pollution. Therefore, efforts would be made to investigate the catalytic performance of supported Ru(III) toward permanganate oxidation in our future study. Ru (III) was employed as catalyst for aniline oxidation by permanganate at environmentally relevant relevant pH for the first time. Ru (III) could significantly improve the oxidation rate of aniline by 5-24 times with its concentration increasing from 2.5 to 15 μmol / L. The reaction of Ru (III) catalyzed permanganate oxidation of aniline was first-order with respect to aniline, permanganate and Ru (III), respectively. Aniline degradation by Ru (III) III with increasing pH from 4.0 to 9.0, which could possibly due to the decrease of III-III) catalyzed permanganate oxidation was markedly influenced by pH, and the second-order rate constant (ktapp) decreased from 643.20 to 2.67 (mol / L) In both the uncatalytic and catalytic permanganate oxidation, six by products of aniline were identified in UPLC-MS / MS analysis. Ru (III), as an electron shuttle, was oxidized by permanganate to Ru (VI) and Ru ( VII), which acted the co-oxidants for decomposition of aniline. Although Ru (III) could catalyze permanganate oxidation of aniline effectively, dosing homogeneous Ru (III) into water would lead to a second pollution. Therefore, it would be made to investigate the catalytic performance of supported Ru (III) toward permanganate oxidation in our future study.
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