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过氧乙酸-钌(III)氧化工艺用于降解水中的微量污染物

Peracetic Acid-Ruthenium(III) Oxidation Process for the Degradation of Micropollutants in Water.

作者信息

Li Ruobai, Manoli Kyriakos, Kim Juhee, Feng Mingbao, Huang Ching-Hua, Sharma Virender K

机构信息

Program for the Environment and Sustainability, Department of Environmental and Occupational Health, School of Public Health, Texas A&M University, 212 Adriance Lab Road, College Station, Texas 77844, United States.

School of Civil and Environmental Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States.

出版信息

Environ Sci Technol. 2021 Jul 6;55(13):9150-9160. doi: 10.1021/acs.est.0c06676. Epub 2021 Jun 15.

Abstract

This paper presents an advanced oxidation process (AOP) of peracetic acid (PAA) and ruthenium(III) (Ru(III)) to oxidize micropollutants in water. Studies of PAA-Ru(III) oxidation of sulfamethoxazole (SMX), a sulfonamide antibiotic, in 0.5-20.0 mM phosphate solution at different pH values (5.0-9.0) showed an optimum pH of 7.0 with a complete transformation of SMX in 2.0 min. At pH 7.0, other metal ions (i.e., Fe(II), Fe(III), Mn(II), Mn(III), Co(II), Cu(II), and Ni(II)) in 10 mM phosphate could activate PAA to oxidize SMX only up to 20%. The PAA-Ru(III) oxidation process was also unaffected by the presence of chloride and carbonate ions in solution. Electron paramagnetic resonance (EPR) measurements and quenching experiments showed the dominant involvement of the acetyl(per)oxyl radicals (i.e., CHC(O)O and CHC(O)OO) for degrading SMX in the PAA-Ru(III) oxidation process. The transformation pathways of SMX by PAA-Ru(III) were proposed based on the identified intermediates. Tests with other pharmaceuticals demonstrated that the PAA-Ru(III) oxidation system could remove efficiently a wide range of pharmaceuticals (9 compounds) in the presence of phosphate ions in 2.0 min at neutral pH. The knowledge gained herein on the effective role of Ru(III) to activate PAA to oxidize micropollutants may aid in developing Ru(III)-containing catalysts for PAA-based AOPs.

摘要

本文提出了一种过氧乙酸(PAA)和钌(III)(Ru(III))的高级氧化工艺(AOP),用于氧化水中的微污染物。在不同pH值(5.0 - 9.0)的0.5 - 20.0 mM磷酸盐溶液中,对磺胺类抗生素磺胺甲恶唑(SMX)进行PAA - Ru(III)氧化研究,结果表明最佳pH值为7.0,在该条件下SMX可在2.0分钟内完全转化。在pH 7.0时,10 mM磷酸盐中的其他金属离子(即Fe(II)、Fe(III)、Mn(II)、Mn(III)、Co(II)、Cu(II)和Ni(II))仅能激活PAA将SMX氧化至20%。PAA - Ru(III)氧化过程也不受溶液中氯离子和碳酸根离子的影响。电子顺磁共振(EPR)测量和猝灭实验表明,在PAA - Ru(III)氧化过程中,乙酰(过)氧自由基(即CHC(O)O和CHC(O)OO)对降解SMX起主要作用。基于所鉴定的中间体,提出了PAA - Ru(III)作用下SMX的转化途径。对其他药物的测试表明,在中性pH值下,PAA - Ru(III)氧化体系在存在磷酸根离子的情况下,可在2.0分钟内有效去除多种药物(9种化合物)。本文所获得的关于Ru(III)激活PAA氧化微污染物的有效作用的知识,可能有助于开发用于基于PAA的AOPs的含Ru(III)催化剂。

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