Advanced reduction processes initiated by oxidative radicals for trichloroacetic acid degradation: Performance, radical generation, and mechanism

IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Water Research Pub Date : 2024-10-06 DOI:10.1016/j.watres.2024.122587
Qiang Zhang, Xiaolei Wang, Nannan Wu, Changyin Zhu, Wenxiu Qin, Danyu Huang, Dongmei Zhou
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Abstract

The degradation of haloacetic acids (HAAs) in aqueous environments poses a challenge due to their oxidative resistance. Given that HAAs are highly carcinogenic disinfection byproducts, it is imperative to develop effective degradation methods to reduce their potential health risk. In this study, we found that only 27.2% of 200 μM trichloroacetic acid (TCA) was removed in the UV-activated persulfate (PS) system after 2 h, while complete removal was achieved with the addition of 15 mM formic acid (FA). The main products of TCA degradation were dichloroacetic acid and monochloroacetic acid. Results from free radical quenching experiments and electron paramagnetic resonance spectroscopy analyses indicated that reductive carbon dioxide radical (CO2•−) was the main active species responsible for TCA reduction. Oxidative radicals (i.e., SO4•− and OH) generated from PS activation reacted with FA to form CO2•−, efficiently degrading TCA. The effects of PS and FA concentrations, solution pH, anions (e.g., Cl, SO42−, and HCO3), and small organic molecules (e.g., methanol, ethanol, and acetic acid) on degradation efficiency were examined. Overall, this study proposes a simple and efficient method to improve the degradation efficiency of HAAs in the UV/PS system and provides new insights into the advanced reduction processes used for water treatments.

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由氧化自由基引发的用于降解三氯乙酸的高级还原过程:性能、自由基生成和机理
由于卤乙酸具有抗氧化性,因此在水环境中降解卤乙酸是一项挑战。鉴于卤乙酸是高致癌的消毒副产物,开发有效的降解方法以降低其潜在的健康风险势在必行。在这项研究中,我们发现在紫外线激活的过硫酸盐(PS)系统中,200 μM的三氯乙酸(TCA)在2小时后仅有27.2%被去除,而加入15 mM甲酸(FA)后则可完全去除。TCA 降解的主要产物是二氯乙酸和一氯乙酸。自由基淬灭实验和电子顺磁共振光谱分析结果表明,还原性二氧化碳自由基(CO2--)是导致 TCA 还原的主要活性物种。PS 活化产生的氧化自由基(即 SO4--和 -OH)与 FA 反应生成 CO2--,从而有效降解 TCA。研究还考察了 PS 和 FA 浓度、溶液 pH 值、阴离子(如 Cl-、SO42- 和 HCO3-)以及小分子有机物(如甲醇、乙醇和乙酸)对降解效率的影响。总之,本研究提出了一种简单而有效的方法来提高 UV/PS 系统中 HAAs 的降解效率,并为用于水处理的高级还原过程提供了新的见解。
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来源期刊
Water Research
Water Research 环境科学-工程:环境
CiteScore
20.80
自引率
9.40%
发文量
1307
审稿时长
38 days
期刊介绍: Water Research, along with its open access companion journal Water Research X, serves as a platform for publishing original research papers covering various aspects of the science and technology related to the anthropogenic water cycle, water quality, and its management worldwide. The audience targeted by the journal comprises biologists, chemical engineers, chemists, civil engineers, environmental engineers, limnologists, and microbiologists. The scope of the journal include: •Treatment processes for water and wastewaters (municipal, agricultural, industrial, and on-site treatment), including resource recovery and residuals management; •Urban hydrology including sewer systems, stormwater management, and green infrastructure; •Drinking water treatment and distribution; •Potable and non-potable water reuse; •Sanitation, public health, and risk assessment; •Anaerobic digestion, solid and hazardous waste management, including source characterization and the effects and control of leachates and gaseous emissions; •Contaminants (chemical, microbial, anthropogenic particles such as nanoparticles or microplastics) and related water quality sensing, monitoring, fate, and assessment; •Anthropogenic impacts on inland, tidal, coastal and urban waters, focusing on surface and ground waters, and point and non-point sources of pollution; •Environmental restoration, linked to surface water, groundwater and groundwater remediation; •Analysis of the interfaces between sediments and water, and between water and atmosphere, focusing specifically on anthropogenic impacts; •Mathematical modelling, systems analysis, machine learning, and beneficial use of big data related to the anthropogenic water cycle; •Socio-economic, policy, and regulations studies.
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