Mechanisms and product toxicity of activated carbon/peracetic acid for degradation of sulfamethoxazole: implications for groundwater remediation

IF 12.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL
Chaomeng Dai , Si Li , Yanping Duan , Kah Hon Leong , Shuguang Liu , Yalei Zhang , Lang Zhou , Yaojen Tu
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引用次数: 66

Abstract

Carbon-based materials activated peracetic acid (PAA) to repair groundwater is an environmentally friendly and low-cost technology to overcome secondary pollution problems. In this study, thermally modified activated carbon (AC600) was applied to activate PAA to degrade sulfamethoxazole (SMX). And the effect of groundwater pH, chloride ion (Cl), bicarbonate (HCO3), sulfate ion (SO42−), and natural organic matter (NOM) on SMX removal by AC600/PAA process was studied in detail. PAA could be effectively activated by AC600. Increasing AC600 dose (10–100mg/L) or PAA dosages (0.065–0.39 mM) generally enhanced the SMX removal, the excellent performance in SMX removal was achieved at 50 mg/L AC600 and 0.26 mM PAA. The removal of SMX was well-described by second-order kinetic, with the rate constant (kobs) of 10.79 M−1s−1, both much greater than the removal constants of PAA alone (0.034 M−1s−1) and AC600 alone (1.774 M−1s−1). R-O·(CH3C(O)OO·, CH3C(O)O·) and electron-transfer process were proved to be responsible for the removal of SMX while HO· and 1O2 made little to no contribution to the novel PAA/AC600 system, which differs from typical advanced oxidation processes. The SMX can be removed effectively over a wide pH range (3-9), exhibiting a remarkable pH-tolerant performance. Sulfate ion (SO42−), dissolved oxygen (DO), NOM displayed negligible influence on the SMX removal. Bicarbonate (HCO3) exerted an inhibitory effect on SMX abatement, while chloride ion (Cl) promoted the removal of SMX. This showed excellent anti-interference capacity and satisfactory decontamination performance under actual groundwater conditions. Furthermore, the degradation pathways of SMX were proposed, there was no obvious difference in the acute toxicity of the mixed products during the degradation process. It will facilitate further research of metal-free catalyst/PAA system as a new strategy for groundwater in-situ remediation technology.

活性炭/过氧乙酸降解磺胺甲恶唑的机理和产物毒性:对地下水修复的影响
碳基材料活化过氧乙酸(PAA)修复地下水是一种环境友好、低成本的解决地下水二次污染问题的技术。本研究采用热改性活性炭(AC600)活化PAA降解磺胺甲恶唑(SMX)。并详细研究了地下水pH、氯离子(Cl−)、碳酸氢盐(HCO3−)、硫酸盐离子(SO42−)和天然有机物(NOM)对AC600/PAA工艺去除SMX的影响。AC600能有效活化PAA。增加AC600 (10 ~ 100mg/L)或PAA (0.065 ~ 0.39 mM)对SMX的去除率普遍提高,其中AC600为50 mg/L, PAA为0.26 mM时SMX去除率最高。SMX的去除符合二级动力学,速率常数(kobs)为10.79 M−1s−1,远远大于单独的PAA (0.034 M−1s−1)和单独的AC600 (1.774 M−1s−1)。与典型的高级氧化工艺不同,R-O·(CH3C(O)OO·)、CH3C(O)O·)和电子转移过程对SMX的去除起主要作用,而HO·和1O2对新型PAA/AC600体系的去除作用很小或没有作用。SMX可以在很宽的pH范围内(3-9)有效去除,表现出卓越的耐pH性能。硫酸盐离子(SO42−)、溶解氧(DO)、NOM对SMX去除率的影响可以忽略不计。碳酸氢盐(HCO3−)对SMX的去除有抑制作用,而氯离子(Cl−)对SMX的去除有促进作用。在实际地下水条件下,具有良好的抗干扰能力和较好的去污性能。此外,提出了SMX的降解途径,在降解过程中混合产物的急性毒性没有明显差异。这将促进无金属催化剂/PAA体系作为地下水原位修复技术新策略的进一步研究。
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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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