Mechanistic insight into the environmental fate of highly concerned transformation products of aqueous micropollutants during the solar/chlorine treatment

IF 12.4 1区环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Water Research Pub Date : 2025-02-28 DOI:10.1016/j.watres.2025.123413

Yuwei Xie, Wenzheng Chen, Zhantu Ye, Junmei Yan, Xin Yu, Mingbao Feng

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Abstract

Transformation products (TPs) arising from the degradation of micropollutants have been frequently detected in various water bodies and may exhibit higher toxicity than their parent compounds. However, the current understanding of their chemical reactivity remains limited, and the mechanisms underlying the solar-driven oxidation processes (e.g., solar/chlorine system) of TPs have not been well investigated. This study explored the elimination of six typical TPs derived from carbamazepine (CBZ) and atrazine (ATZ) by solar/oxidant systems. It was observed that these TPs could be effectively degraded in the solar/oxidant systems, except for the solar/hydrogen peroxide system. The reactivity evaluation and quantitative contribution analysis revealed that hydroxyl radicals (^•OH) and ozone played pivotal roles in the removal of all six typical TPs by the solar/chlorine system, whereas the reactive chlorine species contributed minimally. The transformation mechanisms of carbamazepine 10, 11-epoxide (CBZ-EP) involved hydroxyl addition and electron transfer, while the TPs of ATZ underwent dealkylation only. The computational study indicated that ^•OH primarily reacted with CBZ-EP via radical addition reaction. Furthermore, the TPs of CBZ-EP and hydroxyatrazine showed no obvious change in environmental persistence but enhanced mobility and toxicity compared to the parent compounds, implying treatment-driven secondary risks. Overall, this investigation provided an in-depth mechanistic exploration of the transformation behaviors, fate, and secondary environmental risks of highly concerned TPs under the solar/oxidant treatments.

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在太阳能/氯处理过程中高度关注的水微污染物转化产物的环境命运的机制洞察

各种水体中经常检测到微污染物降解产生的转化产物（TPs），其毒性可能高于母体化合物。然而，目前人们对其化学反应性的了解仍然有限，而且对太阳驱动的 TPs 氧化过程（如太阳/氯系统）的基本机制也没有进行深入研究。本研究探讨了太阳能/氧化剂系统如何消除六种典型的 TPs，这些 TPs 来自卡马西平（CBZ）和阿特拉津（ATZ）。结果表明，除太阳能/过氧化氢系统外，其他太阳能/氧化剂系统都能有效地降解这些 TPs。反应性评估和定量贡献分析表明，羟基自由基（-OH）和臭氧在太阳能/氯气系统去除所有六种典型 TPs 的过程中发挥了关键作用，而反应性氯物种的贡献微乎其微。卡马西平 10、11-环氧化物（CBZ-EP）的转化机制涉及羟基加成和电子转移，而 ATZ 的 TPs 只发生了脱烷基作用。计算研究表明，-OH 主要通过自由基加成反应与 CBZ-EP 发生反应。此外，与母体化合物相比，CBZ-EP 和羟基atrazine 的 TPs 在环境持久性方面没有明显变化，但流动性和毒性增强，这意味着治疗驱动的二次风险。总之，这项研究从机理上深入探讨了在太阳能/氧化剂处理条件下，人们高度关注的可塑性废物的转化行为、归宿和二次环境风险。

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来源期刊

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.