氯化藻有机质介导有机污染物光降解机理研究

IF 11.4 1区环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL

Water Research Pub Date : 2025-04-17 DOI:10.1016/j.watres.2025.123674

Dong Wan, Chengjie Yu, Yafei Zhao, Gaofei Song, Wujuan Mi, Yuxuan Zhu, Changzi Liu, Yonghong Bi

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引用次数: 0

摘要

藻类有机物（AOM）会严重影响水生环境中溶解有机物的光化学行为。本研究调查了氯化对来自铜绿微囊藻的 AOM 的光物理和光化学特性的影响，将这些变化与天然有机物（NOM）中观察到的变化进行了比较，并考察了它们对有机污染物光降解的影响，尤其侧重于以 N,N-二乙基间甲苯胺（DEET）为模型底物。结果表明，氯化大大改变了 AOM 的光化学反应活性。AOM 和 NOM 具有不同的反应活性，反映了它们不同的分子组成和官能团。具体来说，氯化降低了 AOM 的芳香度（SUVA254 降低了 ∼ 42%）和分子量（降低了 ∼ 30%），导致荧光峰向低波长移动。它还增强了单线态氧（1O2）和羟自由基（-OH）的形成。氯化细胞外有机物（EOM）的 -OH 量子产率显著增加，在游离可得氯（FAC）剂量较高（FAC/TOC 比率为 2.0）的情况下增加了 200 倍。在氯化 EOM 中，DEET 的光降解（包括 H-萃取和 -OH 的羟基化）明显加快，这突出表明了氯化 AOM 在推动光敏降解过程中的关键作用。研究结果强调了氯化在改变 AOM 的光化学特性方面的作用，这对促进污染物在自然和工程水生系统中的转化具有重要意义。

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Photodegradation mechanism of organic contaminants mediated by chlorinated algal organic matter

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Photodegradation mechanism of organic contaminants mediated by chlorinated algal organic matter

Algal organic matter (AOM) significantly influences the photochemical behavior of dissolved organic matter in aquatic environments. This study investigated the effects of chlorination on the photophysical and photochemical properties of AOM derived from Microcystis aeruginosa, compared these alterations with those observed for natural organic matter (NOM), and examined their impact on the photodegradation of organic contaminants, with a particular focus on N,N‑diethyl-m-toluamide (DEET) as a model substrate. The results demonstrated that chlorination substantially altered the photochemical reactivity of AOM. AOM and NOM exhibit distinct reactivities, reflecting their varied molecular compositions and functional groups. Specifically, chlorination reduced the aromaticity (SUVA₂₅₄ decreased by ∼42 %) and molecular weight (decreased by ∼30 %) of AOM, resulting in a shift of fluorescence peaks to lower wavelengths. It also enhanced the formation of singlet oxygen (¹O₂) and hydroxyl radical (^•OH). Chlorinated extracellular organic matter (EOM) exhibited a remarkable increase in ^•OH quantum yield, with a 200-fold enhancement at a high free available chlorine (FAC) dose (FAC/TOC ratio of 2.0). The photodegradation of DEET, involved H-abstraction and hydroxylation by ^•OH, was significantly accelerated in chlorinated EOM, highlighting the critical role of chlorinated AOM in driving photosensitized degradation processes. The findings emphasized the role of chlorination in altering AOM's photochemical properties, with significant implications for the enhanced transformation of contaminants in natural and engineered aquatic systems.

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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.