腐殖质与3-氯苯胺光敏反应的多元素同位素分馏分析

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

Water Research Pub Date : 2025-04-25 DOI:10.1016/j.watres.2025.123633

Ning Min, Jun Yao, Hao Li, Steffen Kümmel, Thomas Schaefer, Hartmut Herrmann, Hans Herrmann Richnow

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引用次数: 0

摘要

溶解有机物包括腐殖质样物质（HS），作为光敏剂参与电子转移反应，可产生多种活性物质，如OH自由基和激发态HS （3HS*）等，促进3-氯苯胺（3-CA）等有机污染物的降解。以3-CA为探针，采用多元素化合物特异性稳定同位素分析（ME-CSIA）表征光敏机理。利用人造阳光照射HS，通过研究动力学同位素效应（2H, 13C， 15N和37Cl）来阐明反应机理，表征第一次不可逆变键反应。在HS/UV实验（OH自由基和三重态）中检测到独特的富集因子（13C为-1.0±0.3,2H为7.4±1.7,37Cl为2.3±0.7），表明反应机制复杂。利用人工光敏剂4,5,6,7-四氯-2 ',4 ',5 ',7 ' -四氯荧光素在O2存在或无O2存在（Rose Bengal-O2 free）下的三重态参比实验得到了特征富集因子（13C为-0.3±0.2‰和-1.2±0.2‰，15N为2.7±0.5‰和4.8±1.0‰，37Cl为8.4±3.3‰和11.2±6.8‰），从而解释了与3-CA的三重态反应机理。2H与13C、15N与13C、37N与13C组分的相关性可用于诊断环境中的光敏反应，并可用于区分生物降解、水解和光敏HS反应。

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Multi-Element Isotope Fractionation Analysis to Investigate the Photosensitized Reactions of Humic Substance with 3-Chloroaniline

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Multi-Element Isotope Fractionation Analysis to Investigate the Photosensitized Reactions of Humic Substance with 3-Chloroaniline

Dissolved organic matter including humic-like substances (HS), acting as photosensitizers participating in electron transfer reactions, can generate a variety of reactive species, such as OH radicals and excited triplet state HS (³HS*) and related, which promote the degradation of organic contaminants such as 3-chloroaniline (3-CA). Multi-element-compound-specific stable isotope analysis (ME-CSIA) was applied to characterize photosensitized mechanisms employing 3-CA as a probe. HS were irradiated with artificial sunlight for elucidation of the reaction mechanisms by studying the kinetic isotope effect (²H, ¹³C, ¹⁵N and ³⁷Cl) to characterize the first irreversible bond change reaction. Unique enrichment factors (-1.0±0.3 for ¹³C, 7.4±1.7 for ²H and 2.3±0.7 for ³⁷Cl) have been detected in HS/UV experiments (OH radical and triplet state), which indicate complex reaction mechanisms. Triplet state reference experiments with the artificial photosensitizers 4,5,6,7-tetrachloro-2′,4′,5′,7′-tetraiodofluorescein in the presence O₂ (Rose Bengal-O₂) or absence of O₂ (Rose Bengal-O₂ free) yielded characteristic enrichment factors (-0.3±0.2‰ and -1.2±0.2‰ for ¹³C, 2.7±0.5‰ and 4.8±1.0‰ for ¹⁵N and 8.4±3.3‰ and 11.2±6.8‰ for ³⁷Cl), allowing interpretation of reaction mechanisms of triplet state with 3-CA. The correlation of ²H vs ¹³C, ¹⁵N vs ¹³C and ³⁷N vs ¹³C fractions could be used diagnostically to determine photosensitized reactions in the environment and to differentiate between biodegradation, hydrolysis and photosensitized HS reaction.

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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.