粉煤灰表面光降解过程中 1,2,3,4-四氯二苯并对二恶英与六种共存多环芳烃的交叉偶联反应

IF 11.3 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL
Ying Zhang, Shengnan Zhang, Xiaoyu Li, Zunyao Wang* and Ruijuan Qu*, 
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引用次数: 0

摘要

垃圾焚烧过程中的不利条件会导致产生二恶英和多环芳烃(PAHs)。本研究旨在探讨 1,2,3,4-四氯二苯并对二恶英(1,2,3,4-TCDD)和六种共存的低分子量多环芳烃在飞灰表面光降解过程中的去除效率和可能的交叉耦合效应。由于这六种多环芳烃具有较高的光活性和光屏蔽效应,它们对 1,2,3,4-TCDD 的光降解具有抑制作用,使去除效率降低了 4.1%-21.2%。通过 LC-MS 和 GC-MS 鉴定了 1,2,3,4-TCDD 和多环芳烃的常见降解产物,并通过键离解能、激发能、前沿电子密度和过渡态的理论计算验证了初级产物的形成。此外,在混合辐照样品中观察到了 1,2,3,4-TCDD 的高分子量偶联产物及其与 PAHs 的相互作用产物,并提出了两种偶联消除机制,分别说明了它们是通过 C-O-C 键和 -COO- 键形成的。根据毒性预测分析,大多数相互作用产物的发育毒性和致突变性均高于 1,2,3,4-三氯丁二烯。该研究对垃圾焚烧过程中飞灰表面共存的二恶英和多环芳烃的转化、相互作用及相关生态风险提供了一些新的认识。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Cross-Coupling of 1,2,3,4-Tetrachlororodibenzo-p-dioxin with Six Coexisting Polycyclic Aromatic Hydrocarbons during Photodegradation on a Fly Ash Surface

Cross-Coupling of 1,2,3,4-Tetrachlororodibenzo-p-dioxin with Six Coexisting Polycyclic Aromatic Hydrocarbons during Photodegradation on a Fly Ash Surface

The adverse conditions of the garbage incineration process can lead to the generation of dioxins and polycyclic aromatic hydrocarbons (PAHs). This study aimed to investigate the removal efficiency and possible cross-coupling effect of 1,2,3,4-tetrachlorodibenzo-p-dioxin (1,2,3,4-TCDD) and six coexisting low-molecular-weight PAHs during photodegradation on the fly ash surface. Due to their higher photoreactivity and light-shielding effect, the six PAHs exhibited inhibitory effects on the photodegradation of 1,2,3,4-TCDD, causing a reduction of 4.1%–21.2% in the removal efficiency. Common degradation products of 1,2,3,4-TCDD and PAHs were identified by LC–MS and GC–MS, and the formation of primary products was verified by theoretical calculations of bond dissociate energies, excitation energy, frontier electron densities, and transition states. In addition, high-molecular-weight coupling products of 1,2,3,4-TCDD and its interaction products with PAHs were observed in the mixed irradiation samples, and two coupling elimination mechanisms were proposed to illustrate their formation through C–O–C bonding and −COO– bonding, respectively. According to toxicity prediction analysis, the developmental toxicity and mutagenicity of most interaction products were higher than 1,2,3,4-TCDD. This study provided some new insights into the transformation, interaction, and related ecological risks of dioxins and PAHs coexisting on the surface of fly ash during the waste incineration process.

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来源期刊
环境科学与技术
环境科学与技术 环境科学-工程:环境
CiteScore
17.50
自引率
9.60%
发文量
12359
审稿时长
2.8 months
期刊介绍: Environmental Science & Technology (ES&T) is a co-sponsored academic and technical magazine by the Hubei Provincial Environmental Protection Bureau and the Hubei Provincial Academy of Environmental Sciences. Environmental Science & Technology (ES&T) holds the status of Chinese core journals, scientific papers source journals of China, Chinese Science Citation Database source journals, and Chinese Academic Journal Comprehensive Evaluation Database source journals. This publication focuses on the academic field of environmental protection, featuring articles related to environmental protection and technical advancements.
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