254 nm/313 nm辐照下丁香酚和乙丁香酮水相氧化动力学及产物特性研究

IF 2.9 4区 环境科学与生态学 Q3 ENVIRONMENTAL SCIENCES
Zixuan Wang, Zhaolian Ye, Dandan Hu, Hui Wang, Xinlei Ge
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引用次数: 0

摘要

生物质燃烧释放的酚类化合物是水相二次有机气溶胶(aqSOA)形成的重要前体,但对其形成机制、产物特性和相关动力学的研究有限,特别是在不同波长紫外线(UV)光下的比较研究。因此,本研究选择丁香酚(Eug)和乙酰丁香酮(AS)为前驱体,在254 nm/313 nm两种紫外光源下研究水相氧化反应动力学。结果表明,拟一级速率常数kobs与pH值、初始酚类化合物浓度和H2O2添加量密切相关。kobs的排序为kO2 >; kair > kN2,说明氧气有利于降解。清除实验确定了活性氧(ROS)的相对贡献,结果表明•OH和O2•−在Eug和AS的光衰中都起着重要作用,其中O2•−的作用更为突出。产物在365 nm处的吸光率在前7 h上升,随后下降,表明吸收光物质的形成和随后的光漂白。结合反应过程中有机酸、氧化特性和产物组成的变化,推测两种酚类化合物OH水相氧化的产物发生功能化后破碎,导致氧化程度增加。有机酸通过脱氢或开环形成,进一步影响气候变化和空气质量。本研究首次比较了两种酚类物质在313 nm紫外光源下的反应速率,并全面分析了产物特征和机理,对扩充大气动力学数据库,了解大气中酚类物质的化学活性具有重要意义。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Study on the kinetics and product characteristics of aqueous-phase oxidation of Eugenol and acetosyringone upon 254 nm/313 nm irradiation

Study on the kinetics and product characteristics of aqueous-phase oxidation of Eugenol and acetosyringone upon 254 nm/313 nm irradiation

Phenolic compounds emitted from biomass burning are important precursors for the formation of aqueous secondary organic aerosols (aqSOA), but there is limited research on the formation mechanisms, product characteristics, and related kinetics, especially on comparative studies under different wavelengths of ultraviolet (UV) light. Therefore, this study selected eugenol (Eug) and acetosyringone (AS) as precursors to investigate the kinetics of aqueous-phase oxidation reactions under two UV light sources (254 nm/313 nm). The results showed that the pseudo-first-order rate constant, kobs was highly dependent on pH value, initial phenolic compounds concentration and added H2O2 dosages. The ranking of kobs were kO2 > kair > kN2, indicating that oxygen is beneficial for degradation. Scavenging experiments determined the relative contributions of reactive oxygen species (ROS) and the results showed that both •OH and O2•− played significant roles in the photodecay of Eug and AS, with O2•− being more prominent. Light-absorbance at 365 nm of products increased for the first 7 h, and then decreased at the later stage indicated the formation of light-absorbing substances and subsequent photobleaching. Combining the changes in organic acids, oxidative characteristics, and product composition during the reaction, it is speculated that the products of the OH aqueous-phase oxidation of the two phenolic compounds undergo functionalization followed by fragmentation, leading to an increase in oxidation degree. Organic acids are formed through dehydrogenation or ring-opening, further impacting climate change and air quality. This study for the first time compared the reaction rates of the two phenols under 313 nm UV light source and comprehensively analyze the products characteristics and mechanisms, which was significant for expanding the atmospheric kinetics database and understanding the chemical activity of phenolic substances in the atmosphere.

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来源期刊
Air Quality Atmosphere and Health
Air Quality Atmosphere and Health ENVIRONMENTAL SCIENCES-
CiteScore
8.80
自引率
2.00%
发文量
146
审稿时长
>12 weeks
期刊介绍: Air Quality, Atmosphere, and Health is a multidisciplinary journal which, by its very name, illustrates the broad range of work it publishes and which focuses on atmospheric consequences of human activities and their implications for human and ecological health. It offers research papers, critical literature reviews and commentaries, as well as special issues devoted to topical subjects or themes. International in scope, the journal presents papers that inform and stimulate a global readership, as the topic addressed are global in their import. Consequently, we do not encourage submission of papers involving local data that relate to local problems. Unless they demonstrate wide applicability, these are better submitted to national or regional journals. Air Quality, Atmosphere & Health addresses such topics as acid precipitation; airborne particulate matter; air quality monitoring and management; exposure assessment; risk assessment; indoor air quality; atmospheric chemistry; atmospheric modeling and prediction; air pollution climatology; climate change and air quality; air pollution measurement; atmospheric impact assessment; forest-fire emissions; atmospheric science; greenhouse gases; health and ecological effects; clean air technology; regional and global change and satellite measurements. This journal benefits a diverse audience of researchers, public health officials and policy makers addressing problems that call for solutions based in evidence from atmospheric and exposure assessment scientists, epidemiologists, and risk assessors. Publication in the journal affords the opportunity to reach beyond defined disciplinary niches to this broader readership.
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