酸度对二次有机气溶胶中活性氧生成的影响

IF 6.7 Q1 ENGINEERING, ENVIRONMENTAL ACS Environmental Au Pub Date : 2022-04-29 DOI:10.1021/acsenvironau.2c00018
Jinlai Wei, Ting Fang and Manabu Shiraiwa*, 
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引用次数: 7

摘要

活性氧(Reactive oxygen species, ROS)通过在体内引起氧化应激,在大气二次有机气溶胶(secondary organic aerosol, SOA)的化学转化和气溶胶健康效应中发挥关键作用。酸度是大气气溶胶的一项重要理化性质,但其对SOA形成活性氧的影响尚不清楚。通过应用电子顺磁共振自旋俘获技术和Diogenes化学发光实验,我们发现异戊二烯、α-松油醇、α-蒎烯、β-蒎烯、甲苯和萘在不同pH值范围内氧化产生的SOA在1-7.4范围内的自由基产率和组成有很大差异。我们观察到异戊二烯SOA在中性pH下具有大量的羟基自由基(•OH)和有机自由基产率,其总自由基产率是酸性条件下的1.5-2倍。超氧化物(O2•-)是所有类型SOA在较低pH下生成的主要物质。在中性pH下,α-松油醇SOA能大量生成碳中心有机自由基,而芳香型SOA则没有形成自由基。对模型化合物的进一步实验表明,由于酸催化过氧化物的重排,有机过氧化物的分解导致自由基的形成可能在较低的pH下被抑制。我们还观察到,在酸性条件下,与中性pH相比,生物源性和芳香性SOA的过氧化氢(H2O2)的摩尔产率提高了1.5-3倍,这可能是由于α-羟基过氧化物和醌氧化还原循环的分解增强。这些发现对于理解ROS在大气和生理环境中的形成机制和动力学至关重要。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

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Effects of Acidity on Reactive Oxygen Species Formation from Secondary Organic Aerosols

Reactive oxygen species (ROS) play a critical role in the chemical transformation of atmospheric secondary organic aerosols (SOA) and aerosol health effects by causing oxidative stress in vivo. Acidity is an important physicochemical property of atmospheric aerosols, but its effects on the ROS formation from SOA have been poorly characterized. By applying the electron paramagnetic resonance spin-trapping technique and the Diogenes chemiluminescence assay, we find highly distinct radical yields and composition at different pH values in the range of 1–7.4 from SOA generated by oxidation of isoprene, α-terpineol, α-pinene, β-pinene, toluene, and naphthalene. We observe that isoprene SOA has substantial hydroxyl radical (OH) and organic radical yields at neutral pH, which are 1.5–2 times higher compared to acidic conditions in total radical yields. Superoxide (O2•–) is found to be the dominant species generated by all types of SOAs at lower pH. At neutral pH, α-terpineol SOA exhibits a substantial yield of carbon-centered organic radicals, while no radical formation is observed by aromatic SOA. Further experiments with model compounds show that the decomposition of organic peroxide leading to radical formation may be suppressed at lower pH due to acid-catalyzed rearrangement of peroxides. We also observe 1.5–3 times higher molar yields of hydrogen peroxide (H2O2) in acidic conditions compared to neutral pH by biogenic and aromatic SOA, likely due to enhanced decomposition of α-hydroxyhydroperoxides and quinone redox cycling, respectively. These findings are critical to bridge the gap in understanding ROS formation mechanisms and kinetics in atmospheric and physiological environments.

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ACS Environmental Au
ACS Environmental Au 环境科学-
CiteScore
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期刊介绍: ACS Environmental Au is an open access journal which publishes experimental research and theoretical results in all aspects of environmental science and technology both pure and applied. Short letters comprehensive articles reviews and perspectives are welcome in the following areas:Alternative EnergyAnthropogenic Impacts on Atmosphere Soil or WaterBiogeochemical CyclingBiomass or Wastes as ResourcesContaminants in Aquatic and Terrestrial EnvironmentsEnvironmental Data ScienceEcotoxicology and Public HealthEnergy and ClimateEnvironmental Modeling Processes and Measurement Methods and TechnologiesEnvironmental Nanotechnology and BiotechnologyGreen ChemistryGreen Manufacturing and EngineeringRisk assessment Regulatory Frameworks and Life-Cycle AssessmentsTreatment and Resource Recovery and Waste Management
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