西安市大气PM2.5分子演化和来源对其氧化潜势的影响

王帝伟; 沈振兴; 白鸽子; 李昊楠; 黄沙沙; 杨雪婷; 孙健; 徐红梅

PDF(839 KB)

中国环境科学 ›› 2025, Vol. 45 ›› Issue (2) : 629-636.

大气污染与控制

西安市大气PM_2.5分子演化和来源对其氧化潜势的影响

王帝伟, 沈振兴, 白鸽子, 李昊楠, 黄沙沙, 杨雪婷, 孙健, 徐红梅

作者信息 +

Effects of molecular evolution and emission sources on atmospheric oxidative potential in Xi’an

WANG Di-wei, SHEN Zhen-xing, BAI Ge-zi, LI Hao-nan, HUANG Sha-sha, YANG Xue-ting, SUN Jian, XU Hong-mei

Author information +

文章历史 +

摘要

为探究西安市大气细颗粒物(PM_2.5)氧化潜势(OP)的季节变化及来源,采用二硫苏糖醇(DTT)法测定了质量归一化的OP水平(OP^DTTm),分析了PM_2.5化学组分对OP的影响,结合正矩阵因子分解耦合人工神经网络-多层感知器(PMF-ANN-MLP)模型定量排放源对OP^DTTm的贡献.结果表明:西安市大气OP^DTTm在夏季最高((13.2 ±5.4) pmol/(min∙μg)),冬季最低((5.6 ±2.7) pmol/(min∙μg)).相关性分析结果表明,含硝基的芳香族化合物和羧酸类有机分子对OP^DTTm生成具有重要作用,其分子丰度的差异是导致OP^DTTm呈现季节变化的主要原因.源解析揭示,扬尘源对OP^DTTm的贡献在春季最高(26.7%),夏季交通源的贡献最高(35.1%),二次源的贡献在秋季最高(23.2%),生物质燃烧(24.5%)和燃煤(25.8%)的贡献均在冬季最高.研究结果可为制定有效的大气污染防治措施以保护人群健康提供科学依据.

Abstract

To investigate the seasonal variation and source of oxidative potential (OP) in atmospheric fine particulate matter (PM_2.5) in Xi’an, the mass normalized OP (OP^DTTm) was measured using the dithiothreitol (DTT) method, and the influence of chemical components of PM_2.5 on OP^DTTm was analyzed, and the contributions of different sources to OP^DTTm was quantified using a positive matrix factorization coupled with an artificial neural network multilayer perceptron (PMF-ANN-MLP) model. The findings revealed that OP^DTTm in Xi’an was highest during summer ((13.2 ±5.4) pmol(min∙μg)) and lowest in winter ((5.6 ±2.7) pmol(min∙μg)). Correlation analysis indicated that nitro-containing aromatic compounds and carboxylic acids have a significant impact on OP^DTTm, and the difference in molecular abundance was the main reason for the seasonal variation of OP^DTTm. Source apportionment showed that dust (26.7%), traffic (35.1%), secondary formation (23.2%), and biomass burning (24.5%) and coal combustion (25.8%) were the predominant contributors to OP^DTTm during spring, summer, autumn, and winter, respectively. These results provide a scientific foundation for developing effective air pollution control measures aimed at safeguarding public health.

导出引用

王帝伟, 沈振兴, 白鸽子, 李昊楠, 黄沙沙, 杨雪婷, 孙健, 徐红梅. 西安市大气PM_2.5分子演化和来源对其氧化潜势的影响[J]. 中国环境科学. 2025, 45(2): 629-636

WANG Di-wei, SHEN Zhen-xing, BAI Ge-zi, LI Hao-nan, HUANG Sha-sha, YANG Xue-ting, SUN Jian, XU Hong-mei. Effects of molecular evolution and emission sources on atmospheric oxidative potential in Xi’an[J]. China Environmental Science. 2025, 45(2): 629-636

中图分类号： X51

参考文献

[1] Yan C, Ma S, He Q, et al. Identification of PM_2.5 sources contributing to both brown carbon and reactive oxygen species generation in winter in Beijing, China [J]. Atmospheric Environment, 2021,246:118069.
[2] Ma Y, Cheng Y, Qiu X, et al. Sources and oxidative potential of water-soluble humic-like substances (HULIS_WS) in fine particulate matter (PM_2.5) in Beijing [J]. Atmospheric Chemistry and Physics, 2018,18(8):5607-5617.
[3] Bates J, Fang T, Verma V, et al. Review of acellular assays of ambient particulate matter oxidative potential: methods and relationships with composition, sources, and health effects [J]. Environmental Science & Technology, 2019,53(8):4003-4019.
[4] Yu S, Liu W, Xu Y, et al. Characteristics and oxidative potential of atmospheric PM_2.5 in Beijing: Source apportionment and seasonal variation [J]. Science of the Total Environment, 2019,650:277-287.
[5] Luo Y, Zeng Y, Xu H, et al. Connecting oxidative potential with organic carbon molecule composition and source-specific apportionment in PM_2.5 in Xi'an, China [J]. Atmospheric Environment, 2023,306:119808.
[6] Zhang T, Shen Z, Huang S, et al. Optical properties, molecular characterizations, and oxidative potentials of different polarity levels of water-soluble organic matters in winter PM_2.5 in six China's megacities [J]. Science of the Total Environment, 2022,853:158600.
[7] Gali N, Yang F, Jiang S, et al. Spatial and seasonal heterogeneity of atmospheric particles induced reactive oxygen species in urban areas and the role of water-soluble metals [J]. Environmental Pollution, 2015,198:86-96.
[8] Borlaza L, Weber S, Jaffrezo J, et al. Disparities in particulate matter (PM₁₀) origins and oxidative potential at a city scale (Grenoble, France)-part 2: Sources of PM₁₀ oxidative potential using multiple linear regression analysis and the predictive applicability of multilayer perceptron neural network analysis [J]. Atmospheric Chemistry and Physics, 2021,21(12):9719-9739.
[9] Verma V, Rico-Martinez R, Kotra N, et al. Contribution of water-soluble and insoluble components and their hydrophobic/hydrophilic subfractions to the reactive oxygen species-generating potential of fine ambient aerosols [J]. Environmental Science & Technology, 2012,46(20):11384-11392.
[10] Cao T, Li M, Zou C, et al. Chemical composition, optical properties, and oxidative potential of water-and methanol-soluble organic compounds emitted from the combustion of biomass materials and coal [J]. Atmospheric Chemistry and Physics, 2021,21(17):13187-13205.
[11] Liu Q, Lu Z, Xiong Y, et al. Oxidative potential of ambient PM_2.5 in Wuhan and its comparisons with eight areas of China [J]. Science of the total Environment, 2020,701:134844.
[12] Xing C, Wang Y, Yang X, et al. Seasonal variation of driving factors of ambient PM_2.5 oxidative potential in Shenzhen, China [J]. Science of the total Environment, 2023,862:160771.
[13] Wang J, Lin X, Lu L, et al. Temporal variation of oxidative potential of water soluble components of ambient PM_2.5 measured by dithiothreitol (DTT) assay [J]. Science of the Total Environment, 2019,649:969-978.
[14] Paraskevopoulou D, Bougiatioti A, Stavroulas I, et al. Yearlong variability of oxidative potential of particulate matter in an urban mediterranean environment [J]. Atmospheric Environment, 2019,206: 183-196.
[15] Charrier J, Anastasio C. On dithiothreitol (DTT) as a measure of oxidative potential for ambient particles: Evidence for the importance of soluble transition metals [J]. Atmospheric Chemistry and Physics, 2012,12(19):9321-933.
[16] Fang T, Verma V, Guo H, et al. A semi-automated system for quantifying the oxidative potential of ambient particles in aqueous extracts using the dithiothreitol (DTT) assay: Results from the Southeastern Center for Air Pollution and Epidemiology (SCAPE) [J]. Atmospheric Measurement Techniques, 2015,8(1):471-482.
[17] Janssen N, Yang A, Strak M, et al. Oxidative potential of particulate matter collected at sites with different source characteristics [J]. Science of the Total Environment, 2014,472:572-581.
[18] Perrone M, Zhou J, Malandrino M, et al. PM chemical composition and oxidative potential of the soluble fraction of particles at two sites in the urban area of Milan, Northern Italy [J]. Atmospheric Environment, 2016,128:104-113.
[19] Chirizzi D, Cesari D, Guascito M, et al. Influence of Saharan dust outbreaks and carbon content on oxidative potential of water-soluble fractions of PM_2.5 and PM₁₀ [J]. Atmospheric Environment, 2017,163:1-8.
[20] Patel A, Rastogi N. Oxidative potential of ambient fine aerosol over a semi-urban site in the Indo-Gangetic Plain [J]. Atmospheric Environment, 2018,175:127-134.
[21] Bates J, Weber R, Abrams J, et al. Reactive oxygen species generation linked to sources of atmospheric particulate matter and cardiorespiratory effects [J]. Environmental Science & Technology, 2015,49(22):13605-13612.
[22] Fang T, Verma V, Bates J, et al. Oxidative potential of ambient water-soluble PM_2.5in the southeastern United States: Contrasts in sources and health associations between ascorbic acid (AA) and dithiothreitol (DTT) assays [J]. Atmospheric Chemistry and Physics, 2016,16(6):3865-3879.
[23] Borlaza L, Cosep E, Kim S, et al. Oxidative potential of fine ambient particles in various environments [J]. Environmental Pollution, 2018, 243:1679-1688.
[24] Wang D, Shen Z, Yang X, et al. Insight into the role of NH₃/NH₄⁺ and NO_x/NO₃^- in the formation of nitrogen-containing brown carbon in Chinese megacities [J]. Environmental Science & Technology, 2024, 58:4281-4290.
[25] Wang D, Yang X, Lu H, et al. Oxidative potential of atmospheric brown carbon in six Chinese megacities: seasonal variation and source apportionment [J]. Atmospheric Environment, 2023,309:119909.
[26] Campbell S, Wolfer K, Utinger B, et al. Atmospheric conditions and composition that influence PM_2.5 oxidative potential in Beijing, China [J]. Atmospheric Chemistry and Physics, 2021,21(7):5549-5573.
[27] Yu Y, Cheng P, Li Y, et al. The association of chemical composition particularly the heavy metals with the oxidative potential of ambient PM_2.5 in a megacity (Guangzhou) of southern China [J]. Environmental Research, 2022,213:113489.
[28] Cheng Y, He K, Du Z, et al. The characteristics of brown carbon aerosol during winter in Beijing [J]. Atmospheric Environment, 2016, 127:355-364.
[29] Song J, Li M, Fan X, et al. Molecular characterization of water-and methanol-soluble organic compounds emitted from residential coal combustion using ultrahigh-resolution electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry [J]. Environmental Science & Technology, 2019,53(23):13607-13617.
[30] Kellerman A, Dittmar T, Kothawala D, et al. Chemodiversity of dissolved organic matter in lakes driven by climate and hydrology [J]. Nature Communications, 2014, 5(1):3804.
[31] Jiang H, Li J, Sun R, et al. Molecular dynamics and light absorption properties of atmospheric dissolved organic matter [J]. Environmental Science & Technology, 2021,55(15):10268-10279.
[32] Zeng Y, Shen Z, Takahama S, et al. Molecular absorption and evolution mechanisms of PM_2.5 brown carbon revealed by electrospray ionization Fourier transform-ion cyclotron resonance mass spectrometry during a severe winter pollution episode in Xi'an, China [J]. Geophysical Research Letters, 2020,47(10):e2020GL087977.
[33] Wang X, Hayeck N, Brüggemann M, et al. Chemical characteristics of organic aerosols in Shanghai: A study by ultrahigh-performance liquid chromatography coupled with orbitrap mass spectrometry [J]. Journal of Geophysical Research: Atmospheres, 2017,122(21):11703-11722.
[34] Tang J, Li J, Su T, et al. Molecular compositions and optical properties of dissolved brown carbon in biomass burning, coal combustion, and vehicle emission aerosols illuminated by excitation-emission matrix spectroscopy and Fourier transform ion cyclotron resonance mass spectrometry analysis [J]. Atmospheric Chemistry and Physics, 2020, 20(4):2513-2532.
[35] Glasius M, Thomsen D, Wang K, et al. Chemical characteristics and sources of organosulfates, organosulfonates, and carboxylic acids in aerosols in urban Xi'an, Northwest China [J]. Science of the Total Environment, 2022,810:151187.
[36] Zhang Z, Xu W, Zeng S, et al. Secondary organic aerosol formation from ambient air in summer in urban Beijing: contribution of S/IVOCs and impacts of heat waves [J]. Environmental Science & Technology Letters, 2024,11(7):738-745.
[37] Samara C. On the redox activity of urban aerosol particles: Implications for size distribution and relationships with organic aerosol components [J]. Atmosphere, 2017,8(10):205.
[38] Lin P, Rincon A G, Kalberer M, et al. Elemental composition of HULIS in the Pearl River Delta region, China: Results inferred from positive and negative electrospray high resolution mass spectrometric data [J]. Environmental Science & Technology, 2012,46(14):7454-7462.
[39] Wang K, Huang R J, Brüggemann M, et al. Urban organic aerosol composition in eastern China differs from north to south: molecular insight from a liquid chromatography-mass spectrometry (Orbitrap) study [J]. Atmospheric Chemistry and Physics, 2021,21(11):9089-9104.
[40] Jiang H, Li J, Tang J, et al. Molecular characteristics, sources, and formation pathways of organosulfur compounds in ambient aerosol in Guangzhou, South China [J]. Atmospheric Chemistry and Physics, 2022,22(10):6919-6935.
[41] Lei Y, Shen Z, Zhang T, et al. High time resolution observation of PM_2.5 brown carbon over Xi'an in northwestern China: Seasonal variation and source apportionment [J]. Chemosphere, 2019,237:124530.
[42] Liu B, Zhang J, Wang L, et al. Characteristics and sources of the fine carbonaceous aerosols in Haikou, China [J]. Atmospheric Research, 2018,199:103-112.
[43] Huang X, Bian Q, Louie P, et al. Contributions of vehicular carbonaceous aerosols to PM_2.5 in a roadside environment in Hong Kong [J]. Atmospheric Chemistry and Physics, 2014,14(17):9279-9293.
[44] Shen Z, Sun J, Cao J, et al. Chemical profiles of urban fugitive dust PM_2.5 samples in northern Chinese cities [J]. Science of the Total Environment, 2016,569-570:619-626.
[45] Lei Y, Shen Z, Zhang T, et al. Optical source profiles of brown carbon in size-resolved particulate matter from typical domestic biofuel burning over Guanzhong plain, China [J]. Science of the Total Environment, 2018,622-623:244-251.
[46] Zhang B, Shen Z, He K, et al. Insight into the primary and secondary particle-bound methoxyphenols and nitroaromatic compound emissions from solid fuel combustion and the updated source tracers [J]. Environmental Science & Technology, 2023,57(38):14280-14288.
[47] Verma V, Fang T, Guo H, et al. Reactive oxygen species associated with water-soluble PM_2.5in the southeastern United States: spatiotemporal trends and source apportionment [J]. Atmospheric Chemistry and Physics, 2014,14(23):12915-12930