Articles | Volume 20, issue 22
https://doi.org/10.5194/acp-20-14407-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-20-14407-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
27 Nov 2020
Research article |
| 27 Nov 2020
| 27 Nov 2020
Size-resolved exposure risk of persistent free radicals (PFRs) in atmospheric aerosols and their potential sources
Qingcai Chen
School of Environmental Science and Engineering, Shaanxi University of Science and Technology, Xi'an 710021, China
Haoyao Sun
School of Environmental Science and Engineering, Shaanxi University of Science and Technology, Xi'an 710021, China
Wenhuai Song
Yale – NUIST Center on Atmospheric Environment, International Joint Laboratory on Climate and Environment Change (ILCEC), Nanjing University of Information Science and Technology, Nanjing 210044, China
Fang Cao
Yale – NUIST Center on Atmospheric Environment, International Joint Laboratory on Climate and Environment Change (ILCEC), Nanjing University of Information Science and Technology, Nanjing 210044, China
Chongguo Tian
Key Laboratory of Coastal Environmental Processes and Ecological Remediation, Yantai Institute of Coastal Zone Research, Chinese Academy of Sciences, Yantai 264003, China
Yan-Lin Zhang
CORRESPONDING AUTHOR
Yale – NUIST Center on Atmospheric Environment, International Joint Laboratory on Climate and Environment Change (ILCEC), Nanjing University of Information Science and Technology, Nanjing 210044, China
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Preprint archived
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Hao-Ran Yu, Yan-Lin Zhang, Fang Cao, Xiao-Ying Yang, Tian Xie, Yu-Xian Zhang, and Yongwen Xue
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2022-239, https://doi.org/10.5194/amt-2022-239, 2022
Preprint withdrawn
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We developed a high time resolution method for determining the δ13C values of WSOCp and WSOCg by combination of wet oxidation pretreatment and IRMS. With improvement of oxidation method and determination method, δ13C value of liquid sample with a carbon content between 0.5 to 5 μg can be determined with an accuracy of 0.6 ‰. Using this method, the δ13C value of WSOCp and WSOCg in winter of 2021 at an urban site of Nanjing were determined, which were -25.9 ± 0.7 ‰ and -29.9 ± 0.9 ‰ respectively.
Hongxing Jiang, Jun Li, Jiao Tang, Min Cui, Shizhen Zhao, Yangzhi Mo, Chongguo Tian, Xiangyun Zhang, Bin Jiang, Yuhong Liao, Yingjun Chen, and Gan Zhang
Atmos. Chem. Phys., 22, 6919–6935, https://doi.org/10.5194/acp-22-6919-2022, https://doi.org/10.5194/acp-22-6919-2022, 2022
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Jiyan Wu, Chi Yang, Chunyan Zhang, Fang Cao, Aiping Wu, and Yanlin Zhang
Atmos. Meas. Tech., 15, 2623–2633, https://doi.org/10.5194/amt-15-2623-2022, https://doi.org/10.5194/amt-15-2623-2022, 2022
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We attempt to understand the current state of East Asian organic aerosols with both the molecular marker approach and 14° C data of carbonaceous components. A significant positive correlation of nonfossil- and fossil-derived organic carbon with levoglucosan suggests the importance of biomass burning (BB) and coal combustion sources in the East Asian outflow. Thus, attribution of ambient levoglucosan levels over the western North Pacific to the impact of BB emission may cause large uncertainty.
Ahsan Mozaffar, Yan-Lin Zhang, Yu-Chi Lin, Feng Xie, Mei-Yi Fan, and Fang Cao
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Dongjie Guan, Qingcai Chen, Jinwen Li, Hao Li, Lixin Zhang, Yuqin Wang, Xiaofei Li, and Tian Chang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-842, https://doi.org/10.5194/acp-2021-842, 2021
Preprint withdrawn
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The photochemical reactions of atmospheric aerosols are complicated, some reaction processes exist which have not been identified at present. This study focuses on a new mechanism of photochemical reactions, namely triplet reactions (3C*), and its potential impact on aerosol aging. This study demonstrate the coupling effect of 3C* formation between different aerosol components. The result is novel and useful in explaining how complex components affect photochemical aging of atmospheric aerosol.
Zhen Mu, Qingcai Chen, Lixin Zhang, Dongjie Guan, and Hao Li
Atmos. Chem. Phys., 21, 11581–11591, https://doi.org/10.5194/acp-21-11581-2021, https://doi.org/10.5194/acp-21-11581-2021, 2021
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Sunlight affects the life and chemical composition of atmospheric aerosols and thus alters air quality. This study demonstrated that the photo-aging process not only changed the chemical compositions of chromophoric aerosols but also changed the roles of the chromophoric organic matter in the photo-aging process of aerosol. This study adds to our understanding of how sunlight affects chromophoric aerosol aging.
Jiao Tang, Jiaqi Wang, Guangcai Zhong, Hongxing Jiang, Yangzhi Mo, Bolong Zhang, Xiaofei Geng, Yingjun Chen, Jianhui Tang, Congguo Tian, Surat Bualert, Jun Li, and Gan Zhang
Atmos. Chem. Phys., 21, 11337–11352, https://doi.org/10.5194/acp-21-11337-2021, https://doi.org/10.5194/acp-21-11337-2021, 2021
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This article provides a combined EEM–PARAFAC and statistical analysis method to explore how excitation–emission matrix (EEM) chromophores influence BrC light absorption in soluble organic matter. The application enables us to deduce that BrC absorption is mainly dependent on longer-emission-wavelength chromophores largely associated with biomass burning emissions. This method promotes the application of EEM spectroscopy and helps us understand the light absorption of BrC in the atmosphere.
Mengying Bao, Yan-Lin Zhang, Fang Cao, Yu-Chi Lin, Yuhang Wang, Xiaoyan Liu, Wenqi Zhang, Meiyi Fan, Feng Xie, Robert Cary, Joshua Dixon, and Lihua Zhou
Atmos. Meas. Tech., 14, 4053–4068, https://doi.org/10.5194/amt-14-4053-2021, https://doi.org/10.5194/amt-14-4053-2021, 2021
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We introduce a two-wavelength method for brown C measurements with a modified Sunset carbon analyzer. We defined the enhanced concentrations and gave the possibility of providing an indicator of brown C. Compared with the strong local sources of organic and elemental C, we found that differences in EC mainly originated from regional transport. Biomass burning emissions significantly contributed to high differences in EC concentrations during the heavy biomass burning periods.
Yunhua Chang, Yan-Lin Zhang, Sawaeng Kawichai, Qian Wang, Martin Van Damme, Lieven Clarisse, Tippawan Prapamontol, and Moritz F. Lehmann
Atmos. Chem. Phys., 21, 7187–7198, https://doi.org/10.5194/acp-21-7187-2021, https://doi.org/10.5194/acp-21-7187-2021, 2021
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In this study, we integrated satellite constraints on atmospheric NH3 levels and fire intensity, discrete NH3 concentration measurement, and N isotopic analysis of NH3 in order to assess the regional-scale contribution of biomass burning to ambient atmospheric NH3 in the heartland of Southeast Asia. The combined approach provides a valuable cross-validation framework for source apportioning of NH3 in the lower atmosphere and will thus help to ameliorate predictions of biomass burning emissions.
Jianzhong Sun, Yuzhe Zhang, Guorui Zhi, Regina Hitzenberger, Wenjing Jin, Yingjun Chen, Lei Wang, Chongguo Tian, Zhengying Li, Rong Chen, Wen Xiao, Yuan Cheng, Wei Yang, Liying Yao, Yang Cao, Duo Huang, Yueyuan Qiu, Jiali Xu, Xiaofei Xia, Xin Yang, Xi Zhang, Zheng Zong, Yuchun Song, and Changdong Wu
Atmos. Chem. Phys., 21, 2329–2341, https://doi.org/10.5194/acp-21-2329-2021, https://doi.org/10.5194/acp-21-2329-2021, 2021
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Brown carbon (BrC) emission factors from household biomass fuels were measured with an integrating sphere optics approach supported by iterative calculations. A novel algorithm to directly estimate the absorption contribution of BrC relative to that of BrC + black carbon (FBrC) was proposed based purely on the absorption exponent (AAE)
(FBrC = 0.5519 lnAAE + 0.0067). The FBrC for household biomass fuels was as high as 50.8 % across the strongest solar spectral range of 350−850 nm.
Cited articles
Arangio, A. M., Tong, H., Socorro, J., Pöschl, U., and Shiraiwa, M.: Quantification of environmentally persistent free radicals and reactive oxygen species in atmospheric aerosol particles, Atmos. Chem. Phys., 16, 13105–13119, https://doi.org/10.5194/acp-16-13105-2016, 2016.
Baum, S. L., Anderson, I. G. M., Baker, R. R., Murphy, D. M., and Rowlands, C. C.:
Electron spin resonance and spin trap investigation of free radicals in
cigarette smoke: development of a quantification procedure, Anal. Chim.
Acta., 481, 1–13, https://doi.org/10.1016/S0003-2670(03)00078-3, 2003.
Blakley, R. L., Henry, D. D., and Smith, C. J.: Lack of correlation between
cigarette mainstream smoke particulate phase radicals and hydroquinone
yield, Food. Chem. Toxicol., 39, 401–406, https://doi.org/10.1016/S0278-6915(00)00144-7, 2001.
Chen, N., Huang, Y., Hou, X., Ai, Z., and Zhang, L.: Photochemistry of
hydrochar: Reactive oxygen species generation and sulfadimidine degradation,
Environ. Sci. Technol., 51, 11278–11287, https://doi.org/10.1021/acs.est.7b02740, 2017.
Chen, Q., Miyazaki, Y., Kawamura, K., Matsumoto, K., Coburn, S., Volkamer,
R., Iwamoto, Y., Kagami, S., Deng, Y., and Ogawa, S.: Characterization of
chromophoric water-soluble organic matter in urban, forest, and marine
aerosols by HR-ToF-AMS analysis and excitation-emission matrix spectroscopy,
Environ. Sci. Technol., 50, 10351–10360, https://doi.org/10.1021/acs.est.6b01643, 2016.
Chen, Q., Ikemori, F., Nakamura Y., Vodicka, P., Kawamura, K., and Mochida,
M.: Structural and light-absorption characteristics of complex
water-insoluble organic mixtures in urban submicron aerosols, Environ. Sci.
Technol., 51, 8293–8303, https://doi.org/10.1021/acs.est.7b01630, 2017.
Chen, Q., Wang, M., Sun, H., Wang, X., Wang, Y., Li, Y., Zhang, L., and Mu,
Z.: Enhanced health risks from exposure to environmentally persistent free
radicals and the oxidative stress of PM2.5 from asian dust storms in
erenhot, Zhangbei and Jinan, China, Environ. Int., 123, 260–268, https://doi.org/10.1016/j.envint.2018.09.012, 2018b.
Chen, Q., Sun, H., Wang, M., Mu, Z., Wang, Y., Li, Y., Wang, Y., Zhang, L.,
and Zhang, Z.: Dominant fraction of EPFRs from Nonsolvent-Extractable
organic matter in fine particulates over Xi'an, China, Environ. Sci.
Technol., 52, 9646–9655, https://doi.org/10.1021/acs.est.8b01980, 2018a.
Chen, Q., Mu, Z., Song, W., Wang, Y., Yang, Z., Zhang, L., and Zhang, Y.:
Size-Resolved Characterization of the Chromophores in Atmospheric
Particulate Matter From a Typical Coal-Burning City in China, J. Geophys.
Res.-Atmos., 124, 10546–10563, https://doi.org/10.1029/2019JD031149, 2019a.
Chen, Q., Sun, H., Mu, Z., Wang, Y., Li, Y., Zhang, L., Wang, M., and Zhang,
Z.: Characteristics of environmentally persistent free radicals in
PM2.5: Concentrations, species and sources in Xi'an, Northwestern
China, Environ. Pollut., 247, 18–26, https://doi.org/10.1016/j.envpol.2019.01.015, 2019b.
Chen, Q., Wang, M., Wang, Y., Zhang, L., Xue, J., Sun, H., and Mu, Z.: Rapid
determination of environmentally persistent free radicals (EPFRs) in
atmospheric particles with a quartz sheet-based approach using electron
paramagnetic resonance (EPR) spectroscopy, Atmos. Environ., 184, 140–145,
https://doi.org/10.1016/j.atmosenv.2018.04.046, 2018c.
Chen, Q., Sun, H., Wang, J., Shan, M., Xue, J., Yang, X., Deng, M., Wang,
Y., and Zhang, L.: Long-life type – The dominant fraction of EPFRs in
combustion sources and ambient fine particles in Xi'an, Atmos. Environ.,
219, 117059, https://doi.org/10.1016/j.atmosenv.2019.117059,
2019c.
Chen, Q., Sun, H., Wang, M., Wang, Y., Zhang, L., and Han, Y.:
Environmentally persistent free radical (EPFR) formation by visible-light
illumination of the organic matter in atmospheric particles, Environ. Sci.
Technol., 53, 10053–10061, https://doi.org/10.1021/acs.est.9b02327, 2019d.
Chen, Q., Wang, M., Wang, Y., Zhang, L., Li, Y., and Han, Y.: Oxidative
potential of water-soluble matter associated with chromophoric substances in
PM2.5 over Xi'an, China, Environ. Sci. Technol., 53, 10053–10061,
https://doi.org/10.1021/acs.est.9b01976, 2019e.
Cheng, Y., He, K. B., Du, Z. Y., Engling, G., Liu, J. M., Ma, Y. L., Zheng,
M., and Weber, R. J.: The characteristics of brown carbon aerosol during
winter in Beijing, Atmos. Environ., 127, 355–364, https://doi.org/10.1016/j.atmosenv.2015.12.035, 2016.
Cruz, A. L. N. D., Cook, R. L., Lomnicki, S. M., and Dellinger, B.: Effect of low
temperature thermal treatment on soils contaminated with pentachlorophenol
and environmentally persistent free radicals, Environ. Sci. Technol., 46,
5971–5978, https://doi.org/10.1021/es300362k, 2012.
D'Arienzo, M., Gamba, L., Morazzoni, F., Cosention, U., Creco, C., Lasagni,
M., Pitea, D., Moro, G., Cepek, C., Butera, V., Sicilia, E., Russo, N.,
Muñoz-García, A., and Pavone, M.: Experimental and theoretical
investigation on the catalytic generation of environmentally persistent free
radicals from benzene, J. Phys. Chem. A., 121, 9381–9393, https://doi.org/10.1021/acs.jpcc.7b01449, 2017.
Dellinger, B., Pryor, W. A., Cueto, R., Squadrito, G. L., Hegde, V., and
Deutsch, W. A.: Role of free radicals in the toxicity of airborne fine
particulate matter, Chem. Res. Toxicol., 14, 1371–1377, https://doi.org/10.1021/tx010050x, 2001.
Environmental Protection Agency, Cincinnati, and OH (USA): Recommendations
for and documentation of biological values for use in risk assessment, Ntis,
PB-179874, EPA 600/6-87/008, 5195594, 1988.
Finkelstein, E., Rosen, G. M., and Rauckman, E. J.: Production of hydroxyl
radical by decomposition of superoxide spin-trapped adducts, Mol.
Pharmacol., 21, 262–265, 1982.
Gehling, W. and Dellinger, B.: Environmentally persistent free radicals and
their lifetimes in PM2.5, Environ. Sci. Technol., 47, 8172–8178,
https://doi.org/10.1021/es401767m, 2013.
Han, Y., Chen, Y. J., Saud, A., Feng, Y. L., Zhang, F., Song, W. H., Cao,
F., Zhang, Y., Yang, X., Li, J., and Zhang, G.: High time- and size-resolved
measurements of PM and chemical composition from coal combustion:
Implications for the EC formation process, Environ. Sci. Technol., 52,
6676–6685, https://doi.org/10.1021/acs.est.7b05786, 2018.
Harmon, A. C., Hebert, V. Y., Cormier, S. A., Subramanian, B., Reed, J. R.,
Backes, W. L., and Dugas, T. R.: Particulate matter containing
environmentally persistent free radicals induces AhRdependent cytokine and
reactive oxygen species production in human bronchial epithelial cells,
Plos One, 13, e0205412, https://doi.org/10.1371/journal.pone.0205412, 2018.
Karnae, S. and John, K.: Source apportionment of fine particulate matter
measured in an industrialized coastal urban area of South Texas, Atmos.
Environ., 45, 3769–3776, https://doi.org/10.1016/j.atmosenv.2011.04.040, 2011.
Keiluweit, M., Nico, P. S., Johnson, M. G., and Kleber, M.: Dynamic
molecular structure of plant biomass-derived black carbon (biochar),
Environ. Sci. Technol., 44, 1247–1253, https://doi.org/10.1021/es9031419, 2010.
Khachatryan, L. and Dellinger, B.: Environmentally persistent free radicals
(EPFRs)-2. Are free hydroxyl radicals generated in aqueous solutions?,
Environ. Sci. Technol., 45, 9232–9239, https://doi.org/10.1021/es201702q, 2011.
Li, G. L., Wu, S. Y., Kuang, M. Q., Hu, X. F., and Xu, Y. Q.: Studies on the
g-factors of the copper(II)-oxygen compounds, J. Struct. Chem., 58,
700–705, https://doi.org/10.1134/S0022476617040084, 2017.
Lin, P., Hu, M., Deng, Z., Slanina, J., Han, S., Kondo, Y., Takegawa, N.,
Miyazaki, Y., Zhao, Y., and Sugimoto, N.: Seasonal and diurnal variations of
organic carbon in PM2.5 in Beijing and the estimation of secondary
organic carbon, J. Geophys. Res.-Atmos., 114, 1–41, https://doi.org/10.1029/2008JD010902, 2009.
Liu, J., Bergin, M., Guo, H., King, L., Kotra, N., Edgerton, E., and Weber, R. J.: Size-resolved measurements of brown carbon in water and methanol extracts and estimates of their contribution to ambient fine-particle light absorption, Atmos. Chem. Phys., 13, 12389–12404, https://doi.org/10.5194/acp-13-12389-2013, 2013.
Lyons, M. J. and Spence, J. B.: Environmental free radicals, Br. J. Canc.,
14, 703–708, https://doi.org/10.1038/bjc.1960.79, 1960.
Lyu, L., Yu, G., Zhang, L., Hu, C., and Sun, Y.:
4-Phenoxyphenolfunctionalized reduced graphene oxide nanosheets: A
metal-free fenton-like catalyst for pollutant destruction, Environ. Sci.
Technol., 52, 747–756, https://doi.org/10.1021/acs.est.7b04865, 2018.
Mihara, T. and Michihiro, M.: Characterization of solvent-extractable
organics in urban aerosols based on mass spectrum analysis and hygroscopic
growth measurement, Environ. Sci. Technol., 45, 9168–9174, https://doi.org/10.1021/es201271w, 2011.
Mukome, F. N. D., Zhang, X., Silva, L. C. R., Six, J., and Parikh, S. J.:
Use of Chemical and physical characteristics to investigate trends in
biochar feedstocks, J. Agric. Food Chem., 61, 2196–2204, https://doi.org/10.1021/jf3049142, 2013.
Nikitenko, V. A.: Luminescence and EPR of zinc oxide (review), J. Appl.
Spectrosc., 57, 783–798, https://doi.org/10.1007/BF00663923, 1992.
Oyana, T. J., Lomnicki, S. M., Guo, C., and Cormier, S. A.: A scalable field
study protocol and rationale for passive ambient air sampling: a spatial
phytosampling for leaf data collection, Environ. Sci. Technol., 51,
10663–10673, https://doi.org/10.1021/acs.est.7b03643, 2017.
Pan, Y., Wang, Y., Sun, Y., Tian, S., and Cheng, M.: Size-resolved aerosol
trace elements at a rural mountainous site in Northern China: importance of
regional transport, Sci. Total Environ., 461–462, 761–771, https://doi.org/10.1016/j.scitotenv.2013.04.065, 2013.
Patterson, M. C., Keilbart, N. D., Kiruri, L. W., Thibodeaux, C. A.,
Lomnicki, S., Kurtz, R. L., Poliakoff, E. D., Dellinger, B., and Sprunger,
P. T.: EPFR formation from phenol adsorption on Al2O3 and
TiO2: EPR and EELS studies, Chem. Phys., 422, 277–282, https://doi.org/10.1016/j.chemphys.2012.12.003, 2013.
Pryor, W. A.: Oxy-Radicals and Related Species: Their Formation, Lifetimes,
and Reactions, Annu. Rev. Physiol., 48, 657–667, https://doi.org/10.1146/annurev.ph.48.030186.003301, 1986.
Pryor, W. A., Prier, D. G., and Church, D. F.: Electron-spin resonance study of
mainstream and sidestream cigarette smoke: nature of the free radicals in
gas-phase smoke and in cigarette tar, Environ. Health Perspect., 47,
345–355, https://doi.org/10.1289/ehp.8347345, 1983.
Qi, L., Zhang, Y., Ma, Y., Chen, M., Ge, X., Ma, Y., Zheng, J., Wang, Z.,
and Li, S.: Source identification of trace elements in the atmosphere during
the second Asian Youth Games in Nanjing, China: Influence of control
measures on air quality, Atmos. Pollut. Res., 7, 547–556, https://doi.org/10.1016/j.apr.2016.01.003, 2016.
Salma, I., Balásházy, I., Winkler-Heil, R., Hofmann, W., and
Záray, G.: Effect of particle mass size distribution on the deposition
of aerosols in the human respiratory tract, J. Aerosol. Sci., 33,
119–132, https://doi.org/10.1016/S0021-8502(01)00154-9, 2002.
Seabra, A. B., Paula, A. J., Lima, R. D., Alves, O. L., and Durán, N.:
Nanotoxicity of graphene and graphene oxide, Chem. Res. Toxicol., 27,
159–168, https://doi.org/10.1021/tx400385x, 2014.
Shaltout, A. A., Boman, J., Shehadeh, Z. F., Al-Malawi, D. A. R., Hemeda, O.
M., and Morsy, M. M.: Spectroscopic investigation of PM2.5, collected
at industrial, residential and traffic sites in taif, Saudi Arabia, J.
Aerosol. Sci., 79, 97–108, https://doi.org/10.1016/j.jaerosci.2014.09.004, 2015.
Song, W., Cao, F., Lin, Y., Haque, M. M., Wu, X., Zhang, Y., Zhang, C., Xie,
F., and Zhang, Y.: Extremely high abundance of polycyclic aromatic
hydrocarbons in aerosols from a typical coal-combustion rural site in China:
Size distribution, source identification and cancer risk assessment, Atmos.
Res., 248, 105192, https://doi.org/10.1016/j.atmosres.2020.105192, 2020.
Srivastava, A. and Jain, V. K.: Size distribution and source identification
of total suspended particulate matter and associated heavy metals in the
urban atmosphere of Delhi, Chemosphere, 68, 579–589, https://doi.org/10.1016/j.chemosphere.2006.12.046, 2007.
Strak, M., Janssen, N. A. H., Godri, K. J., Gosens, I., Mudway, I. S.,
Cassee, F. R., Lebret, E., Kelly F. J., Harrison, R. M., Brunekreef, B.,
Steenhof, M., and Hoek, G.: Respiratory health effects of airborne
particulate matter: The role of particle size, composition, and oxidative
potential-the RAPTES project, Eviron. Health. Persp., 120, 1183–1189,
https://doi.org/10.1289/ehp.1104389, 2012.
Thevenot, P. T., Saravia, J., Jin, N., Giaimo, J. D., Chustz, R. E., Mahne,
S., Kelley, M. A., Hebert, V. Y., Dellinger, B., Dugas, T. R., Demayo, F.
G., and Cormier, S. A.: Radical-containing ultrafine particulate matter
initiates epithelial-to-mesenchymal transitions in airway epithelial cells,
Am. J. Respir. Cell. Mol. Biol., 48, 188–197, https://doi.org/10.1165/rcmb.2012-0052OC, 2013.
Tian, H. Z., Wang, Y., Xue, Z. G., Cheng, K., Qu, Y. P., Chai, F. H., and Hao, J. M.: Trend and characteristics of atmospheric emissions of Hg, As, and Se from coal combustion in China, 1980–2007, Atmos. Chem. Phys., 10, 11905–11919, https://doi.org/10.5194/acp-10-11905-2010, 2010.
Tong, H., Lakey, P. S. J., Arangio, A. M., Socorro, J., Shen, F., Lucas, K.,
Brune, W. H., Pöschl, U., and Shiraiwa, M.: Reactive
oxygen species formed by secondary organic aerosols in water and surrogate
lung fluid, Environ. Sci. Technol., 52, 11642–11651, https://doi.org/10.1021/acs.est.8b03695, 2018.
Trapp, J. M., Millero, F. J., and Prospero, J. M.: Temporal variability of
the elemental composition of African dust measured in trade wind aerosols at
Barbados and Miami, Mar. Chem., 120, 71–82, https://doi.org/10.1016/j.marchem.2008.10.004, 2010.
Truong, H., Lomnicki, S., and Dellinger, B.: Potential for misidentification
of environmentally persistent free radicals as molecular pollutants in
particulate matter, Environ. Sci. Technol., 44, 1933–1939, https://doi.org/10.1021/es902648t, 2010.
Valavanidis, A. and Haralambous, E.: A comparative study by electron
paramagnetic resonance of free radical species in the mainstream and
sidestream smoke of cigarettes with conventional acetate filters and
bio-filters, Redox. Rep., 6, 161–171, https://doi.org/10.1179/135100001101536274, 2001.
Valavanidis, A., Fiotakis, K., and Vlachogianni, T.: Airborne particulate
matterand human health: toxicological assessment and importance of size and
composition of particles for oxidative damage and carcinogenic mechanisms,
J. Environ. Sci. Heal. C., 26, 339–362, https://doi.org/10.1080/10590500802494538, 2008.
Vejerano, E., Lomnicki, S., and Dellinger, B.: Formation and stabilization
of combustion-generated environmentally persistent free radicals on an
Fe(III)2O3/silica surface, Environ. Sci. Technol., 45,
589–594, https://doi.org/10.1021/es102841s, 2011.
Vejerano, E., Lomnicki, S. M., and Dellinger, B.: Formation and
stabilization of combustion-generated, environmentally persistent radicals
on Ni(II)O supported on a silica surface, Environ. Sci. Technol., 46,
9406–9411, https://doi.org/10.1021/es301136d, 2012a.
Vejerano, E., Lomnicki, S., and Dellinger, B.: Lifetime of
combustion-generated environmentally persistent free radicals on Zn(II)O and
other transition metal oxides, J. Environ. Monit., 14, 2803–2806,
https://doi.org/10.1039/c2em30545c, 2012b.
Vejerano, E. P., Rao, G., Khachatryan, L., Cormier, S. A., and Lomnicki, S.:
Environmentally persistent free radicals: Insights on a new class of
pollutants, Environ. Sci. Technol., 52, 2468–2481, https://doi.org/10.1021/acs.est.7b04439, 2018.
Wang, P., Pan, B., Li, H., Huang, Y., Dong, X., Fang, A., Liu, L., Wu, M.,
and Xing, B.: The overlooked occurrence of environmentally persistent free
radicals in an area with low-rank coal burning, Xuanwei, China, Environ.
Sci. Technol., 52, 1054–1061, https://doi.org/10.1021/acs.est.7b05453, 2018.
Wang, Y., Li, S., Wang, M., Sun, H., Mu, Z., Zhang, L., Li, Y., and Chen,
Q.: Source apportionment of environmentally persistent free radicals (EPFRs)
in PM2.5 over Xi'an, China, Sci. Total. Environ., 689, 193–202,
https://doi.org/10.1016/j.scitotenv.2019.06.424, 2019.
Yang, L., Liu, G., Zheng, M., Jin, R., Zhu, Q, Zhao, Y., Wu, X., and Yang,
X.: Highly elevated levels and particle-size distributions of
environmentally persistent free radicals in haze-associated atmosphere,
Environ. Sci. Technol., 51, 7936–7944, https://doi.org/10.1021/acs.est.7b01929, 2017.
Yu, T., Wang, J., Shen, M., and Li, W.: NH3-SCR over Cu/SAPO-34
catalysts with various acid contents and low Cu loading, Catal. Sci.
Technol., 3, 3234–3241, https://doi.org/10.1039/c3cy00453h, 2017.
Short summary
This study found environmentally persistent free radicals (EPFRs) are widely present in atmospheric particles of different particle sizes and exhibit significant particle size distribution characteristics. EPFR concentrations are higher in coarse particles than in fine particles in summer and vice versa in winter. The potential toxicity caused by EPFRs may also vary with particle size and season. Combustion is the most important source of EPFRs (>70 %).
This study found environmentally persistent free radicals (EPFRs) are widely present in...
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