Articles | Volume 24, issue 19
https://doi.org/10.5194/acp-24-11029-2024
© Author(s) 2024. 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-24-11029-2024
© Author(s) 2024. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
02 Oct 2024
Research article |
| 02 Oct 2024
| 02 Oct 2024
Atmospheric evolution of environmentally persistent free radicals in the rural North China Plain: effects on water solubility and PM2.5 oxidative potential
Xu Yang
Department of Environmental Science and Engineering, School of Energy and Power Engineering, Xi'an Jiaotong University, Xi'an, Shaanxi 710049, China
Department of Environmental Science and Engineering, School of Energy and Power Engineering, Xi'an Jiaotong University, Xi'an, Shaanxi 710049, China
Shuqi Yang
Department of Environmental Science and Engineering, School of Energy and Power Engineering, Xi'an Jiaotong University, Xi'an, Shaanxi 710049, China
Yuling Yang
State Key Laboratory of Nutrient Use and Management, College of Resources and Environmental Sciences, National Academy of Agriculture Green Development, National Observation and Research Station of Agriculture Green Development (Quzhou, Hebei), China Agricultural University, Beijing 100193, China
Yanan Wang
Department of Environmental Science and Engineering, School of Energy and Power Engineering, Xi'an Jiaotong University, Xi'an, Shaanxi 710049, China
Jingjing Li
State Key Laboratory of Nutrient Use and Management, College of Resources and Environmental Sciences, National Academy of Agriculture Green Development, National Observation and Research Station of Agriculture Green Development (Quzhou, Hebei), China Agricultural University, Beijing 100193, China
Mingyu Zhao
State Key Laboratory of Nutrient Use and Management, College of Resources and Environmental Sciences, National Academy of Agriculture Green Development, National Observation and Research Station of Agriculture Green Development (Quzhou, Hebei), China Agricultural University, Beijing 100193, China
Zhao Wang
Department of Environmental Science and Engineering, School of Energy and Power Engineering, Xi'an Jiaotong University, Xi'an, Shaanxi 710049, China
Shaanxi Provincial Land Engineering Construction Group Co., Ltd., Xi'an, Shaanxi 710075, China
State Key Laboratory of Nutrient Use and Management, College of Resources and Environmental Sciences, National Academy of Agriculture Green Development, National Observation and Research Station of Agriculture Green Development (Quzhou, Hebei), China Agricultural University, Beijing 100193, China
Chi He
Department of Environmental Science and Engineering, School of Energy and Power Engineering, Xi'an Jiaotong University, Xi'an, Shaanxi 710049, China
Institute of Surface Science, Helmholtz-Zentrum Hereon, Max-Planck-Str. 1, 21502 Geesthacht, Germany
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Cited articles
Abrams, J. Y., Weber, R. J., Klein, M., Sarnat, S. E., Chang, H. H., Strickland, M. J., Verma, V., Fang, T., Bates, J. T., Mulholland, J. A., Russell, A. G., and Tolbert, P. E.: Associations between Ambient Fine Particulate Oxidative Potential and Cardiorespiratory Emergency Department Visits, Environ. Health Perspect., 125, 9, https://doi.org/10.1289/ehp3048, 2017.
Ai, J., Qin, W. H., Chen, J., Sun, Y. W., Yu, Q., Xin, K., Huang, H. Y., Zhang, L. Y., Ahmad, M., and Liu, X. A.: Pollution characteristics and light-driven evolution of environmentally persistent free radicals in PM2.5 in two typical northern cities of China, J. Hazard. Mater., 454, 131466, https://doi.org/10.1016/j.jhazmat.2023.131466, 2023.
Ainur, D., Chen, Q. C., Wang, Y. Q., Li, H., Lin, H., Ma, X. Y., and Xu, X.: Pollution characteristics and sources of environmentally persistent free radicals and oxidation potential in fine particulate matter related to city lockdown (CLD) in Xi'an, China, Environ. Res., 210, 11, https://doi.org/10.1016/j.envres.2022.112899, 2022.
Ainur, D., Chen, Q. C., Sha, T., Zarak, M., Dong, Z. P., Guo, W., Zhang, Z. M., Dina, K., and An, T. C.: Outdoor Health Risk of Atmospheric Particulate Matter at Night in Xi'an, Northwestern China, Environ. Sci. Technol., 57, 9252–9265, https://doi.org/10.1021/acs.est.3c02670, 2023.
Alleman, L. Y., Lamaison, L., Perdrix, E., Robache, A., and Galloo, J. C.: PM10 metal concentrations and source identification using positive matrix factorization and wind sectoring in a French industrial zone, Atmos. Res., 96, 612–625, https://doi.org/10.1016/j.atmosres.2010.02.008, 2010.
An, J. L., Duan, Q., Wang, H. L., Miao, Q., Shao, P., Wang, J., and Zou, J. N.: Fine particulate pollution in the Nanjing northern suburb during summer: composition and sources, Environ. Monit. Assess., 187, 561, https://doi.org/10.1007/s10661-015-4765-2, 2015.
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.
Balakrishna, S., Lomnicki, S., McAvey, K. M., Cole, R. B., Dellinger, B., and Cormier, S. A.: Environmentally persistent free radicals amplify ultrafine particle mediated cellular oxidative stress and cytotoxicity, Part. Fibre Toxicol., 6, 11, https://doi.org/10.1186/1743-8977-6-11, 2009.
Begum, B. A., Biswas, S. K., and Hopke, P. K.: Key issues in controlling air pollutants in Dhaka, Bangladesh, Atmos. Environ., 45, 7705–7713, https://doi.org/10.1016/j.atmosenv.2010.10.022, 2011.
Bhattu, D., Tripathi, S. N., Bhowmik, H. S., Moschos, V., Lee, C. P., Rauber, M., Salazar, G., Abbaszade, G., Cui, T., Slowik, J. G., Vats, P., Mishra, S., Lalchandani, V., Satish, R., Rai, P., Casotto, R., Tobler, A., Kumar, V., Hao, Y., and Qi, L.: Local incomplete combustion emissions define the PM2.5 oxidative potential in Northern India, Nat. Commun., 15, 3517, https://doi.org/10.1038/s41467-024-47785-5, 2024.
Borrowman, C. K., Zhou, S. M., Burrow, T. E., and Abbatt, J. P. D.: Formation of environmentally persistent free radicals from the heterogeneous reaction of ozone and polycyclic aromatic compounds, Phys. Chem. Chem. Phys., 18, 205–212, https://doi.org/10.1039/c5cp05606c, 2016.
Brown, S. G., Eberly, S., Paatero, P., and Norris, G. A.: Methods for estimating uncertainty in PMF solutions: Examples with ambient air and water quality data and guidance on reporting PMF results, Sci. Total Environ., 518, 626–635, https://doi.org/10.1016/j.scitotenv.2015.01.022, 2015.
Calas, A., Uzu, G., Kelly, F. J., Houdier, S., Martins, J. M. F., Thomas, F., Molton, F., Charron, A., Dunster, C., Oliete, A., Jacob, V., Besombes, J.-L., Chevrier, F., and Jaffrezo, J.-L.: Comparison between five acellular oxidative potential measurement assays performed with detailed chemistry on PM10 samples from the city of Chamonix (France), Atmos. Chem. Phys., 18, 7863–7875, https://doi.org/10.5194/acp-18-7863-2018, 2018.
Campbell, S. J., Wolfer, K., Utinger, B., Westwood, J., Zhang, Z.-H., Bukowiecki, N., Steimer, S. S., Vu, T. V., Xu, J., Straw, N., Thomson, S., Elzein, A., Sun, Y., Liu, D., Li, L., Fu, P., Lewis, A. C., Harrison, R. M., Bloss, W. J., Loh, M., Miller, M. R., Shi, Z., and Kalberer, M.: Atmospheric conditions and composition that influence PM2.5 oxidative potential in Beijing, China, Atmos. Chem. Phys., 21, 5549–5573, https://doi.org/10.5194/acp-21-5549-2021, 2021.
Cao, J. J., Wu, F., Chow, J. C., Lee, S. C., Li, Y., Chen, S. W., An, Z. S., Fung, K. K., Watson, J. G., Zhu, C. S., and Liu, S. X.: Characterization and source apportionment of atmospheric organic and elemental carbon during fall and winter of 2003 in Xi'an, China, Atmos. Chem. Phys., 5, 3127–3137, https://doi.org/10.5194/acp-5-3127-2005, 2005.
Charrier, J. G. and Anastasio, C.: Rates of Hydroxyl Radical Production from Transition Metals and Quinones in a Surrogate Lung Fluid, Environ. Sci. Technol., 49, 9317–9325, https://doi.org/10.1021/acs.est.5b01606, 2015.
Chen, Q., Sun, H., Song, W., Cao, F., Tian, C., and Zhang, Y.-L.: Size-resolved exposure risk of persistent free radicals (PFRs) in atmospheric aerosols and their potential sources, Atmos. Chem. Phys., 20, 14407–14417, https://doi.org/10.5194/acp-20-14407-2020, 2020.
Chen, Q. C., Sun, H. Y., Wang, M. M., Wang, Y. Q., Zhang, L. X., and Han, Y. M.: 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, 2019.
Chen, Q. C., Wang, M. M., Sun, H. Y., Wang, X., Wang, Y. Q., Li, Y. G., Zhang, L. X., 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., 121, 260–268, https://doi.org/10.1016/j.envint.2018.09.012, 2018a.
Chen, Q. C., Sun, H. Y., Wang, M. M., Mu, Z., Wang, Y. Q., Li, Y. G., Wang, Y. S., Zhang, L. X., and Zhang, Z. M.: 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, 2018b.
Comandini, A., Malewicki, T., and Brezinsky, K.: Chemistry of Polycyclic Aromatic Hydrocarbons Formation from Phenyl Radical Pyrolysis and Reaction of Phenyl and Acetylene, J. Phys. Chem. A, 116, 2409–2434, https://doi.org/10.1021/jp207461a, 2012.
Cormier, S. A., Lomnicki, S., Backes, W., and Dellinger, B.: Origin and health impacts of emissions of toxic by-products and fine particles from combustion and thermal treatment of hazardous wastes and materials, Environ. Health Perspect., 114, 810–817, https://doi.org/10.1289/ehp.8629, 2006.
Daellenbach, K. R., Uzu, G., Jiang, J. H., Cassagnes, L. E., Leni, Z., Vlachou, A., Stefenelli, G., Canonaco, F., Weber, S., Segers, A., Kuenen, J. J. P., Schaap, M., Favez, O., Albinet, A., Aksoyoglu, S., Dommen, J., Baltensperger, U., Geiser, M., El Haddad, I., Jaffrezo, J. L., and Prévôt, A. S. H.: Sources of particulate-matter air pollution and its oxidative potential in Europe, Nature, 587, 414–419, https://doi.org/10.1038/s41586-020-2902-8, 2020.
Dalal, N. S., Jafari, B., Petersen, M., Green, F. H. Y., and Vallyathan, V.: Presence of stable coal radicals in autopsied coal miners' lungs and its possible correlation to coal workers' pneumoconiosis, Arch. Environ. Health, 46, 366–372, https://doi.org/10.1080/00039896.1991.9934404, 1991.
Dong, Z., Wang, S. B., Sun, J. B., Shang, L. Q., Li, Z. H., and Zhang, R. Q.: Impact of COVID-19 lockdown on carbonaceous aerosols in a polluted city: Composition characterization, source apportionment, influence factors of secondary formation, Chemosphere, 307, 11, https://doi.org/10.1016/j.chemosphere.2022.136028, 2022.
Dugas, T. R., Lomnicki, S., Cormier, S. A., Dellinger, B., and Reams, M.: Addressing Emerging Risks: Scientific and Regulatory Challenges Associated with Environmentally Persistent Free Radicals, Int. J. Environ. Res. Pu., 13, 17, https://doi.org/10.3390/ijerph13060573, 2016.
Fang, T., Verma, V., Guo, H., King, L. E., Edgerton, E. S., and Weber, R. J.: 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), Atmos. Meas. Tech., 8, 471–482, https://doi.org/10.5194/amt-8-471-2015, 2015.
Fang, T., Lakey, P. S. J., Weber, R. J., and Shiraiwa, M.: Oxidative Potential of Particulate Matter and Generation of Reactive Oxygen Species in Epithelial Lining Fluid, Environ. Sci. Technol., 53, 12784–12792, https://doi.org/10.1021/acs.est.9b03823, 2019.
Fang, T., Hwang, B. C. H., Kapur, S., Hopstock, K. S., Wei, J. L., Nguyen, V., Nizkorodov, S. A., and Shiraiwa, M.: Wildfire particulate matter as a source of environmentally persistent free radicals and reactive oxygen species, Environ. Sci.-Atmospheres, 3, 581–594, https://doi.org/10.1039/d2ea00170e, 2023.
Filippi, A., Sheu, R., Berkemeier, T., Pöschl, U., Tong, H., and Gentner, D. R.: Environmentally persistent free radicals in indoor particulate matter, dust, and on surfaces, Environ. Sci.-Atmospheres, 2, 128–136, https://doi.org/10.1039/d1ea00075f, 2022.
Gao, D., Fang, T., Verma, V., Zeng, L., and Weber, R. J.: A method for measuring total aerosol oxidative potential (OP) with the dithiothreitol (DTT) assay and comparisons between an urban and roadside site of water-soluble and total OP, Atmos. Meas. Tech., 10, 2821–2835, https://doi.org/10.5194/amt-10-2821-2017, 2017.
Gao, D., Mulholland, J. A., Russell, A. G., and Weber, R. J.: Characterization of the water-insoluble oxidative potential of PM2.5 using the dithiothreitol assay, Atmos. Environ., 224, 117327, https://doi.org/10.1016/j.atmosenv.2020.117327, 2020.
Gao, J., Huang, J., Li, X., Tian, G., Wang, X., Yang, C., and Ma, C.: Challenges of the UK government and industries regarding emission control after ICE vehicle bans, Sci. Total Environ., 835, 155406, https://doi.org/10.1016/j.scitotenv.2022.155406, 2022.
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.
Gehling, W., Khachatryan, L., and Dellinger, B.: Hydroxyl Radical Generation from Environmentally Persistent Free Radicals (EPFRs) in PM2.5, Environ. Sci. Technol., 48, 4266–4272, https://doi.org/10.1021/es401770y, 2014.
Guo, H. B., Wang, Y. D., Yao, K. X., Zheng, H., Zhang, X. J., Li, R., Wang, N., and Fu, H. Y.: The overlooked formation of environmentally persistent free radicals on particulate matter collected from biomass burning under light irradiation, Environ. Int., 171, 10, https://doi.org/10.1016/j.envint.2022.107668, 2023.
Guo, X. W., Zhang, N., Hu, X., Huang, Y., Ding, Z. H., Chen, Y. J., and Lian, H. Z.: Characteristics and potential inhalation exposure risks of PM2.5-bound environmental persistent free radicals in Nanjing, a mega-city in China, Atmos. Environ., 224, 117355, https://doi.org/10.1016/j.atmosenv.2020.117355, 2020.
Heo, J. B., Dulger, M., Olson, M. R., McGinnis, J. E., Shelton, B. R., Matsunaga, A., Sioutas, C., and Schauer, J. J.: Source apportionments of PM2.5 organic carbon using molecular marker Positive Matrix Factorization and comparison of results from different receptor models, Atmos. Environ., 73, 51–61, https://doi.org/10.1016/j.atmosenv.2013.03.004, 2013.
Hwang, B., Fang, T., Pham, R., Wei, J. L., Gronstal, S., Lopez, B., Frederickson, C., Galeazzo, T., Wang, X. L., Jung, H., and Shiraiwa, M.: Environmentally Persistent Free Radicals, Reactive Oxygen Species Generation, and Oxidative Potential of Highway PM2.5, ACS Earth Space Chem., 5, 1865–1875, https://doi.org/10.1021/acsearthspacechem.1c00135, 2021.
Ikemori, F., Uranishi, K., Asakawa, D., Nakatsubo, R., Makino, M., Kido, M., Mitamura, N., Asano, K., Nonaka, S., Nishimura, R., and Sugata, S.: Source apportionment in PM2.5 in central Japan using positive matrix factorization focusing on small-scale local biomass burning, Atmos. Pollut. Res., 12, 349–359, https://doi.org/10.1016/j.apr.2021.01.006, 2021.
Jang, E., Jeong, T., Yoon, N., and Jeong, S.: Source apportionment of airborne PCDD/F at industrial and urban sites in Busan, South Korea, Chemosphere, 239, 124717, https://doi.org/10.1016/j.chemosphere.2019.124717, 2020.
Jia, H. Z., Zhao, S., Nulaji, G., Tao, K. L., Wang, F., Sharma, V. K., and Wang, C. Y.: Environmentally Persistent Free Radicals in Soils of Past Coking Sites: Distribution and Stabilization, Environ. Sci. Technol., 51, 6000–6008, https://doi.org/10.1021/acs.est.7b00599, 2017.
Jia, S.-M., Wang, D.-Q., Liu, L.-Y., Zhang, Z.-F., and Ma, W.-L.: Size-resolved environmentally persistent free radicals in cold region atmosphere: Implications for inhalation exposure risk, J. Hazard. Mater., 443, 130263, https://doi.org/10.1016/j.jhazmat.2022.130263, 2023.
Jin, L., Xie, J. W., Wong, C. K. C., Chan, S. K. Y., Abbaszade, G., Schnelle-Kreis, J., Zimmermann, R., Li, J., Zhang, G., Fu, P. Q., and Li, X. D.: Contributions of City-Specific Fine Particulate Matter (PM2.5) to Differential in Vitro Oxidative Stress and Toxicity Implications between Beijing and Guangzhou of China, Environ. Sci. Technol., 53, 2881–2891, https://doi.org/10.1021/acs.est.9b00449, 2019.
Johnson, K. S., de Foy, B., Zuberi, B., Molina, L. T., Molina, M. J., Xie, Y., Laskin, A., and Shutthanandan, V.: Aerosol composition and source apportionment in the Mexico City Metropolitan Area with PIXE/PESA/STIM and multivariate analysis, Atmos. Chem. Phys., 6, 4591–4600, https://doi.org/10.5194/acp-6-4591-2006, 2006.
Khobragade, P. P. and Ahirwar, A. V.: Source identification and ambient trace element concentrations of PM10 using receptor modeling in an urban area of Chhattisgarh, India, Geocarto Int., 37, 12267–12293, https://doi.org/10.1080/10106049.2022.2066201, 2022.
Kim, E. and Hopke, P. K.: Improving source identification of fine particles in a rural northeastern US area utilizing temperature-resolved carbon fractions, J. Geophys. Res.-Atmos., 109, 13, https://doi.org/10.1029/2003jd004199, 2004.
Kundu, S., Kawamura, K., Andreae, T. W., Hoffer, A., and Andreae, M. O.: Diurnal variation in the water-soluble inorganic ions, organic carbon and isotopic compositions of total carbon and nitrogen in biomass burning aerosols from the LBA-SMOCC campaign in Rondonia, Brazil, J. Aerosol Sci., 41, 118–133, https://doi.org/10.1016/j.jaerosci.2009.08.006, 2010.
Lei, M., Huang, X. Z., Wang, C. B., Yan, W. Q., and Wang, S. L.: Investigation on SO2, NO and NO2 release characteristics of Datong bituminous coal during pressurized oxy-fuel combustion, J. Therm. Anal. Calorim., 126, 1067–1075, https://doi.org/10.1007/s10973-016-5652-y, 2016.
Li, C., Hakkim, H., Sinha, V., Sinha, B., Pardo, M., Cai, D., Reicher, N., Chen, J., Hao, K., and Rudich, Y.: Variation of PM2.5 Redox Potential and Toxicity During Monsoon in Delhi, India, ACS ES&T Air., 1, 316–329, https://doi.org/10.1021/acsestair.3c00096, 2024.
Li, H., Chen, Q. C., Wang, C., Wang, R. H., Sha, T., Yang, X. Q., and Ainur, D.: Pollution characteristics of environmental persistent free radicals (EPFRs) and their contribution to oxidation potential in road dust in a large city in northwest China, J. Hazard. Mater., 442, 130087, https://doi.org/10.1016/j.jhazmat.2022.130087, 2023.
Li, X. Y., Kuang, X. B. M., Yan, C. Q., Ma, S. X., Paulson, S. E., Zhu, T., Zhang, Y. H., and Zheng, M.: Oxidative Potential by PM2.5 in the North China Plain: Generation of Hydroxyl Radical, Environ. Sci. Technol., 53, 512–520, https://doi.org/10.1021/acs.est.8b05253, 2019.
Liu, F. and Ng, N. L.: Toxicity of Atmospheric Aerosols: Methodologies & Assays, American Chemical Society, Washington, DC, https://doi.org/10.1021/acsinfocus.7e7012, 2023.
Liu, S. J., Huang, W. L., Yang, J. J., Xiong, Y., Huang, Z. Q., Wang, J. L., Cai, T. T., Dang, Z., and Yang, C.: Formation of environmentally persistent free radicals on microplastics under UV irradiations, J. Hazard. Mater., 453, 10, https://doi.org/10.1016/j.jhazmat.2023.131277, 2023.
Liu, S. T., Liu, G. R., Yang, L. L., Liu, X. Y., Wang, M. X., Qin, L. J., and Zheng, M. H.: Metal-Catalyzed Formation of Organic Pollutants Intermediated by Organic Free Radicals, Environ. Sci. Technol., 56, 14550–14561, https://doi.org/10.1021/acs.est.2c05892, 2022.
Liu, X. Y., Yang, L. L., Liu, G. R., and Zheng, M. H.: Formation of Environmentally Persistent Free Radicals during Thermochemical Processes and their Correlations with Unintentional Persistent Organic Pollutants, Environ. Sci. Technol., 55, 6529–6541, https://doi.org/10.1021/acs.est.0c08762, 2021.
Liu, Y., Wang, R. S., Zhao, T. N., Zhang, Y., Wang, J. H., Wu, H. X., and Hu, P.: Source apportionment and health risk due to PM10 and TSP at the surface workings of an underground coal mine in the arid desert region of northwestern China, Sci. Total Environ., 803, 149901, https://doi.org/10.1016/j.scitotenv.2021.149901, 2022.
Nagpure, A. S., Gurjar, B. R., Kumar, V., and Kumar, P.: Estimation of exhaust and non-exhaust gaseous, particulate matter and air toxics emissions from on-road vehicles in Delhi, Atmos. Environ., 127, 118–124, https://doi.org/10.1016/j.atmosenv.2015.12.026, 2016.
Ni, Z., Gao, N., Chen, N., Zhang, C., Liu, Z., Zhu, K. C., Sharma, V. K., and Jia, H. Z.: Particle-size distributions of environmentally persistent free radicals and oxidative potential of soils from a former gasworks site, Sci. Total Environ., 869, 9, https://doi.org/10.1016/j.scitotenv.2023.161747, 2023.
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 gasphase smoke and in cigarette tar, Environ. Health Perspect., 47, 345–355, https://doi.org/10.1289/ehp.8347345, 1983.
Qin, L. J., Yang, L. L., Yang, J. H., Weber, R., Ranguelova, K., Liu, X. Y., Lin, B. C., Li, C., Zheng, M. H., and Liu, G. R.: Photoinduced formation of persistent free radicals, hydrogen radicals, and hydroxyl radicals from catechol on atmospheric particulate matter, iScience, 24, 102193, https://doi.org/10.1016/j.isci.2021.102193, 2021.
Ramadan, Z., Song, X. H., and Hopke, P. K.: Identification of sources of Phoenix aerosol by positive matrix factorization, J. Air Waste Manage., 50, 1308–1320, https://doi.org/10.1080/10473289.2000.10464173, 2000.
Ramya, C. B., Aswini, A. R., Hegde, P., Boreddy, S. K. R., and Babu, S. S.: Water-soluble organic aerosols over South Asia-Seasonal changes and source characteristics, Sci. Total Environ., 900, 10, https://doi.org/10.1016/j.scitotenv.2023.165644, 2023.
Reff, A., Eberly, S. I., and Bhave, P. V.: Receptor modeling of ambient particulate matter data using positive matrix factorization: Review of existing methods, J. Air Waste Manage., 57, 146–154, https://doi.org/10.1080/10473289.2007.10465319, 2007.
Runberg, H. L., Mitchell, D. G., Eaton, S. S., Eaton, G. R., and Majestic, B. J.: Stability of environmentally persistent free radicals (EPFR) in atmospheric particulate matter and combustion particles, Atmos. Environ., 240, 117809, https://doi.org/10.1016/j.atmosenv.2020.117809, 2020.
Sarmiento, D. J. and Majestic, B. J.: Formation of Environmentally Persistent Free Radicals from the Irradiation of Polycyclic Aromatic Hydrocarbons, J. Phys. Chem. A, 127, 5390–5401, https://doi.org/10.1021/acs.jpca.3c01405, 2023.
Sharma, S. K., Mandal, T. K., Saxena, M., Sharma, R. A., Datta, A., and Saud, T.: Variation of OC, EC, WSIC and trace metals of PM10 in Delhi, India, J. Atmos. Sol.-Terr. Phy., 113, 10–22, https://doi.org/10.1016/j.jastp.2014.02.008, 2014.
Shiraiwa, M., Sosedova, Y., Rouvière, A., Yang, H., Zhang, Y. Y., Abbatt, J. P. D., Ammann, M., and Pöschl, U.: The role of long-lived reactive oxygen intermediates in the reaction of ozone with aerosol particles, Nat. Chem., 3, 291–295, https://doi.org/10.1038/nchem.988, 2011.
Son, Y., Mishin, V., Welsh, W., Lu, S. E., Laskin, J. D., Kipen, H., and Meng, Q. M.: A Novel High-Throughput Approach to Measure Hydroxyl Radicals Induced by Airborne Particulate Matter, Int. J. Environ. Res. Pu., 12, 13678–13695, https://doi.org/10.3390/ijerph121113678, 2015.
Stanimirova, I., Rich, D. Q., Russell, A. G., and Hopke, P. K.: A long-term, dispersion normalized PMF source apportionment of PM2.5 in Atlanta from 2005 to 2019, Atmos. Environ., 312, 10, https://doi.org/10.1016/j.atmosenv.2023.120027, 2023.
Tian, L. W., Koshland, C. P., Yano, J. K., Yachandra, V. K., Yu, I. T. S., Lee, S. C., and Lucas, D.: Carbon-Centered Free Radicals in Particulate Matter Emissions from Wood and Coal Combustion, Energ. Fuel., 23, 2523–2526, https://doi.org/10.1021/ef8010096, 2009.
Tong, H. J., Lakey, P. S. J., Arangio, A. M., Socorro, J., Shen, F. X., 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.
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., Fiotakis, K., Bakeas, E., and Vlahogianni, T.: Electron paramagnetic resonance study of the generation of reactive oxygen species catalysed by transition metals and quinoid redox cycling by inhalable ambient particulate matter, Redox Rep., 10, 37–51, https://doi.org/10.1179/135100005X21606, 2005.
Vejerano, E. P. and Ahn, J.: Leaves are a Source of Biogenic Persistent Free Radicals, Environ. Sci. Tech. Let., 10, 662–667, https://doi.org/10.1021/acs.estlett.3c00277, 2023.
Vejerano, E. P., Rao, G. Y., 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.
Verma, V., Rico-Martinez, R., Kotra, N., King, L., Liu, J. M., Snell, T. W., and Weber, R. J.: Contribution of Water-Soluble and Insoluble Components and Their Hydrophobic/Hydrophilic Subfractions to the Reactive Oxygen Species-Generating Potential of Fine Ambient Aerosols, Environ. Sci. Technol., 46, 11384–11392, https://doi.org/10.1021/es302484r, 2012.
Wang, C., Huang, Y. P., Zhang, Z. T., and Cai, Z. W.: Levels, spatial distribution, and source identification of airborne environmentally persistent free radicals from tree leaves, Environ. Pollut., 257, 11353, https://doi.org/10.1016/j.envpol.2019.113353, 2020.
Wang, C. A., Wang, P. Q., Zhao, L., Du, Y. B., and Che, D. F.: Experimental Study on NOx Reduction in Oxy-fuel Combustion Using Synthetic Coals with Pyridinic or Pyrrolic Nitrogen, Appl. Sci.-Basel., 8, 12, https://doi.org/10.3390/app8122499, 2018.
Wang, P., Pan, B., Li, H., Huang, Y., Dong, X. D., Ai, F., Liu, L. Y., Wu, M., and Xing, B. S.: 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, P. L., Thevenot, P., Saravia, J., Ahlert, T., and Cormier, S. A.: Radical-Containing Particles Activate Dendritic Cells and Enhance Th17 Inflammation in a Mouse Model of Asthma, Am. J. Resp. Cell Mol., 45, 977–983, https://doi.org/10.1165/rcmb.2011-0001OC, 2011.
Wang, S., Ye, J., Soong, R., Wu, B., Yu, L., Simpson, A. J., and Chan, A. W. H.: Relationship between chemical composition and oxidative potential of secondary organic aerosol from polycyclic aromatic hydrocarbons, Atmos. Chem. Phys., 18, 3987–4003, https://doi.org/10.5194/acp-18-3987-2018, 2018.
Wang, Y. D., Yao, K. X., Fu, X., Zhai, X. Y., Jin, L., and Guo, H. B.: Size-resolved exposure risk and subsequent role of environmentally persistent free radicals (EPFRs) from atmospheric particles, Atmos. Environ., 276, 9, https://doi.org/10.1016/j.atmosenv.2022.119059, 2022.
Wang, Y. Q., Li, S. P., Wang, M. M., Sun, H. Y., Mu, Z., Zhang, L. X., Li, Y. G., and Chen, Q. C.: 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.
Wang, Y. Q., Wang, M. M., Li, S. P., Sun, H. Y., Mu, Z., Zhang, L. X., Li, Y. G., and Chen, Q. C.: Study on the oxidation potential of the water-soluble components of ambient PM2.5 over Xi'an, China: Pollution levels, source apportionment and transport pathways, Environ. Int., 136, 11, https://doi.org/10.1016/j.envint.2020.105515, 2020.
Weichenthal, S., Lavigne, E., Evans, G., Pollitt, K., and Burnett, R. T.: Ambient PM2.5 and risk of emergency room visits for myocardial infarction: impact of regional PM2.5 oxidative potential: a case-crossover study, Environ. Health, 15, 9, https://doi.org/10.1186/s12940-016-0129-9, 2016.
Xu, Y., Yang, L. L., Wang, X. P., Zheng, M. H., Li, C., Zhang, A. Q., Fu, J. J., Yang, Y. P., Qin, L. J., Liu, X. Y., and Liu, G. R.: Risk evaluation of environmentally persistent free radicals in airborne particulate matter and influence of atmospheric factors, Ecotox. Environ. Safe., 196, 9, https://doi.org/10.1016/j.ecoenv.2020.110571, 2020.
Yang, L. L., Liu, G. R., Zheng, M. H., Jin, R., Zhu, Q. Q., Zhao, Y. Y., Wu, X. L., and Xu, Y.: 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.
Yang, Y., Battaglia, M. A., Mohan, M. K., Robinson, E. S., DeCarlo, P. F., Edwards, K. C., Fang, T., Kapur, S., Shiraiwa, M., Cesler-Maloney, M., Simpson, W. R., Campbell, J. R., Nenes, A., Mao, J., and Weber, R. J.: Assessing the Oxidative Potential of Outdoor PM2.5 in Wintertime Fairbanks, Alaska, ACS ES&T Air, 1, 175–187, https://doi.org/10.1021/acsestair.3c00066, 2024.
Yi, J.-F., Lin, Z.-Z., Li, X., Zhou, Y.-Q., and Guo, Y.: A short review on environmental distribution and toxicity of the environmentally persistent free radicals, Chemosphere, 340, 139922, https://doi.org/10.1016/j.chemosphere.2023.139922, 2023.
Yu, H. R., Wei, J. L., Cheng, Y. L., Subedi, K., and Verma, V.: Synergistic and Antagonistic Interactions among the Particulate Matter Components in Generating Reactive Oxygen Species Based on the Dithiothreitol Assay, Environ. Sci. Technol., 52, 2261–2270, https://doi.org/10.1021/acs.est.7b04261, 2018.
Yu, Q., Chen, J., Qin, W. H., Ahmad, M., Zhang, Y. P., Sun, Y. W., Xin, K., and Ai, J.: Oxidative potential associated with water-soluble components of PM2.5 in Beijing: The important role of anthropogenic organic aerosols, J. Hazard. Mater., 433, 12, https://doi.org/10.1016/j.jhazmat.2022.128839, 2022.
Zhang, X. J., Wang, Y. D., Yao, K. X., Zheng, H., and Guo, H. B.: Oxidative potential, environmentally persistent free radicals and reactive oxygen species of size-resolved ambient particles near highways, Environ. Pollut., 341, 122858, https://doi.org/10.1016/j.envpol.2023.122858, 2024.
Zhao, S., Miao, D., Zhu, K. C., Tao, K. L., Wang, C. Y., Sharma, V. K., and Jia, H. Z.: Interaction of benzo [a] pyrene with Cu(II)-montmorillonite: Generation and toxicity of environmentally persistent free radicals and reactive oxygen species, Environ. Int., 129, 154–163, https://doi.org/10.1016/j.envint.2019.05.037, 2019a.
Zhao, S., Gao, P., Miao, D., Wu, L., Qian, Y. J., Chen, S. P., Sharma, V. K., and Jia, H. Z.: Formation and Evolution of Solvent-Extracted and Nonextractable Environmentally Persistent Free Radicals in Fly Ash of Municipal Solid Waste Incinerators, Environ. Sci. Technol., 53, 10120–10130, https://doi.org/10.1021/acs.est.9b03453, 2019b.
Zhong, H., Huang, R.-J., Lin, C., Xu, W., Duan, J., Gu, Y., Huang, W., Ni, H., Zhu, C., You, Y., Wu, Y., Zhang, R., Ovadnevaite, J., Ceburnis, D., and O'Dowd, C. D.: Measurement report: On the contribution of long-distance transport to the secondary aerosol formation and aging, Atmos. Chem. Phys., 22, 9513–9524, https://doi.org/10.5194/acp-22-9513-2022, 2022.
Short summary
A study in the rural North China Plain showed environmentally persistent free radicals (EPFRs) in atmospheric particulate matter (PM), with a notable water-soluble fraction likely from atmospheric oxidation during transport. Significant positive correlations between EPFRs and the water-soluble oxidative potential of PM2.5 were found, primarily attributable to the water-soluble fractions of EPFRs. These findings emphasize understanding EPFRs' atmospheric evolution for climate and health impacts.
A study in the rural North China Plain showed environmentally persistent free radicals (EPFRs)...
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