Articles | Volume 24, issue 14
https://doi.org/10.5194/acp-24-8397-2024
© 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-24-8397-2024
© Author(s) 2024. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
26 Jul 2024
Research article |
| 26 Jul 2024
| 26 Jul 2024
Critical contribution of chemically diverse carbonyl molecules to the oxidative potential of atmospheric aerosols
Feifei Li
State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China
College of Resources and Environment, University of Chinese Academy of Sciences, Beijing 100049, China
Shanshan Tang
Hangzhou International Innovation Institute, Beihang University, Hangzhou 311115, China
Jitao Lv
CORRESPONDING AUTHOR
State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China
College of Resources and Environment, University of Chinese Academy of Sciences, Beijing 100049, China
Shiyang Yu
State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China
College of Resources and Environment, University of Chinese Academy of Sciences, Beijing 100049, China
Xu Sun
State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China
Beijing Urban Ecosystem Research Station, State Key Laboratory of Urban and Regional Ecology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China
Dong Cao
State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China
Yawei Wang
CORRESPONDING AUTHOR
State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China
College of Resources and Environment, University of Chinese Academy of Sciences, Beijing 100049, China
School of Environment, Hangzhou Institute for Advanced Study, University of Chinese Academy of Sciences, Hangzhou 310024, China
Hubei Key Laboratory of Environmental and Health Effects of Persistent Toxic Substances, Institute of Environment and Health, Jianghan University, Wuhan 430056, China
Guibin Jiang
State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China
College of Resources and Environment, University of Chinese Academy of Sciences, Beijing 100049, China
School of Environment, Hangzhou Institute for Advanced Study, University of Chinese Academy of Sciences, Hangzhou 310024, China
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Cited articles
Baluha, D. R., Blough, N. V., and Del Vecchio, R.: Selective Mass Labeling for Linking the Optical Properties of Chromophoric Dissolved Organic Matter to Structure and Composition via Ultrahigh Resolution Electrospray Ionization Mass Spectrometry, Environ. Sci. Technol., 47, 9891–9897, https://doi.org/10.1021/es402400j, 2013.
Bates, J. T., Fang, T., Verma, V., Zeng, L., Weber, R. J., Tolbert, P. E., Abrams, J. Y., Sarnat, S. E., Klein, M., Mulholland, J. A., and Russell, A. G.: Review of Acellular Assays of Ambient Particulate Matter Oxidative Potential: Methods and Relationships with Composition, Sources, and Health Effects, Environ. Sci. Technol., 53, 4003–4019, https://doi.org/10.1021/acs.est.8b03430, 2019.
Bianco, A., Deguillaume, L., Vaïtilingom, M., Nicol, E., Baray, J.-L., Chaumerliac, N., and Bridoux, M.: Molecular Characterization of Cloud Water Samples Collected at the Puy de Dôme (France) by Fourier Transform Ion Cyclotron Resonance Mass Spectrometry, Environ. Sci. Technol., 52, 10275–10285, https://doi.org/10.1021/acs.est.8b01964, 2018.
Bora, S. and Shankarrao Adole, P.: Carbonyl stress in diabetics with acute coronary syndrome, Clin. Chim. Acta, 520, 78–86, https://doi.org/10.1016/j.cca.2021.06.002, 2021.
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.
Chen, J. Y., Jiang, H., Chen, S. J., Cullen, C., Ahmed, C. M. S., and Lin, Y.-H.: Characterization of electrophilicity and oxidative potential of atmospheric carbonyls, Environ. Sci.-Proc. Imp., 21, 856–866, https://doi.org/10.1039/C9EM00033J, 2019.
Chen, K., Raeofy, N., Lum, M., Mayorga, R., Woods, M., Bahreini, R., Zhang, H., and Lin, Y.-H.: Solvent effects on chemical composition and optical properties of extracted secondary brown carbon constituents, Aerosol Sci. Tech., 56, 917–930, https://doi.org/10.1080/02786826.2022.2100734, 2022.
Chen, K., Mayorga, R., Hamilton, C., Bahreini, R., Zhang, H., and Lin, Y.-H.: Contribution of Carbonyl Chromophores in Secondary Brown Carbon from Nighttime Oxidation of Unsaturated Heterocyclic Volatile Organic Compounds, Environ. Sci. Technol., 57, 20085–20096, https://doi.org/10.1021/acs.est.3c08872, 2023.
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, 8574–8584, https://doi.org/10.1021/acs.est.9b01976, 2019.
Claeys, M., Graham, B., Vas, G., Wang, W., Vermeylen, R., Pashynska, V., Cafmeyer, J., Guyon, P., Andreae, M. O., Artaxo, P., and Maenhaut, W.: Formation of Secondary Organic Aerosols Through Photooxidation of Isoprene, Science, 303, 1173–1176, https://doi.org/10.1126/science.1092805, 2004.
Daellenbach, K. R., Uzu, G., Jiang, J., 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.
Dou, J., Lin, P., Kuang, B.-Y., and Yu, J. Z.: Reactive Oxygen Species Production Mediated by Humic-like Substances in Atmospheric Aerosols: Enhancement Effects by Pyridine, Imidazole, and Their Derivatives, Environ. Sci. Technol., 49, 6457–6465, https://doi.org/10.1021/es5059378, 2015.
Du, H., Li, J., Wang, Z., Chen, X., Yang, W., Sun, Y., Xin, J., Pan, X., Wang, W., Ye, Q., and Dao, X.: Assessment of the effect of meteorological and emission variations on winter PM2.5 over the North China Plain in the three-year action plan against air pollution in 2018–2020, Atmos. Res., 280, 106395, https://doi.org/10.1016/j.atmosres.2022.106395, 2022.
Fu, T.-M., Jacob, D. J., Wittrock, F., Burrows, J. P., Vrekoussis, M., and Henze, D. K.: Global budgets of atmospheric glyoxal and methylglyoxal, and implications for formation of secondary organic aerosols, J. Geophys. Res.-Atmos., 113, D15303, https://doi.org/10.1029/2007JD009505, 2008.
Graber, E. R. and Rudich, Y.: Atmospheric HULIS: How humic-like are they? A comprehensive and critical review, Atmos. Chem. Phys., 6, 729–753, https://doi.org/10.5194/acp-6-729-2006, 2006.
Grosjean, D., Grosjean, E., and Gertler, A. W.: On-Road Emissions of Carbonyls from Light-Duty and Heavy-Duty Vehicles, Environ. Sci. Technol., 35, 45–53, https://doi.org/10.1021/es001326a, 2001.
Han, J., Wang, S., Yeung, K., Yang, D., Gu, W., Ma, Z., Sun, J., Wang, X., Chow, C.-W., Chan, A. W. H., and Peng, H.: Proteome-wide effects of naphthalene-derived secondary organic aerosol in BEAS-2B cells are caused by short-lived unsaturated carbonyls, P. Natl. Acad. Sci. USA, 117, 25386–25395, https://doi.org/10.1073/pnas.2001378117, 2020.
Havers, N., Burba, P., Lambert, J., and Klockow, D.: Spectroscopic Characterization of Humic-Like Substances in Airborne Particulate Matter, J. Atmos. Chem., 29, 45–54, https://doi.org/10.1023/A:1005875225800, 1998.
He, L. and Zhang, J. (Jim): Particulate matter (PM) oxidative potential: Measurement methods and links to PM physicochemical characteristics and health effects, Critical Reviews in Environmental Science and Technology, 9, 822–828, https://doi.org/10.1080/10643389.2022.2050148, 2022.
Ho, S. S. H. and Yu, J. Z.: Determination of Airborne Carbonyls: Comparison of a Thermal Desorption/GC Method with the Standard DNPH/HPLC Method, Environ. Sci. Technol., 38, 862–870, https://doi.org/10.1021/es034795w, 2004.
Huang, R.-J., Yang, L., Cao, J., Chen, Y., Chen, Q., Li, Y., Duan, J., Zhu, C., Dai, W., Wang, K., Lin, C., Ni, H., Corbin, J. C., Wu, Y., Zhang, R., Tie, X., Hoffmann, T., O'Dowd, C., and Dusek, U.: Brown Carbon Aerosol in Urban Xi'an, Northwest China: The Composition and Light Absorption Properties, Environ. Sci. Technol., 52, 6825–6833, https://doi.org/10.1021/acs.est.8b02386, 2018.
Huang, R.-J., Yang, L., Shen, J., Yuan, W., Gong, Y., Guo, J., Cao, W., Duan, J., Ni, H., Zhu, C., Dai, W., Li, Y., Chen, Y., Chen, Q., Wu, Y., Zhang, R., Dusek, U., O'Dowd, C., and Hoffmann, T.: Water-Insoluble Organics Dominate Brown Carbon in Wintertime Urban Aerosol of China: Chemical Characteristics and Optical Properties, Environ. Sci. Technol., 54, 7836–7847, https://doi.org/10.1021/acs.est.0c01149, 2020.
Huo, Y., Guo, Z., Li, Q., Wu, D., Ding, X., Liu, A., Huang, D., Qiu, G., Wu, M., Zhao, Z., Sun, H., Song, W., Li, X., Chen, Y., Wu, T., and Chen, J.: Chemical Fingerprinting of HULIS in Particulate Matters Emitted from Residential Coal and Biomass Combustion, Environ. Sci. Technol., 55, 3593–3603, https://doi.org/10.1021/acs.est.0c08518, 2021.
Ji, Y., Shi, Q., Li, Y., An, T., Zheng, J., Peng, J., Gao, Y., Chen, J., Li, G., Wang, Y., Zhang, F., Zhang, A. L., Zhao, J., Molina, M. J., and Zhang, R.: Carbenium ion-mediated oligomerization of methylglyoxal for secondary organic aerosol formation, P. Natl. Acad. Sci. USA, 117, 13294–13299, https://doi.org/10.1073/pnas.1912235117, 2020.
Jiang, H. and Jang, M.: Dynamic Oxidative Potential of Atmospheric Organic Aerosol under Ambient Sunlight, Environ. Sci. Technol., 52, 7496–7504, https://doi.org/10.1021/acs.est.8b00148, 2018.
Jiang, H., Li, J., Sun, R., Tian, C., Tang, J., Jiang, B., Liao, Y., Chen, C.-E., and Zhang, G.: Molecular Dynamics and Light Absorption Properties of Atmospheric Dissolved Organic Matter, Environ. Sci. Technol., 55, 10268–10279, https://doi.org/10.1021/acs.est.1c01770, 2021.
Jiang, H., Li, J., Tang, J., Cui, M., Zhao, S., Mo, Y., Tian, C., Zhang, X., Jiang, B., Liao, Y., Chen, Y., and Zhang, G.: Molecular characteristics, sources, and formation pathways of organosulfur compounds in ambient aerosol in Guangzhou, South China, Atmos. Chem. Phys., 22, 6919–6935, https://doi.org/10.5194/acp-22-6919-2022, 2022.
Kalberer, M., Paulsen, D., Sax, M., Steinbacher, M., Dommen, J., Prevot, A. S. H., Fisseha, R., Weingartner, E., Frankevich, V., Zenobi, R., and Baltensperger, U.: Identification of Polymers as Major Components of Atmospheric Organic Aerosols, Science, 303, 1659–1662, https://doi.org/10.1126/science.1092185, 2004.
Kenseth, C. M., Hafeman, N. J., Rezgui, S. P., Chen, J., Huang, Y., Dalleska, N. F., Kjaergaard, H. G., Stoltz, B. M., Seinfeld, J. H., and Wennberg, P. O.: Particle-phase accretion forms dimer esters in pinene secondary organic aerosol, Science, 382, 787–792, https://doi.org/10.1126/science.adi0857, 2023.
Kroll, J. H., Donahue, N. M., Jimenez, J. L., Kessler, S. H., Canagaratna, M. R., Wilson, K. R., Altieri, K. E., Mazzoleni, L. R., Wozniak, A. S., Bluhm, H., Mysak, E. R., Smith, J. D., Kolb, C. E., and Worsnop, D. R.: Carbon oxidation state as a metric for describing the chemistry of atmospheric organic aerosol, Nat. Chem., 3, 133–139, https://doi.org/10.1038/nchem.948, 2011.
Kumagai, Y., Koide, S., Taguchi, K., Endo, A., Nakai, Y., Yoshikawa, T., and Shimojo, N.: Oxidation of Proximal Protein Sulfhydryls by Phenanthraquinone, a Component of Diesel Exhaust Particles, Chem. Res. Toxicol., 15, 483–489, https://doi.org/10.1021/tx0100993, 2002.
Lary, D. J. and Shallcross, D. E.: Central role of carbonyl compounds in atmospheric chemistry, J. Geophys. Res.-Atmos., 105, 19771–19778, https://doi.org/10.1029/1999JD901184, 2000.
Li, F., Tang, S., Lv, J., He, A., Wang, Y., Liu, S., Cao, H., Zhao, L., Wang, Y., and Jiang, G.: Molecular-Scale Investigation on the Formation of Brown Carbon Aerosol via Iron-Phenolic Compound Reactions in the Dark, Environ. Sci. Technol., 57, 11173–11184, https://doi.org/10.1021/acs.est.3c04263, 2023.
Li, M., Yang, D., Brock, G., Knipp, R. J., Bousamra, M., Nantz, M. H., and Fu, X.-A.: Breath carbonyl compounds as biomarkers of lung cancer, Lung Cancer, 90, 92–97, https://doi.org/10.1016/j.lungcan.2015.07.005, 2015.
Li, Y., Lei, L., Sun, J., Gao, Y., Wang, P., Wang, S., Zhang, Z., Du, A., Li, Z., Wang, Z., Kim, J. Y., Kim, H., Zhang, H., and Sun, Y.: Significant Reductions in Secondary Aerosols after the Three-Year Action Plan in Beijing Summer, Environ. Sci. Technol., 57, 15945–15955, https://doi.org/10.1021/acs.est.3c02417, 2023.
Lin, M. and Yu, J. Z.: Assessment of Interactions between Transition Metals and Atmospheric Organics: Ascorbic Acid Depletion and Hydroxyl Radical Formation in Organic-Metal Mixtures, Environ. Sci. Technol., 54, 1431–1442, https://doi.org/10.1021/acs.est.9b07478, 2020.
Lin, P. and Yu, J. Z.: Generation of Reactive Oxygen Species Mediated by Humic-like Substances in Atmospheric Aerosols, Environ. Sci. Technol., 45, 10362–10368, https://doi.org/10.1021/es2028229, 2011.
Liu, F., Joo, T., Ditto, J. C., Saavedra, M. G., Takeuchi, M., Boris, A. J., Yang, Y., Weber, R. J., Dillner, A. M., Gentner, D. R., and Ng, N. L.: Oxidized and Unsaturated: Key Organic Aerosol Traits Associated with Cellular Reactive Oxygen Species Production in the Southeastern United States, Environ. Sci. Technol., 57, 14150–14161, https://doi.org/10.1021/acs.est.3c03641, 2023.
Liu, Q., Gao, Y., Huang, W., Ling, Z., Wang, Z., and Wang, X.: Carbonyl compounds in the atmosphere: A review of abundance, source and their contributions to O3 and SOA formation, Atmos. Res., 274, 106184, https://doi.org/10.1016/j.atmosres.2022.106184, 2022.
Liu, W., Xu, Y., Liu, W., Liu, Q., Yu, S., Liu, Y., Wang, X., and Tao, S.: Oxidative potential of ambient PM2.5 in the coastal cities of the Bohai Sea, northern China: Seasonal variation and source apportionment, Environ. Pollut., 236, 514–528, https://doi.org/10.1016/j.envpol.2018.01.116, 2018.
Liu, X., Liu, R., Zhu, B., Ruan, T., and Jiang, G.: Characterization of Carbonyl Disinfection By-Products During Ozonation, Chlorination, and Chloramination of Dissolved Organic Matters, Environ. Sci. Technol., 54, 2218–2227, https://doi.org/10.1021/acs.est.9b04875, 2020.
Liu, Y., Xu, X., Yang, X., He, J., Ji, D., and Wang, Y.: Significant Reduction in Fine Particulate Matter in Beijing during 2022 Beijing Winter Olympics, Environ. Sci. Tech. Let., 53, 177–197, https://doi.org/10.1021/acs.estlett.2c00532, 2022.
Lv, J., Zhang, S., Wang, S., Luo, L., Cao, D., and Christie, P.: Molecular-Scale Investigation with ESI-FT-ICR-MS on Fractionation of Dissolved Organic Matter Induced by Adsorption on Iron Oxyhydroxides, Environ. Sci. Technol., 50, 2328–2336, https://doi.org/10.1021/acs.est.5b04996, 2016.
Lyu, Y., Guo, H., Cheng, T., and Li, X.: Particle Size Distributions of Oxidative Potential of Lung-Deposited Particles: Assessing Contributions from Quinones and Water-Soluble Metals, Environ. Sci. Technol., 52, 6592–6600, https://doi.org/10.1021/acs.est.7b06686, 2018.
Ma, J., Del Vecchio, R., Golanoski, K. S., Boyle, E. S., and Blough, N. V.: Optical Properties of Humic Substances and CDOM: Effects of Borohydride Reduction, Environ. Sci. Technol., 44, 5395–5402, https://doi.org/10.1021/es100880q, 2010.
Ma, J., Ungeheuer, F., Zheng, F., Du, W., Wang, Y., Cai, J., Zhou, Y., Yan, C., Liu, Y., Kulmala, M., Daellenbach, K. R., and Vogel, A. L.: Nontarget Screening Exhibits a Seasonal Cycle of PM2.5 Organic Aerosol Composition in Beijing, Environ. Sci. Technol., 56, 7017–7028, https://doi.org/10.1021/acs.est.1c06905, 2022.
Ma, Y., Cheng, Y., Qiu, X., Cao, G., Fang, Y., Wang, J., Zhu, T., Yu, J., and Hu, D.: Sources and oxidative potential of water-soluble humic-like substances (HULISWS) in fine particulate matter (PM2.5) in Beijing, Atmos. Chem. Phys., 18, 5607–5617, https://doi.org/10.5194/acp-18-5607-2018, 2018.
Nguyen, T. B., Roach, P. J., Laskin, J., Laskin, A., and Nizkorodov, S. A.: Effect of humidity on the composition of isoprene photooxidation secondary organic aerosol, Atmos. Chem. Phys., 11, 6931–6944, https://doi.org/10.5194/acp-11-6931-2011, 2011.
Papazian, S., D'Agostino, L. A., Sadiktsis, I., Froment, J., Bonnefille, B., Sdougkou, K., Xie, H., Athanassiadis, I., Budhavant, K., Dasari, S., Andersson, A., Gustafsson, Ö., and Martin, J. W.: Nontarget mass spectrometry and in silico molecular characterization of air pollution from the Indian subcontinent, Commun. Earth Environ., 3, 35, https://doi.org/10.1038/s43247-022-00365-1, 2022.
Phillips, S. M. and Smith, G. D.: Light Absorption by Charge Transfer Complexes in Brown Carbon Aerosols, Environ. Sci. Tech. Let., 1, 382–386, https://doi.org/10.1021/ez500263j, 2014.
Phillips, S. M. and Smith, G. D.: Further Evidence for Charge Transfer Complexes in Brown Carbon Aerosols from Excitation–Emission Matrix Fluorescence Spectroscopy, J. Phys. Chem. A, 119, 4545–4551, https://doi.org/10.1021/jp510709e, 2015.
Powelson, M. H., Espelien, B. M., Hawkins, L. N., Galloway, M. M., and De Haan, D. O.: Brown Carbon Formation by Aqueous-Phase Carbonyl Compound Reactions with Amines and Ammonium Sulfate, Environ. Sci. Technol., 48, 985–993, https://doi.org/10.1021/es4038325, 2014.
Qian, X., Shen, H., and Chen, Z.: Characterizing summer and winter carbonyl compounds in Beijing atmosphere, Atmos. Environ., 214, 116845, https://doi.org/10.1016/j.atmosenv.2019.116845, 2019.
Rappaport, S. M., Li, H., Grigoryan, H., Funk, W. E., and Williams, E. R.: Adductomics: Characterizing exposures to reactive electrophiles, Toxicol. Lett., 213, 83–90, https://doi.org/10.1016/j.toxlet.2011.04.002, 2012.
Shen, H., Chen, Z., Li, H., Qian, X., Qin, X., and Shi, W.: Gas-Particle Partitioning of Carbonyl Compounds in the Ambient Atmosphere, Environ. Sci. Technol., 52, 10997–11006, https://doi.org/10.1021/acs.est.8b01882, 2018.
Song, J., Li, M., Fan, X., Zou, C., Zhu, M., Jiang, B., Yu, Z., Jia, W., Liao, Y., and Peng, P.: 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, Environ. Sci. Technol., 53, 13607–13617, https://doi.org/10.1021/acs.est.9b04331, 2019.
Song, J., Li, M., Zou, C., Cao, T., Fan, X., Jiang, B., Yu, Z., Jia, W., and Peng, P.: Molecular Characterization of Nitrogen-Containing Compounds in Humic-like Substances Emitted from Biomass Burning and Coal Combustion, Environ. Sci. Technol., 56, 119–130, https://doi.org/10.1021/acs.est.1c04451, 2022.
Steimer, S. S., Patton, D. J., Vu, T. V., Panagi, M., Monks, P. S., Harrison, R. M., Fleming, Z. L., Shi, Z., and Kalberer, M.: Differences in the composition of organic aerosols between winter and summer in Beijing: a study by direct-infusion ultrahigh-resolution mass spectrometry, Atmos. Chem. Phys., 20, 13303–13318, https://doi.org/10.5194/acp-20-13303-2020, 2020.
Su, S., Xie, Q., Lang, Y., Cao, D., Xu, Y., Chen, J., Chen, S., Hu, W., Qi, Y., Pan, X., Sun, Y., Wang, Z., Liu, C.-Q., Jiang, G., and Fu, P.: High Molecular Diversity of Organic Nitrogen in Urban Snow in North China, Environ. Sci. Technol., 55, 4344–4356, https://doi.org/10.1021/acs.est.0c06851, 2021.
Tang, S., Li, F., Lv, J., Liu, L., Wu, G., Wang, Y., Yu, W., Wang, Y., and Jiang, G.: Unexpected molecular diversity of brown carbon formed by Maillard-like reactions in aqueous aerosols, Chem. Sci., 13, 8401–8411, https://doi.org/10.1039/D2SC02857C, 2022.
Tuet, W. Y., Chen, Y., Xu, L., Fok, S., Gao, D., Weber, R. J., and Ng, N. L.: Chemical oxidative potential of secondary organic aerosol (SOA) generated from the photooxidation of biogenic and anthropogenic volatile organic compounds, Atmos. Chem. Phys., 17, 839–853, https://doi.org/10.5194/acp-17-839-2017, 2017.
Verma, V., Rico-Martinez, R., Kotra, N., King, L., Liu, J., 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, J., Lin, X., Lu, L., Wu, Y., Zhang, H., Lv, Q., Liu, W., Zhang, Y., and Zhuang, S.: Temporal variation of oxidative potential of water soluble components of ambient PM2.5 measured by dithiothreitol (DTT) assay, Sci. Total Environ., 649, 969–978, https://doi.org/10.1016/j.scitotenv.2018.08.375, 2019.
Wang, L., Lin, Y., Ye, L., Qian, Y., Shi, Y., Xu, K., Ren, H., and Geng, J.: Microbial Roles in Dissolved Organic Matter Transformation in Full-Scale Wastewater Treatment Processes Revealed by Reactomics and Comparative Genomics, Environ. Sci. Technol., 55, 11294–11307, https://doi.org/10.1021/acs.est.1c02584, 2021.
Wang, L., Wen, W., Yan, J., Zhang, R., Li, C., Jiang, H., Chen, S., Pardo, M., Zhu, K., Jia, B., Zhang, W., Bai, Z., Shi, L., Cheng, Y., Rudich, Y., Morawska, L., and Chen, J.: Influence of Polycyclic Aromatic Compounds and Oxidation States of Soot Organics on the Metabolome of Human-Lung Cells (A549): Implications for Vehicle Fuel Selection, Environ. Sci. Technol., 57, 21593–21604, https://doi.org/10.1021/acs.est.3c05228, 2023.
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, Z., Chen, X., Liang, Y., and Shi, Q.: Molecular characterization of carbonyl compounds in atmospheric fine particulate matters (PM2.5) in Beijing by derivatization with Girard's reagent T combined with positive-ion ESI Orbitrap MS, Atmos. Res., 273, 106176, https://doi.org/10.1016/j.atmosres.2022.106176, 2022.
Xie, Q., Su, S., Dai, Y., Hu, W., Yue, S., Cao, D., Jiang, G., and Fu, P.: Deciphering 13C and 34S Isotopes of Organosulfates in Urban Aerosols by FT-ICR Mass Spectrometry, Environ. Sci. Tech. Let., 9, 526–532, https://doi.org/10.1021/acs.estlett.2c00255, 2022.
Xu, Y., Feng, X., Chen, Y., Zheng, P., Hui, L., Chen, Y., Yu, J. Z., and Wang, Z.: Development of an enhanced method for atmospheric carbonyls and characterizing their roles in photochemistry in subtropical Hong Kong, Sci. Total Environ., 896, 165135, https://doi.org/10.1016/j.scitotenv.2023.165135, 2023.
Yang, L., Huang, R.-J., Shen, J., Wang, T., Gong, Y., Yuan, W., Liu, Y., Huang, H., You, Q., Huang, D. D., and Huang, C.: New Insights into the Brown Carbon Chromophores and Formation Pathways for Aqueous Reactions of α-Dicarbonyls with Amines and Ammonium, Environ. Sci. Technol., 57, 12351–12361, https://doi.org/10.1021/acs.est.3c04133, 2023.
Ye, C., Liu, Y., Yuan, B., Wang, Z., Lin, Y., Hu, W., Chen, W., Li, T., Song, W., Wang, X., Lv, D., Gu, D., and Shao, M.: Low-NO-like Oxidation Pathway Makes a Significant Contribution to Secondary Organic Aerosol in Polluted Urban Air, Environ. Sci. Technol., 57, 13912–13924, https://doi.org/10.1021/acs.est.3c01055, 2023.
Yu, Q., Chen, J., Qin, W., Ahmad, M., Zhang, Y., Sun, Y., 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, 128839, https://doi.org/10.1016/j.jhazmat.2022.128839, 2022.
Yu, S., Tang, S., Lv, J., Li, F., Huang, Z., Zhao, L., Cao, D., and Wang, Y.: High throughput identification of carbonyl compounds in natural organic matter by directional derivatization combined with ultra-high resolution mass spectrometry, Water Res., 258, 121769, https://doi.org/10.1016/j.watres.2024.121769, 2024.
Yu, W., Shen, X., Wu, B., Kong, L., Xuan, K., Zhao, C., Cao, X., Hao, X., Li, X., Zhang, H., and Yao, Z.: Real-world emission characteristics of carbonyl compounds from agricultural machines based on a portable emission measurement system, J. Environ. Sci., 124, 846–859, https://doi.org/10.1016/j.jes.2022.02.031, 2023.
Yue, S., Zhu, J., Chen, S., Xie, Q., Li, W., Li, L., Ren, H., Su, S., Li, P., Ma, H., Fan, Y., Cheng, B., Wu, L., Deng, J., Hu, W., Ren, L., Wei, L., Zhao, W., Tian, Y., Pan, X., Sun, Y., Wang, Z., Wu, F., Liu, C.-Q., Su, H., Penner, J. E., Pöschl, U., Andreae, M. O., Cheng, Y., and Fu, P.: Brown carbon from biomass burning imposes strong circum-Arctic warming, One Earth, 5, 293–304, https://doi.org/10.1016/j.oneear.2022.02.006, 2022.
Zeng, Y., Shen, Z., Takahama, S., Zhang, L., Zhang, T., Lei, Y., Zhang, Q., Xu, H., Ning, Y., Huang, Y., Cao, J., and Rudolf, H.: Molecular Absorption and Evolution Mechanisms of PM2.5 Brown Carbon Revealed by Electrospray Ionization Fourier Transform–Ion Cyclotron Resonance Mass Spectrometry During a Severe Winter Pollution Episode in Xi'an, China, Geophys. Res. Lett., 47, e2020GL087977, https://doi.org/10.1029/2020GL087977, 2020.
Zhang, Q., Ma, H., Li, J., Jiang, H., Chen, W., Wan, C., Jiang, B., Dong, G., Zeng, X., Chen, D., Lu, S., You, J., Yu, Z., Wang, X., and Zhang, G.: Nitroaromatic Compounds from Secondary Nitrate Formation and Biomass Burning Are Major Proinflammatory Components in Organic Aerosols in Guangzhou: A Bioassay Combining High-Resolution Mass Spectrometry Analysis, Environ. Sci. Technol., 57, 21570–21580, https://doi.org/10.1021/acs.est.3c04983, 2023.
Short summary
Targeted derivatization and non-targeted analysis with Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) were used to reveal the molecular composition of carbonyl molecules in PM2.5, and the important role of carbonyls in increasing the oxidative potential of organic aerosol was found in real samples.
Targeted derivatization and non-targeted analysis with Fourier transform ion cyclotron resonance...
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