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One-year observation of the mixing states of oxygenated organics-containing single particles in Guangzhou, China

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Abstract

Oxygenated organic molecules (OOMs) play an important role in the formation of secondary organic aerosols (SOAs), but the mixing states of OOMs are still unclear. This study investigates the mixing states of OOM-containing single particles from the measurements taken using a single particle aerosol mass spectrometer in Guangzhou, China in 2022. Generally, the particle counts of OOM particles and the mass concentration of secondary organic carbon (SOC) exhibited similar temporal trends throughout the entire year. The OOM particles were consistently enriched in secondary ions, including 16O−, 26CN−, 46NO2−, 62NO3−, and 97HSO4−. In contrast, the number fractions and diurnal patterns of OOM particles among the total detected particles showed similar distributions in August and October; however, the SOC ratios in fine particulate matter were quite different, suggesting that there were different mixing states of single-particle oxygenated organics. In addition, further classification results indicated that the OOM particles were more aged in October than August, even though the SOC ratios were higher in August. Furthermore, the distribution of hydrocarbon fragments exhibited a notable decrease from January to October, emphasizing the more aged state of the organics in October. In addition, the sharp increase in elemental carbon (EC)-OOM particles in the afternoon in October suggests the potential role of EC in the aging process of organics. Overall, in contrast to the bulk analysis of SOC mass concentration, the mixing states of the OOM particles provide insights into the formation process of SOAs in field studies.

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Data availability The observational data, including SPAMS, and the meteorological parameters obtained in this study are available from the corresponding authors upon request (chengcl@jnu.edu.cn).

References

  • Cao L M, Wei J, He L Y, Zeng H, Li M L, Zhu Q, Yu G H, Huang X F (2022). Aqueous aging of secondary organic aerosol coating onto black carbon: insights from simultaneous L-ToF-AMS and SPAMS measurements at an urban site in southern China. Journal of Cleaner Production, 330: 129888

    Article  CAS  Google Scholar 

  • Cao Y, Ma Q, Chu B, He H (2023). Homogeneous and heterogeneous photolysis of nitrate in the atmosphere: state of the science, current research needs, and future prospects. Frontiers of Environmental Science & Engineering, 17(4): 48

    Article  CAS  Google Scholar 

  • Castro L, Pio C, Harrison R M, Smith D (1999). Carbonaceous aerosol in urban and rural European atmospheres: estimation of secondary organic carbon concentrations. Atmospheric Environment, 33(17): 2771–2781

    Article  CAS  ADS  Google Scholar 

  • Chen C, Zhang Z, Wei L, Qiu Y, Xu W, Song S, Sun J, Li Z, Chen Y, Ma N, et al. (2022). The importance of hydroxymethanesulfonate (HMS) in winter haze episodes in North China Plain. Environmental Research, 211: 113093

    Article  CAS  PubMed  ADS  Google Scholar 

  • Chen Y, Cao J, Huang R, Yang F, Wang Q, Wang Y (2016). Characterization, mixing state, and evolution of urban single particles in Xi’an (China) during wintertime haze days. Science of the Total Environment, 573: 937–945

    Article  CAS  PubMed  ADS  Google Scholar 

  • Cheng C, Chan C K, Lee B P, Gen M, Li M, Yang S, Hao F, Wu C, Cheng P, Wu D, et al. (2021). Single particle diversity and mixing state of carbonaceous aerosols in Guangzhou, China. Science of the Total Environment, 754: 142182

    Article  CAS  PubMed  ADS  Google Scholar 

  • Cheng C, Li M, Chan C K, Tong H, Chen C, Chen D, Wu D, Li L, Wu C, Cheng P, et al. (2017). Mixing state of oxalic acid containing particles in the rural area of Pearl River Delta, China: implications for the formation mechanism of oxalic acid. Atmospheric Chemistry and Physics, 17(15): 9519–9533

    Article  CAS  ADS  Google Scholar 

  • Chhabra P, Ng N, Canagaratna M, Corrigan A, Russell L, Worsnop D, Flagan R, Seinfeld J (2011). Elemental composition and oxidation of chamber organic aerosol. Atmospheric Chemistry and Physics, 11(17): 8827–8845

    Article  CAS  ADS  Google Scholar 

  • Ehn M, Thornton J A, Kleist E, Sipilä M, Junninen H, Pullinen I, Springer M, Rubach F, Tillmann R, Lee B, et al. (2014). A large source of low-volatility secondary organic aerosol. Nature, 506(7489): 476–479

    Article  CAS  PubMed  ADS  Google Scholar 

  • Ervens B, Turpin B, Weber R (2011). Secondary organic aerosol formation in cloud droplets and aqueous particles (aqSOA): a review of laboratory, field and model studies. Atmospheric Chemistry and Physics, 11(21): 11069–11102

    Article  CAS  ADS  Google Scholar 

  • Feng J, Li M, Zhang P, Gong S, Zhong M, Wu M, Zheng M, Chen C, Wang H, Lou S (2013). Investigation of the sources and seasonal variations of secondary organic aerosols in PM2.5 in Shanghai with organic tracers. Atmospheric Environment, 79: 614–622

    Article  CAS  ADS  Google Scholar 

  • Gautam S, Patra A K, Kumar P (2019). Status and chemical characteristics of ambient PM2.5 pollutions in China: a review. Environment, Development and Sustainability, 21(4): 1649–1674

    Article  Google Scholar 

  • Gong H, Cheng C, Li M, Yang S, Zhou Q, Zhong Q E, Zhang Y, Xie Y, Zhou Z (2021). The enhanced mixing states of oxalate with metals in single particles in Guangzhou, China. Science of the Total Environment, 783: 146962

    Article  CAS  PubMed  ADS  Google Scholar 

  • Guo S, Hu M, Guo Q, Zhang X, Zheng M, Zheng J, Chang C C, Schauer J J, Zhang R (2012). Primary sources and secondary formation of organic aerosols in Beijing, China. Environmental Science & Technology, 46(18): 9846–9853

    Article  CAS  ADS  Google Scholar 

  • Hallquist M, Wenger J C, Baltensperger U, Rudich Y, Simpson D, Claeys M, Dommen J, Donahue N, George C, Goldstein A, et al. (2009). The formation, properties and impact of secondary organic aerosol: current and emerging issues. Atmospheric Chemistry and Physics, 9(14): 5155–5236

    Article  CAS  ADS  Google Scholar 

  • Jimenez J L, Canagaratna M, Donahue N, Prevot A, Zhang Q, Kroll J H, Decarlo P F, Allan J D, Coe H, Ng N (2009). Evolution of organic aerosols in the atmosphere. Science, 326(5959): 1525–1529

    Article  CAS  PubMed  ADS  Google Scholar 

  • Li W, Shao L, Zhang D, Ro C U, Hu M, Bi X, Geng H, Matsuki A, Niu H, Chen J (2016). A review of single aerosol particle studies in the atmosphere of East Asia: morphology, mixing state, source, and heterogeneous reactions. Journal of Cleaner Production, 112: 1330–1349

    Article  CAS  Google Scholar 

  • Li W, Teng X, Chen X, Liu L, Xu L, Zhang J, Wang Y, Zhang Y, Shi Z (2021). Organic coating reduces hygroscopic growth of phase-separated aerosol particles. Environmental Science & Technology, 55(24): 16339–16346

    Article  CAS  ADS  Google Scholar 

  • Liang C, Wang S, Hu R, Huang G, Xie J, Zhao B, Li Y, Zhu W, Guo S, Jiang J, et al. (2023). Molecular tracers, mass spectral tracers and oxidation of organic aerosols emitted from cooking and fossil fuel burning sources. Science of the Total Environment, 868: 161635

    Article  CAS  PubMed  ADS  Google Scholar 

  • Lim Y, Tan Y, Perri M, Seitzinger S, Turpin B (2010). Aqueous chemistry and its role in secondary organic aerosol (SOA) formation. Atmospheric Chemistry and Physics, 10(21): 10521–10539

    Article  CAS  ADS  Google Scholar 

  • Ling Z, Wu L, Wang Y, Shao M, Wang X, Huang W (2022). Roles of semivolatile and intermediate-volatility organic compounds in secondary organic aerosol formation and its implication: a review. Journal of Environmental Sciences-China, 114: 259–285

    Article  CAS  PubMed  Google Scholar 

  • Liu D, Whitehead J, Alfarra M R, Reyes-Villegas E, Spracklen D V, Reddington C L, Kong S, Williams P I, Ting Y C, Haslett S, et al. (2017). Black-carbon absorption enhancement in the atmosphere determined by particle mixing state. Nature Geoscience, 10(3): 184–188

    Article  ADS  Google Scholar 

  • Liu Y, Nie W, Li Y, Ge D, Liu C, Xu Z, Chen L, Wang T, Wang L, Sun P, et al. (2021). Formation of condensable organic vapors from anthropogenic and biogenic volatile organic compounds (VOCs) is strongly perturbed by NOx in eastern China. Atmospheric Chemistry and Physics, 21(19): 14789–14814

    Article  CAS  ADS  Google Scholar 

  • Liu Z, Chen H, Li L, Xie G, Ouyang H, Tang X, Ju R, Li B, Zhang R, Chen J (2022). Real-time single particle characterization of oxidized organic aerosols in the East China Sea. npj Climate and Atmospheric Science, 5(1): 47

    Article  CAS  ADS  Google Scholar 

  • Mahrt F, Peng L, Zaks J, Huang Y, Ohno P E, Smith N R, Gregson F K, Qin Y, Faiola C L, Martin S T, et al. (2022). Not all types of secondary organic aerosol mix: two phases observed when mixing different secondary organic aerosol types. Atmospheric Chemistry and Physics, 22(20): 13783–13796

    Article  CAS  ADS  Google Scholar 

  • Ng N, Canagaratna M, Jimenez J, Chhabra P, Seinfeld J, Worsnop D (2011). Changes in organic aerosol composition with aging inferred from aerosol mass spectra. Atmospheric Chemistry and Physics, 11(13): 6465–6474

    Article  CAS  ADS  Google Scholar 

  • Ng N, Canagaratna M, Zhang Q, Jimenez J, Tian J, Ulbrich I, Kroll J, Docherty K, Chhabra P, Bahreini R, et al. (2010). Organic aerosol components observed in Northern Hemispheric datasets from Aerosol Mass Spectrometry. Atmospheric Chemistry and Physics, 10(10): 4625–4641

    Article  CAS  ADS  Google Scholar 

  • Nie W, Yan C, Huang D D, Wang Z, Liu Y, Qiao X, Guo Y, Tian L, Zheng P, Xu Z, et al. (2022). Secondary organic aerosol formed by condensing anthropogenic vapours over China’s megacities. Nature Geoscience, 15(4): 255–261

    Article  CAS  ADS  Google Scholar 

  • Nozière B, Kalberer M, Claeys M, Allan J, D’Anna B, Decesari S, Finessi E, Glasius M, Grgic I, Hamilton J F, et al. (2015). The molecular identification of organic compounds in the atmosphere: state of the art and challenges. Chemical Reviews, 115(10): 3919–3983

    Article  PubMed  Google Scholar 

  • Peng J, Hu M, Guo S, Du Z, Zheng J, Shang D, Levy Zamora M, Zeng L, Shao M, Wu Y S, et al. (2016). Markedly enhanced absorption and direct radiative forcing of black carbon under polluted urban environments. Proceedings of the National Academy of Sciences of the United States of America, 113(16): 4266–4271

    Article  CAS  PubMed  PubMed Central  ADS  Google Scholar 

  • Pratt K A, Prather K A (2012). Mass spectrometry of atmospheric aerosols: recent developments and applications. Part II: On-line mass spectrometry techniques. Mass Spectrometry Reviews, 31(1): 17–48

    Article  CAS  PubMed  ADS  Google Scholar 

  • Qi L, Tian Z, Jiang N, Zheng F, Zhao Y, Geng Y, Duan X (2023). Collaborative control of fine particles and ozone required in China for health benefit. Frontiers of Environmental Science & Engineering, 17(8): 92

    Article  CAS  Google Scholar 

  • Qian Y, Cai D, Zhang M, Huang X, Huo J, Duan Y, Cheng T (2023). Chemical composition, sources and evolution of wintertime inorganic and organic aerosols in urban Shanghai, China. Frontiers in Environmental Science, 11: 1199652

    Article  Google Scholar 

  • Wang J, Ge X, Chen Y, Shen Y, Zhang Q, Sun Y, Xu J, Ge S, Yu H, Chen M (2016). Highly time-resolved urban aerosol characteristics during springtime in Yangtze River Delta, China: insights from soot particle aerosol mass spectrometry. Atmospheric Chemistry and Physics, 16(14): 9109–9127

    Article  CAS  ADS  Google Scholar 

  • Wang J, Wang J, Nie W, Chi X, Ge D, Zhu C, Wang L, Li Y, Huang X, Qi X, et al. (2023). Response of organic aerosol characteristics to emission reduction in Yangtze River Delta region. Frontiers of Environmental Science & Engineering, 17(9): 114

    Article  CAS  ADS  Google Scholar 

  • Wang Y, Huang R J, Ni H, Chen Y, Wang Q, Li G, Tie X, Shen Z, Huang Y, Liu S, et al. (2017). Chemical composition, sources and secondary processes of aerosols in Baoji City of northwest China. Atmospheric Environment, 158: 128–137

    Article  CAS  ADS  Google Scholar 

  • Wu M X, Cheng C L, Huang B, Li M, Chen D H (2020). Impact of differents in the concentrations of ozone on the chemical composition of single particles. EnvironmentalScience, 41(5): 2006–2016 (in Chinese)

    Google Scholar 

  • Xu B, Tang J, Tang T, Zhao S, Zhong G, Zhu S, Li J, Zhang G (2023). Fates of secondary organic aerosols in the atmosphere identified from compound-specific dual-carbon isotope analysis of oxalic acid. Atmospheric Chemistry and Physics, 23(2): 1565–1578

    Article  CAS  ADS  Google Scholar 

  • Yuan Q, Lai S, Song J, Ding X, Zheng L, Wang X, Zhao Y, Zheng J, Yue D, Zhong L, et al. (2018). Seasonal cycles of secondary organic aerosol tracers in rural Guangzhou, Southern China: the importance of atmospheric oxidants. Environmental Pollution, 240: 884–893

    Article  CAS  PubMed  Google Scholar 

  • Yun L, Cheng C, Yang S, Wang Z, Li M, Zhong Q E, Mao L, Liu S, Cheng X, Chen D, et al. (2024). Mixing states and secondary formation processes of organic nitrogen-containing single particles in Guangzhou, China. Journal of Environmental Sciences (China), 138: 62–73

    Article  PubMed  ADS  Google Scholar 

  • Zhai M, Kuang Y, Liu L, He Y, Luo B, Xu W, Tao J, Zou Y, Li F, Yin C, et al. (2023). Insights into characteristics and formation mechanisms of secondary organic aerosols in the Guangzhou urban area. Atmospheric Chemistry and Physics, 23(9): 5119–5133

    Article  CAS  ADS  Google Scholar 

  • Zhan B, Zhong H, Chen H, Chen Y, Li X, Wang L, Wang X, Mu Y, Huang R J, George C, et al. (2021). The roles of aqueous-phase chemistry and photochemical oxidation in oxygenated organic aerosols formation. Atmospheric Environment, 266: 118738

    Article  CAS  Google Scholar 

  • Zhang C, Lu X, Zhai J, Chen H, Yang X, Zhang Q, Zhao Q, Fu Q, Sha F, Jin J (2018a). Insights into the formation of secondary organic carbon in the summertime in urban Shanghai. Journal of Environmental Sciences (China), 72: 118–132

    Article  CAS  PubMed  Google Scholar 

  • Zhang G, Lian X, Fu Y, Lin Q, Li L, Song W, Wang Z, Tang M, Chen D, Bi X, et al. (2020). High secondary formation of nitrogen-containing organics (NOCs) and its possible link to oxidized organics and ammonium. Atmospheric Chemistry and Physics, 20(3): 1469–1481

    Article  CAS  ADS  Google Scholar 

  • Zhang G, Lin Q, Peng L, Yang Y, Fu Y, Bi X, Li M, Chen D, Chen J, Cai Z, et al. (2017). Insight into the in-cloud formation of oxalate based on in situ measurement by single particle mass spectrometry. Atmospheric Chemistry and Physics, 17(22): 13891–13901

    Article  CAS  ADS  Google Scholar 

  • Zhang Q, Jimenez J L, Canagaratna M R, Ulbrich I M, Ng N L, Worsnop D R, Sun Y (2011). Understanding atmospheric organic aerosols via factor analysis of aerosol mass spectrometry: a review. Analytical and Bioanalytical Chemistry, 401(10): 3045–3067

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  • Zhang Q, Liu J, Wei N, Song C, Peng J, Wu L, Mao H (2023). Identify the contribution of vehicle non-exhaust emissions: a single particle aerosol mass spectrometer test case at typical road environment. Frontiers of Environmental Science & Engineering, 17(5): 62

    Article  CAS  Google Scholar 

  • Zhang Q, Worsnop D, Canagaratna M, Jimenez J (2005). Hydrocarbon-like and oxygenated organic aerosols in Pittsburgh: insights into sources and processes of organic aerosols. Atmospheric Chemistry and Physics, 5(12): 3289–3311

    Article  CAS  ADS  Google Scholar 

  • Zhang R, Wang G, Guo S, Zamora M L, Ying Q, Lin Y, Wang W, Hu M, Wang Y (2015). Formation of urban fine particulate matter. Chemical Reviews, 115(10): 3803–3855

    Article  CAS  PubMed  Google Scholar 

  • Zhang Y, Li X, Li M, Zheng Y, Geng G, Hong C, Li H, Tong D, Zhang X, Cheng Y, et al. (2018b). Reduction in black carbon light absorption due to multi-pollutant emission control during APEC China 2014. Atmospheric Chemistry and Physics, 18(14): 10275–10287

    Article  CAS  ADS  Google Scholar 

  • Zhang Y, Zhang X, Zhong J, Sun J, Shen X, Zhang Z, Xu W, Wang Y, Liang L, Liu Y, et al. (2022). On the fossil and non-fossil fuel sources of carbonaceous aerosol with radiocarbon and AMS-PMF methods during winter hazy days in a rural area of North China Plain. Environmental Research, 208: 112672

    Article  CAS  PubMed  ADS  Google Scholar 

  • Zhao D, Pullinen I, Fuchs H, Schrade S, Wu R, Acir I H, Tillmann R, Rohrer F, Wildt J, Guo Y, et al. (2021). Highly oxygenated organic molecule (HOM) formation in the isoprene oxidation by NO3 radical. Atmospheric Chemistry and Physics, 21(12): 9681–9704

    Article  CAS  ADS  Google Scholar 

  • Zheng M, Zhang Y, Yan C, Zhu X, Schauer J J, Zhang Y (2014). Review of PM2.5 source apportionment methods in China. Acta Scientiarum Naturalium Universitatis Pekinensis, 50(6): 1141–1154 (in Chinese)

    Google Scholar 

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (Grant Nos. 41827804 and 41805093), the Natural Science Foundation of Guangdong Province (China) (No. 2021A1515011206), the State Key Laboratory of Marine Resource Utilization in the South China Sea, Hainan University (China) (No. MRUKF2023009), and the State Key Laboratory of Loess and Quaternary Geology, Institute of Earth Environment, CAS (No. SKLLQG2218).

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Authors and Affiliations

  1. Institute of Mass Spectrometry and Atmospheric Environment, Guangdong Provincial Engineering Research Center for the On-line Source Apportionment System of Air Pollution, Jinan University, Guangzhou, 510632, China

    Liyuan Mao, Xiaoya Cheng, Sulin Liu, Duanying Chen, Zhen Zhou, Mei Li & Chunlei Cheng

  2. Guangdong-Hongkong-Macau Joint Laboratory of Collaborative Innovation for Environmental Quality, Guangzhou, 510632, China

    Liyuan Mao, Xiaoya Cheng, Sulin Liu, Duanying Chen, Zhen Zhou, Mei Li & Chunlei Cheng

  3. Guangzhou Research Institute of Environment Protection Co., Ltd., Guangzhou, 510620, China

    Suxia Yang

  4. Guangzhou Ecological and Environmental Monitoring Center of Guangdong Province, Guangzhou, 510030, China

    Chenglei Pei

  5. State Key Laboratory of Marine Resource Utilization in South China Sea, Hainan University, Haikou, 570228, China

    Chunlei Cheng

  6. State Key Laboratory of Loess and Quaternary Geology, Institute of Earth Environment, Chinese Academy Sciences, Xi’an, 710061, China

    Chunlei Cheng

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  1. Liyuan Mao
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  2. Suxia Yang
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  3. Xiaoya Cheng
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  4. Sulin Liu
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  6. Zhen Zhou
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  7. Mei Li
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  8. Chenglei Pei
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  9. Chunlei Cheng
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Contributions

Author Contributions Liyuan Mao, Chenglei Pei, and Chunlei Cheng: Sampling, methodology, writing of original draft, and revision of the manuscript. Sulin Liu, Xiaoya Cheng, and Duanying Chen: Sampling and data analysis. Suxia Yang, Mei Li, and Zhen Zhou: Discussion and revision of the manuscript.

Corresponding authors

Correspondence to Chenglei Pei or Chunlei Cheng.

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Conflict of Interests The authors declare that the research was conducted in the absence of any commercial or financial relationships that could be construed as a potential conflict of interest

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Highlights

• The OOM particles exhibited characteristics similar to those of the SOC in summer.

• The OOM particles were enriched with secondary species.

• The organics were more oxygenated in October than in January.

• Few hydrocarbon species were found in EC-OOM particles due to photochemistry.

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Mao, L., Yang, S., Cheng, X. et al. One-year observation of the mixing states of oxygenated organics-containing single particles in Guangzhou, China. Front. Environ. Sci. Eng. 18, 64 (2024). https://doi.org/10.1007/s11783-024-1824-3

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