Articles | Volume 23, issue 2
https://doi.org/10.5194/acp-23-1565-2023
© Author(s) 2023. 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-23-1565-2023
© Author(s) 2023. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Fates of secondary organic aerosols in the atmosphere identified from compound-specific dual-carbon isotope analysis of oxalic acid
Buqing Xu
State Key Laboratory of Organic Geochemistry, Guangzhou Institute of
Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, China
CAS Center for Excellence in Deep Earth Science, Guangzhou 510640,
China
Jiao Tang
State Key Laboratory of Organic Geochemistry, Guangzhou Institute of
Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, China
CAS Center for Excellence in Deep Earth Science, Guangzhou 510640,
China
Tiangang Tang
State Key Laboratory of Organic Geochemistry, Guangzhou Institute of
Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, China
Key Laboratory of Agro-ecological Processes in Subtropical Region,
Institute of Subtropical Agriculture, Chinese Academy of Sciences, Changsha,
410125, China
Shizhen Zhao
State Key Laboratory of Organic Geochemistry, Guangzhou Institute of
Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, China
CAS Center for Excellence in Deep Earth Science, Guangzhou 510640,
China
Guangcai Zhong
State Key Laboratory of Organic Geochemistry, Guangzhou Institute of
Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, China
CAS Center for Excellence in Deep Earth Science, Guangzhou 510640,
China
Sanyuan Zhu
State Key Laboratory of Organic Geochemistry, Guangzhou Institute of
Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, China
CAS Center for Excellence in Deep Earth Science, Guangzhou 510640,
China
State Key Laboratory of Organic Geochemistry, Guangzhou Institute of
Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, China
CAS Center for Excellence in Deep Earth Science, Guangzhou 510640,
China
Gan Zhang
CORRESPONDING AUTHOR
State Key Laboratory of Organic Geochemistry, Guangzhou Institute of
Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, China
CAS Center for Excellence in Deep Earth Science, Guangzhou 510640,
China
Related authors
No articles found.
Pingyang Li, Boji Lin, Zhineng Cheng, Jing Li, Jun Li, Duohong Chen, Tao Zhang, Run Lin, Sanyuan Zhu, Jun Liu, Yujun Lin, Shizhen Zhao, Guangcai Zhong, Zhenchuan Niu, Ping Ding, and Gan Zhang
EGUsphere, https://doi.org/10.5194/egusphere-2025-1931, https://doi.org/10.5194/egusphere-2025-1931, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
Short summary
Short summary
Our study indicates fossil fuel CO2 (CO2ff) reductions in Chinese megacities via atmospheric Δ(14CO2) and δ(13CO2) measurements, driven by coal-to-gas transitions and combustion efficiency improvement. Three-decade data show steeper declined urban RCO/CO2ff ratios than inventory estimates, implying underestimation of efficiency improvements and CO reductions. Integrating top-down observations with inventories is critical to track policy-driven emission shifts and optimize co-benefit strategies.
Yuying Wu, Yuhan Wang, Wenzheng Yang, Jie Zhang, Yanhong Wu, Jun Li, Gan Zhang, and Haijian Bing
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2025-302, https://doi.org/10.5194/essd-2025-302, 2025
Revised manuscript under review for ESSD
Short summary
Short summary
We developed a large, open-access dataset of mountain soil chemistry in China, based on over 1,300 samples from 166 sites across diverse climates and vegetation types. The dataset includes concentrations of 24 elements and key environmental variables like temperature, rainfall, and soil properties. This dataset offers a valuable resource for studying mountain ecosystems, supporting Earth system modeling, and predicting how soils respond to environmental change.
Tao Cao, Cuncun Xu, Hao Chen, Jianzhong Song, Jun Li, Haiyan Song, Bin Jiang, Yin Zhong, and Ping’an Peng
EGUsphere, https://doi.org/10.5194/egusphere-2025-561, https://doi.org/10.5194/egusphere-2025-561, 2025
Short summary
Short summary
This study investigated the evolution of biomass and coal combustion-derived WSOM during aqueous photochemical process. The results indicate that photochemical aging induces distinct changes in the optical and molecular properties of WSOM and more pronounced alterations were observed during ·OH photooxidation than direct photolysis. Notably, our results also demostrated that atmospheric photooxidation may represent a significant source of BC-like substances.
Yangzhi Mo, Jun Li, Guangcai Zhong, Sanyuan Zhu, Shizhen Zhao, Jiao Tang, Hongxing Jiang, Zhineng Cheng, Chongguo Tian, Yingjun Chen, and Gan Zhang
Atmos. Chem. Phys., 24, 7755–7772, https://doi.org/10.5194/acp-24-7755-2024, https://doi.org/10.5194/acp-24-7755-2024, 2024
Short summary
Short summary
In this study, we found that biomass burning (31.0 %) and coal combustion (31.1 %) were the dominant sources of water-insoluble organic carbon in China, with coal combustion sources exhibiting the strongest light-absorbing capacity. Additionally, we propose a light-absorbing carbonaceous continuum, revealing that components enriched with fossil sources tend to have stronger light-absorbing capacity, higher aromaticity, higher molecular weights, and greater recalcitrance in the atmosphere.
Wenwen Ma, Rong Sun, Xiaoping Wang, Zheng Zong, Shizhen Zhao, Zeyu Sun, Chongguo Tian, Jianhui Tang, Song Cui, Jun Li, and Gan Zhang
Atmos. Chem. Phys., 24, 1509–1523, https://doi.org/10.5194/acp-24-1509-2024, https://doi.org/10.5194/acp-24-1509-2024, 2024
Short summary
Short summary
This is the first report of long-term atmospheric PAH monitoring around the Bohai Sea. The results showed that the concentrations of PAHs in the atmosphere around the Bohai Sea decreased from June 2014 to May 2019, especially the concentrations of highly toxic PAHs. This indicates that the contributions from PAH sources changed to a certain extent in different areas, and it also led to reductions in the related health risk and medical costs following pollution prevention and control.
Zeyu Sun, Zheng Zong, Yang Tan, Chongguo Tian, Zeyu Liu, Fan Zhang, Rong Sun, Yingjun Chen, Jun Li, and Gan Zhang
Atmos. Chem. Phys., 23, 12851–12865, https://doi.org/10.5194/acp-23-12851-2023, https://doi.org/10.5194/acp-23-12851-2023, 2023
Short summary
Short summary
This is the first report of ship-emitted nitrogen stable isotope composition (δ15N) of nitrogen oxides (NOx). The results showed that δ15N–NOx from ships was −18.5 ± 10.9 ‰ and increased monotonically with tightening emission regulations. The selective catalytic reduction system was the most vital factor. The temporal variation in δ15N–NOx was evaluated and can be used to select suitable δ15N–NOx for a more accurate assessment of the contribution of ship-emitted exhaust to atmospheric NOx.
Xiangyun Zhang, Jun Li, Sanyuan Zhu, Junwen Liu, Ping Ding, Shutao Gao, Chongguo Tian, Yingjun Chen, Ping'an Peng, and Gan Zhang
Atmos. Chem. Phys., 23, 7495–7502, https://doi.org/10.5194/acp-23-7495-2023, https://doi.org/10.5194/acp-23-7495-2023, 2023
Short summary
Short summary
The results show that 14C elemental carbon (EC) was not only related to the isolation method but also to the types and proportions of the biomass sources in the sample. The hydropyrolysis (Hypy) method, which can be used to isolate a highly stable portion of ECHypy and avoid charring, is a more effective and stable approach for the matrix-independent 14C quantification of EC in aerosols, and the 13C–ECHypy and non-fossil ECHypy values of SRM1649b were –24.9 ‰ and 11 %, respectively.
Tingting Li, Jun Li, Zeyu Sun, Hongxing Jiang, Chongguo Tian, and Gan Zhang
Atmos. Chem. Phys., 23, 6395–6407, https://doi.org/10.5194/acp-23-6395-2023, https://doi.org/10.5194/acp-23-6395-2023, 2023
Short summary
Short summary
N-NH4+ and N-NO3- were vital components in nitrogenous aerosols and contributed 69 % to total nitrogen in PM2.5. Coal combustion was still the most important source of urban atmospheric NO3-. However, the non-agriculture sources play an increasingly important role in NH4+ emissions.
Jiao Tang, Jun Li, Shizhen Zhao, Guangcai Zhong, Yangzhi Mo, Hongxing Jiang, Bin Jiang, Yingjun Chen, Jianhui Tang, Chongguo Tian, Zheng Zong, Jabir Hussain Syed, Jianzhong Song, and Gan Zhang
EGUsphere, https://doi.org/10.5194/egusphere-2023-403, https://doi.org/10.5194/egusphere-2023-403, 2023
Preprint archived
Short summary
Short summary
This study provides a comprehensive molecular identification of atmospheric common fluorescent components and deciphers their related formation pathways. The fluorescent components varied in molecular composition, and a dominant oxidation pathway for the formation of humic-like fluorescent components was suggested, notwithstanding their different precursor types. Our findings are expected to be helpful to further studies using the EEM-PARAFAC as a tool to study atmospheric BrC.
Tao Cao, Meiju Li, Cuncun Xu, Jianzhong Song, Xingjun Fan, Jun Li, Wanglu Jia, and Ping'an Peng
Atmos. Chem. Phys., 23, 2613–2625, https://doi.org/10.5194/acp-23-2613-2023, https://doi.org/10.5194/acp-23-2613-2023, 2023
Short summary
Short summary
This work comprehensively investigated the fluorescence data of light-absorbing organic compounds, water-soluble organic matter in different types of aerosol samples, soil dust, and fulvic and humic acids using an excitation–emission matrix (EEM) method and parallel factor modeling. The results revealed which light-absorbing species can be detected by EEM and also provided important information for identifying the chemical composition and possible sources of these species in atmospheric samples.
Chunlin Zou, Tao Cao, Meiju Li, Jianzhong Song, Bin Jiang, Wanglu Jia, Jun Li, Xiang Ding, Zhiqiang Yu, Gan Zhang, and Ping'an Peng
Atmos. Chem. Phys., 23, 963–979, https://doi.org/10.5194/acp-23-963-2023, https://doi.org/10.5194/acp-23-963-2023, 2023
Short summary
Short summary
In this study, PM2.5 samples were obtained during a winter haze event in Guangzhou, China, and light absorption and molecular composition of humic-like substances (HULIS) were investigated by UV–Vis spectrophotometry and ultrahigh-resolution mass spectrometry. The findings obtained present some differences from the results reported in other regions of China and significantly enhanced our understanding of HULIS evolution during haze bloom-decay processes in the subtropic region of southern China.
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
Short summary
Short summary
We conducted field observation employing Fourier transform ion cyclotron resonance mass spectrometry to characterize the molecular composition and major formation pathways or sources of organosulfur compounds in Guangzhou, where is heavily influenced by biogenic–anthropogenic interactions and has high relative humidity and temperature. We suggested that heterogeneous reactions such as SO2 uptake and heterogeneous oxidations are important to the molecular variations of organosulfur compounds.
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
Short summary
Short summary
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.
Xuewu Fu, Chen Liu, Hui Zhang, Yue Xu, Hui Zhang, Jun Li, Xiaopu Lyu, Gan Zhang, Hai Guo, Xun Wang, Leiming Zhang, and Xinbin Feng
Atmos. Chem. Phys., 21, 6721–6734, https://doi.org/10.5194/acp-21-6721-2021, https://doi.org/10.5194/acp-21-6721-2021, 2021
Short summary
Short summary
TGM concentrations and isotopic compositions in 10 Chinese cities showed strong seasonality with higher TGM concentrations and Δ199Hg and lower δ202Hg in summer. We found the seasonal variations in TGM concentrations and isotopic compositions were highly related to regional surface Hg(0) emissions, suggesting land surface Hg(0) emissions are an important source of atmospheric TGM that contribute dominantly to the seasonal variations in TGM concentrations and isotopic compositions.
Cited articles
Aggarwal, S. G. and Kawamura, K.: Molecular distributions and stable carbon
isotopic compositions of dicarboxylic acids and related compounds in
aerosols from Sapporo, Japan: Implications for photochemical aging during
long-range atmospheric transport, J. Geophys. Res.-Atmos., 113, D14301,
https://doi.org/10.1029/2007jd009365, 2008.
Anderson, R. S., Huang, L., Iannone, R., Thompson, A. E., and Rudolph, J.:
Carbon Kinetic Isotope Effects in the Gas Phase Reactions of Light Alkanes
and Ethene with the OH Radical at 296 ± 4 K, J. Phys. Chem. A, 108,
11537–11544, https://doi.org/10.1021/jp0472008, 2004.
Andersson, A., Deng, J., Du, K., Zheng, M., Yan, C., Skold, M., and
Gustafsson, O.: Regionally-varying combustion sources of the January 2013
severe haze events over eastern China, Environ. Sci. Technol., 49,
2038–2043, https://doi.org/10.1021/es503855e, 2015.
Bikkina, S., Kawamura, K., Miyazaki, Y., and Fu, P.: High abundances of
oxalic, azelaic, and glyoxylic acids and methylglyoxal in the open ocean
with high biological activity: Implication for secondary OA formation from
isoprene, Geophys. Res. Lett., 41, 3649–3657, https://doi.org/10.1002/2014gl059913, 2014.
Bikkina, S., Kawamura, K., and Sarin, M.: Secondary organic aerosol
formation over coastal ocean: inferences from atmospheric water-soluble low
molecular weight organic compounds, Environ. Sci. Technol., 51, 4347–4357,
https://doi.org/10.1021/acs.est.6b05986, 2017a.
Bikkina, S., Andersson, A., Ram, K., Sarin, M. M., Sheesley, R. J.,
Kirillova, E. N., Rengarajan, R., Sudheer, A. K., and Gustafsson, Ö.:
Carbon isotope-constrained seasonality of carbonaceous aerosol sources from
an urban location (Kanpur) in the Indo-Gangetic Plain, J. Geophys. Res.-Atmos., 122, 4903–4923, https://doi.org/10.1002/2016jd025634, 2017b.
Bikkina, S., Kawamura, K., Sakamoto, Y., and Hirokawa, J.: Low molecular
weight dicarboxylic acids, oxocarboxylic acids and α-dicarbonyls as
ozonolysis products of isoprene: Implication for the gaseous-phase formation
of secondary organic aerosols, Sci. Total Environ., 769, 144472,
https://doi.org/10.1016/j.scitotenv.2020.144472, 2021.
Boreddy, S. K. R. and Kawamura, K.: Investigation on the hygroscopicity of
oxalic acid and atmospherically relevant oxalate salts under sub- and
supersaturated conditions, Environ. Sci.-Proc. Imp., 20, 1069–1080,
https://doi.org/10.1039/c8em00053k, 2018.
Bosch, C., Andersson, A., Kirillova, E. N., Budhavant, K., Tiwari, S.,
Praveen, P. S., Russell, L. M., Beres, N. D., Ramanathan, V., and
Gustafsson, Ö.: Source-diagnostic dual-isotope composition and optical
properties of water-soluble organic carbon and elemental carbon in the South
Asian outflow intercepted over the Indian Ocean, J. Geophys. Res.-Atmos.,
119, 11743–11759, https://doi.org/10.1002/2014jd022127, 2014.
Cao, J.-J., Chow, J. C., Tao, J., Lee, S.-C., Watson, J. G., Ho, K.-F.,
Wang, G.-H., Zhu, C.-S., and Han, Y.-M.: Stable carbon isotopes in aerosols
from Chinese cities: Influence of fossil fuels, Atmos. Environ., 45,
1359–1363, https://doi.org/10.1016/j.atmosenv.2010.10.056, 2011.
Carlton, A. G., Turpin, B. J., Altieri, K. E., Seitzinger, S., Reff, A.,
Lim, H.-J., and Ervens, B.: Atmospheric oxalic acid and SOA production from
glyoxal: Results of aqueous photooxidation experiments, Atmos. Environ., 41,
7588–7602, https://doi.org/10.1016/j.atmosenv.2007.05.035, 2007.
Carlton, A. G., Wiedinmyer, C., and Kroll, J. H.: A review of Secondary Organic Aerosol (SOA) formation from isoprene, Atmos. Chem. Phys., 9, 4987–5005, https://doi.org/10.5194/acp-9-4987-2009, 2009.
Chang, X., Zhao, B., Zheng, H., Wang, S., Cai, S., Guo, F., Gui, P., Huang,
G., Wu, D., Han, L., Xing, J., Man, H., Hu, R., Liang, C., Xu, Q., Qiu, X.,
Ding, D., Liu, K., Han, R., Robinson, A. L., and Donahue, N. M.:
Full-volatility emission framework corrects missing and underestimated
secondary organic aerosol sources, One Earth, 5, 403–412,
https://doi.org/10.1016/j.oneear.2022.03.015, 2022.
Chen, Y., Guo, H., Nah, T., Tanner, D. J., Sullivan, A. P., Takeuchi, M.,
Gao, Z., Vasilakos, P., Russell, A. G., Baumann, K., Huey, L. G., Weber, R.
J., and Ng, N. L.: Low-Molecular-Weight Carboxylic Acids in the Southeastern
U.S.: Formation, Partitioning, and Implications for Organic Aerosol Aging,
Environ. Sci. Technol., 55, 6688–6699, https://doi.org/10.1021/acs.est.1c01413, 2021.
Dasari, S., Andersson, A., Bikkina, S., Holmstrand, H., Budhavant, K.,
Satheesh, S., Asmi, E., Kesti, J., Backman, J., Salam, A., Bisht, D. S.,
Tiwari, S., Hameed, Z., and Gustafsson, Ö.: Photochemical degradation
affects the light absorption of water-soluble brown carbon in the South
Asian outflow, Sci. Adv., 5, eaau8066, https://doi.org/10.1126/sciadv.aau8066, 2019.
Elmquist, M., Cornelissen, G., Kukulska, Z., and Gustafsson, O.: Distinct
oxidative stabilities of char versus soot black carbon: Implications for
quantification and environmental recalcitrance, Global Biogeochem. Cy.,
20, GB2009, https://doi.org/10.1029/2005gb002629, 2006.
Ervens, B., Turpin, B. J., and Weber, R. J.: Secondary organic aerosol formation in cloud droplets and aqueous particles (aqSOA): a review of laboratory, field and model studies, Atmos. Chem. Phys., 11, 11069–11102, https://doi.org/10.5194/acp-11-11069-2011, 2011.
Fang, W., Du, K., Andersson, A., Xing, Z., Cho, C., Kim, S.-W., Deng, J.,
and Gustafsson, Ö.: Dual-Isotope Constraints on Seasonally Resolved
Source Fingerprinting of Black Carbon Aerosols in Sites of the Four Emission
Hot Spot Regions of China, J. Geophys. Res.-Atmos., 123, 11735–11747,
https://doi.org/10.1029/2018jd028607, 2018.
Fisseha, R., Spahn, H., Wegener, R., Hohaus, T., Brasse, G., Wissel, H.,
Tillmann, R., Wahner, A., Koppmann, R., and Kiendler-Scharr, A.: Stable
carbon isotope composition of secondary organic aerosol from β-pinene
oxidation, J. Geophys. Res.-Atmos., 114, D02304, https://doi.org/10.1029/2008jd011326, 2009.
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.
Gkatzelis, G. I., Papanastasiou, D. K., Karydis, V. A., Hohaus, T., Liu, Y.,
Schmitt, S. H., Schlag, P., Fuchs, H., Novelli, A., Chen, Q., Cheng, X.,
Broch, S., Dong, H., Holland, F., Li, X., Liu, Y., Ma, X., Reimer, D.,
Rohrer, F., Shao, M., Tan, Z., Taraborrelli, D., Tillmann, R., Wang, H.,
Wang, Y., Wu, Y., Wu, Z., Zeng, L., Zheng, J., Hu, M., Lu, K., Hofzumahaus,
A., Zhang, Y., Wahner, A., and Kiendler-Scharr, A.: Uptake of water-soluble
gas-phase oxidation products drives organic particulate pollution in
Beijing, Geophys. Res. Lett., 48, e2020GL091351,
https://doi.org/10.1029/2020GL091351, 2021.
Gustafsson, Ö., Kruså, M., Zencak, Z., Sheesley, R. J., Granat, L.,
Engström, E., Praveen, P. S., Rao, P. S. P., Leck, C., and Rodhe, H.:
Brown Clouds over South Asia: Biomass or Fossil Fuel Combustion, Science,
323, 495–498, https://doi.org/10.1126/science.1164857, 2009.
Hallquist, M., Wenger, J. C., Baltensperger, U., Rudich, Y., Simpson, D., Claeys, M., Dommen, J., Donahue, N. M., George, C., Goldstein, A. H., Hamilton, J. F., Herrmann, H., Hoffmann, T., Iinuma, Y., Jang, M., Jenkin, M. E., Jimenez, J. L., Kiendler-Scharr, A., Maenhaut, W., McFiggans, G., Mentel, Th. F., Monod, A., Prévôt, A. S. H., Seinfeld, J. H., Surratt, J. D., Szmigielski, R., and Wildt, J.: The formation, properties and impact of secondary organic aerosol: current and emerging issues, Atmos. Chem. Phys., 9, 5155–5236, https://doi.org/10.5194/acp-9-5155-2009, 2009.
Ho, K. F., Lee, S. C., Cao, J. J., Kawamura, K., Watanabe, T., Cheng, Y.,
and Chow, J. C.: Dicarboxylic acids, ketocarboxylic acids and dicarbonyls in
the urban roadside area of Hong Kong, Atmos. Environ., 40, 3030–3040,
https://doi.org/10.1016/j.atmosenv.2005.11.069, 2006.
Ho, K. F., Cao, J. J., Lee, S. C., Kawamura, K., Zhang, R. J., Chow, J. C.,
and Watson, J. G.: Dicarboxylic acids, ketocarboxylic acids, and dicarbonyls
in the urban atmosphere of China, J. Geophys. Res.-Atmos., 112, D22S27,
https://doi.org/10.1029/2006JD008011, 2007.
Huang, L., Brook, J. R., Zhang, W., Li, S. M., Graham, L., Ernst, D.,
Chivulescu, A., and Lu, G.: Stable isotope measurements of carbon fractions
(OC/EC) in airborne particulate: A new dimension for source characterization
and apportionment, Atmos. Environ., 40, 2690–2705,
https://doi.org/10.1016/j.atmosenv.2005.11.062, 2006.
Huang, R.-J., Zhang, Y., Bozzetti, C., Ho, K.-F., Cao, J.-J., Han, Y.,
Daellenbach, K. R., Slowik, J. G., Platt, S. M., Canonaco, F., Zotter, P.,
Wolf, R., Pieber, S. M., Bruns, E. A., Crippa, M., Ciarelli, G.,
Piazzalunga, A., Schwikowski, M., Abbaszade, G., Schnelle-Kreis, J.,
Zimmermann, R., An, Z., Szidat, S., Baltensperger, U., El Haddad, I., and
Prevot, A. S. H.: High secondary aerosol contribution to particulate
pollution during haze events in China, Nature, 514, 218–222,
10.1038/nature13774, 2014.
Huang, X.-F. and Yu, J. Z.: Is vehicle exhaust a significant primary source
of oxalic acid in ambient aerosols?, Geophys. Res. Lett., 34, L02808,
https://doi.org/10.1029/2006gl028457, 2007.
Irei, S., Huang, L., Collin, F., Zhang, W., Hastie, D., and Rudolph, J.:
Flow reactor studies of the stable carbon isotope composition of secondary
particulate organic matter generated by OH-radical-induced reactions of
toluene, Atmos. Environ., 40, 5858–5867,
https://doi.org/10.1016/j.atmosenv.2006.05.001, 2006.
Kawamura, K. and Bikkina, S.: A review of dicarboxylic acids and related
compounds in atmospheric aerosols: Molecular distributions, sources and
transformation, Atmos. Res., 170, 140–160, https://doi.org/10.1016/j.atmosres.2015.11.018,
2016.
Kawashima, H. and Haneishi, Y.: Effects of combustion emissions from the
Eurasian continent in winter on seasonal δ13C of elemental carbon in
aerosols in Japan, Atmos. Environ., 46, 568–579,
https://doi.org/10.1016/j.atmosenv.2011.05.015, 2012.
Kirillova, E. N., Sheesley, R. J., Andersson, A., and Gustafsson, Ö.:
Natural abundance 13C and 14C analysis of water-soluble organic carbon in
atmospheric aerosols, Anal. Chem., 82, 7973, https://doi.org/10.1021/ac1014436, 2010.
Kirillova, E. N., Andersson, A., Sheesley, R. J., Kruså, M., Praveen, P.
S., Budhavant, K., Safai, P. D., Rao, P. S. P., and Gustafsson, Ö.: 13C-
and 14C-based study of sources and atmospheric processing of water-soluble
organic carbon (WSOC) in South Asian aerosols, J. Geophys. Res.-Atmos.,
118, 614–626, https://doi.org/10.1002/jgrd.50130, 2013.
Kirillova, E. N., Andersson, A., Han, J., Lee, M., and Gustafsson, Ö.: Sources and light absorption of water-soluble organic carbon aerosols in the outflow from northern China, Atmos. Chem. Phys., 14, 1413–1422, https://doi.org/10.5194/acp-14-1413-2014, 2014a.
Kirillova, E. N., Andersson, A., Tiwari, S., Srivastava, A. K., Bisht, D.
S., and Gustafsson, O.: Water-soluble organic carbon aerosols during a full
New Delhi winter: Isotope-based source apportionment and optical properties,
J. Geophys. Res.-Atmos., 119, 3476–3485, https://doi.org/10.1002/2013jd020041, 2014b.
Lim, Y. B., Tan, Y., Perri, M. J., Seitzinger, S. P., and Turpin, B. J.: Aqueous chemistry and its role in secondary organic aerosol (SOA) formation, Atmos. Chem. Phys., 10, 10521–10539, https://doi.org/10.5194/acp-10-10521-2010, 2010.
Lim, Y. B., Tan, Y., and Turpin, B. J.: Chemical insights, explicit chemistry, and yields of secondary organic aerosol from OH radical oxidation of methylglyoxal and glyoxal in the aqueous phase, Atmos. Chem. Phys., 13, 8651–8667, https://doi.org/10.5194/acp-13-8651-2013, 2013.
Link, M. F., Brophy, P., Fulgham, S. R., Murschell, T., and Farmer, D. K.:
Isoprene versus Monoterpenes as Gas-Phase Organic Acid Precursors in the
Atmosphere, ACS Earth Space Chem., 5, 1600–1612,
https://doi.org/10.1021/acsearthspacechem.1c00093, 2021.
Liu, D., Li, J., Cheng, Z., Zhong, G., Zhu, S., Ding, P., Shen, C., Tian, C., Chen, Y., Zhi, G., and Zhang, G.: Sources of non-fossil-fuel emissions in carbonaceous aerosols during early winter in Chinese cities, Atmos. Chem. Phys., 17, 11491–11502, https://doi.org/10.5194/acp-17-11491-2017, 2017.
Liu, D., Vonwiller, M., Li, J., Liu, J., Szidat, S., Zhang, Y., Tian, C.,
Chen, Y., Cheng, Z., Zhong, G., Fu, P., and Zhang, G.: Fossil and Non-fossil
Fuel Sources of Organic and Elemental Carbonaceous Aerosol in Beijing,
Shanghai, and Guangzhou: Seasonal Carbon Source Variation, Aerosol Air Qual.
Res., 20, 2495–2506, https://doi.org/10.4209/aaqr.2019.12.0642, 2020.
Liu, J., Li, J., Zhang, Y., Liu, D., Ding, P., Shen, C., Shen, K., He, Q.,
Ding, X., Wang, X., Chen, D., Szidat, S., and Zhang, G.: Source
apportionment using radiocarbon and organic tracers for PM2.5 carbonaceous
aerosols in Guangzhou, South China: contrasting local- and regional-scale
haze events, Environ. Sci. Technol., 48, 12002–12011, https://doi.org/10.1021/es503102w,
2014.
Liu, J., Li, J., Liu, D., Ding, P., Shen, C., Mo, Y., Wang, X., Luo, C., Cheng, Z., Szidat, S., Zhang, Y., Chen, Y., and Zhang, G.: Source apportionment and dynamic changes of carbonaceous aerosols during the haze bloom-decay process in China based on radiocarbon and organic molecular tracers, Atmos. Chem. Phys., 16, 2985–2996, https://doi.org/10.5194/acp-16-2985-2016, 2016a.
Liu, J., Li, J., Vonwiller, M., Liu, D., Cheng, H., Shen, K., Salazar, G.,
Agrios, K., Zhang, Y., He, Q., Ding, X., Zhong, G., Wang, X., Szidat, S.,
and Zhang, G.: The importance of non-fossil sources in carbonaceous aerosols
in a megacity of central China during the 2013 winter haze episode: A source
apportionment constrained by radiocarbon and organic tracers, Atmos.
Environ., 144, 60–68, https://doi.org/10.1016/j.atmosenv.2016.08.068, 2016b.
Lv, S., Wang, F., Wu, C., Chen, Y., Liu, S., Zhang, S., Li, D., Du, W.,
Zhang, F., Wang, H., Huang, C., Fu, Q., Duan, Y., and Wang, G.:
Gas-to-Aerosol Phase Partitioning of Atmospheric Water-Soluble Organic
Compounds at a Rural Site in China: An Enhancing Effect of NH3 on SOA
Formation, Environ. Sci. Technol., 56, 3915–3924, https://doi.org/10.1021/acs.est.1c06855,
2022.
Martinelli, L. A., Camargo, P. B., Lara, L., Victoria, R. L., and Artaxo,
P.: Stable carbon and nitrogen isotopic composition of bulk aerosol
particles in a C4 plant landscape of southeast Brazil, Atmos. Environ., 36,
2427–2432, https://doi.org/10.1016/s1352-2310(01)00454-x, 2002.
Meng, J., Wang, G., Hou, Z., Liu, X., Wei, B., Wu, C., Cao, C., Wang, J., Li, J., Cao, J., Zhang, E., Dong, J., Liu, J., Ge, S., and Xie, Y.: Molecular distribution and stable carbon isotopic compositions of dicarboxylic acids and related SOA from biogenic sources in the summertime atmosphere of Mt. Tai in the North China Plain, Atmos. Chem. Phys., 18, 15069–15086, https://doi.org/10.5194/acp-18-15069-2018, 2018.
Mo, Y., Li, J., Cheng, Z., Zhong, G., Zhu, S., Tian, C., Chen, Y., and
Zhang, G.: Dual carbon isotope-based source apportionment and light
absorption properties of water-soluble organic carbon in PM2.5 over China,
J. Geophys. Res.-Atmos., 126, e2020JD033920,
https://doi.org/10.1029/2020JD033920, 2021.
Myriokefalitakis, S., Tsigaridis, K., Mihalopoulos, N., Sciare, J., Nenes, A., Kawamura, K., Segers, A., and Kanakidou, M.: In-cloud oxalate formation in the global troposphere: a 3-D modeling study, Atmos. Chem. Phys., 11, 5761–5782, https://doi.org/10.5194/acp-11-5761-2011, 2011.
Pavuluri, C. M. and Kawamura, K.: Evidence for 13-carbon enrichment in
oxalic acid via iron catalyzed photolysis in aqueous phase, Geophys. Res.
Lett., 39, L03802, https://doi.org/10.1029/2011gl050398, 2012.
Pavuluri, C. M., Kawamura, K., and Swaminathan, T.: Water-soluble organic
carbon, dicarboxylic acids, ketoacids, and α-dicarbonyls in the
tropical Indian aerosols, J. Geophys. Res.-Atmos., 115, D11302,
https://doi.org/10.1029/2009jd012661, 2010.
Pavuluri, C. M., Kawamura, K., Swaminathan, T., and Tachibana, E.: Stable
carbon isotopic compositions of total carbon, dicarboxylic acids and
glyoxylic acid in the tropical Indian aerosols: Implications for sources and
photochemical processing of organic aerosols, J. Geophys. Res.-Atmos., 116, D18307,
https://doi.org/10.1029/2011jd015617, 2011.
Qi, W., Wang, G., Dai, W., Liu, S., Zhang, T., Wu, C., Li, J., Shen, M.,
Guo, X., Meng, J., and Li, J.: Molecular characteristics and stable carbon
isotope compositions of dicarboxylic acids and related compounds in
wintertime aerosols of Northwest China, Sci. Rep., 12, 11266,
https://doi.org/10.1038/s41598-022-15222-6, 2022.
Qiu, X., Duan, L., Chai, F., Wang, S., Yu, Q., and Wang, S.: Deriving
High-Resolution Emission Inventory of Open Biomass Burning in China based on
Satellite Observations, Environ. Sci. Technol., 50, 11779–11786,
https://doi.org/10.1021/acs.est.6b02705, 2016.
Shen, M., Ho, K. F., Dai, W., Liu, S., Zhang, T., Wang, Q., Meng, J., Chow, J. C., Watson, J. G., Cao, J., and Li, J.: Distribution and stable carbon isotopic composition of dicarboxylic acids, ketocarboxylic acids and α-dicarbonyls in fresh and aged biomass burning aerosols, Atmos. Chem. Phys., 22, 7489–7504, https://doi.org/10.5194/acp-22-7489-2022, 2022.
Smith, B. N. and Epstein, S.: Two categories of 13C 12C ratios for higher
plants, Plant Physiol., 47, 380–384, https://doi.org/10.1104/pp.47.3.380, 1971.
Szidat, S., Jenk, T. M., Gaggeler, H. W., Synal, H. A., Fisseha, R.,
Baltensperger, U., Kalberer, M., Samburova, V., Wacker, L., Saurer, M.,
Schwikowski, M., and Hajdas, I.: Source apportionment of aerosols by C-14
measurements in different carbonaceous particle fractions, Radiocarbon, 46,
475–484, https://doi.org/10.1017/s0033822200039783, 2004.
Szidat, S., Jenk, T. M., Synal, H. A., Kalberer, M., Wacker, L., Hajdas, I.,
Kasper-Giebl, A., and Baltensperger, U.: Contributions of fossil fuel,
biomass-burning, and biogenic emissions to carbonaceous aerosols in Zurich
as traced by C-14, J. Geophys. Res.-Atmos., 111, D07206, https://doi.org/10.1029/2005jd006590,
2006.
van Pinxteren, D., Neusüß, C., and Herrmann, H.: On the abundance and source contributions of dicarboxylic acids in size-resolved aerosol particles at continental sites in central Europe, Atmos. Chem. Phys., 14, 3913–3928, https://doi.org/10.5194/acp-14-3913-2014, 2014.
Wang, J., Wang, G., Wu, C., Li, J., Cao, C., Li, J., Xie, Y., Ge, S., Chen,
J., Zeng, L., Zhu, T., Zhang, R., and Kawamura, K.: Enhanced aqueous-phase
formation of secondary organic aerosols due to the regional biomass burning
over North China Plain, Environ. Pollut., 256, 113401,
https://doi.org/10.1016/j.envpol.2019.113401, 2020.
Wang, J., Ye, J., Zhang, Q., Zhao, J., Wu, Y., Li, J., Liu, D., Li, W.,
Zhang, Y., Wu, C., Xie, C., Qin, Y., Lei, Y., Huang, X., Guo, J., Liu, P.,
Fu, P., Li, Y., Lee, H. C., Choi, H., Zhang, J., Liao, H., Chen, M., Sun,
Y., Ge, X., Martin, S. T., and Jacob, D. J.: Aqueous production of secondary
organic aerosol from fossil-fuel emissions in winter Beijing haze, P.
Natl. Acad. Sci. USA, 118, e2022179118, https://doi.org/10.1073/pnas.2022179118, 2021.
Warneck, P.: In-cloud chemistry opens pathway to the formation of oxalic
acid in the marine atmosphere, Atmos. Environ., 37, 2423–2427,
https://doi.org/10.1016/S1352-2310(03)00136-5, 2003.
Widory, D., Roy, S., Le Moullec, Y., Goupil, G., Cocherie, A., and Guerrot,
C.: The origin of atmospheric particles in Paris: a view through carbon and
lead isotopes, Atmos. Environ., 38, 953–961,
https://doi.org/10.1016/j.atmosenv.2003.11.001, 2004.
Wu, Z., Wang, Y., Tan, T., Zhu, Y., Li, M., Shang, D., Wang, H., Lu, K.,
Guo, S., Zeng, L., and Zhang, Y.: Aerosol liquid water driven by
anthropogenic inorganic salts: implying its key role in haze formation over
the North China Plain, Environ. Sci. Tech. Let., 5, 160–166,
https://doi.org/10.1021/acs.estlett.8b00021, 2018.
Xing, J., Lu, X., Wang, S., Wang, T., Ding, D., Yu, S., Shindell, D., Ou,
Y., Morawska, L., Li, S., Ren, L., Zhang, Y., Loughlin, D., Zheng, H., Zhao,
B., Liu, S., Smith, K. R., and Hao, J.: The quest for improved air quality
may push China to continue its CO2 reduction beyond the Paris Commitment,
P. Natl. Acad. Sci. USA, 117, 29535–29542, https://doi.org/10.1073/pnas.2013297117, 2020.
Xu, B., Cheng, Z., Gustafsson, Ö., Kawamura, K., Jin, B., Zhu, S., Tang,
T., Zhang, B., Li, J., and Zhang, G.: Compound-specific radiocarbon analysis
of low molecular weight dicarboxylic acids in ambient aerosols using
preparative gas chromatography: method development, Environ. Sci. Technol.
Lett., 8, 135–141, https://doi.org/10.1021/acs.estlett.0c00887, 2021.
Xu, B., Zhang, G., Gustafsson, Ö., Kawamura, K., Li, J., Andersson, A.,
Bikkina, S., Kunwar, B., Pokhrel, A., Zhong, G., Zhao, S., Li, J., Huang,
C., Cheng, Z., Zhu, S., Peng, P., and Sheng, G.: Large contribution of
fossil-derived components to aqueous secondary organic aerosols in China,
Nat. Commun., 13, 5115, https://doi.org/10.1038/s41467-022-32863-3, 2022.
Yu, Q., Chen, J., Cheng, S., Qin, W., Zhang, Y., Sun, Y., and Ahmad, M.:
Seasonal variation of dicarboxylic acids in PM2.5 in Beijing: Implications
for the formation and aging processes of secondary organic aerosols, Sci.
Total Environ., 763, 142964,
https://doi.org/10.1016/j.scitotenv.2020.142964, 2021.
Zhang, G., Liu, J., Li, J., Li, P., Wei, N., and Xu, B.: Radiocarbon isotope
technique as a powerful tool in tracking anthropogenic emissions of
carbonaceous air pollutants and greenhouse gases: A review, Fundam. Res., 1,
306–316, https://doi.org/10.1016/j.fmre.2021.03.007, 2021.
Zhang, Y., Ren, H., Sun, Y., Cao, F., Chang, Y., Liu, S., Lee, X., Agrios,
K., Kawamura, K., Liu, D., Ren, L., Du, W., Wang, Z., Prévôt, A. S.
H., Szidat, S., and Fu, P.: High Contribution of Nonfossil Sources to
Submicrometer Organic Aerosols in Beijing, China, Environ. Sci. Technol.,
51, 7842–7852, https://doi.org/10.1021/acs.est.7b01517, 2017.
Zhang, Y.-L., Schnelle-Kreis, J., Abbaszade, G., Zimmermann, R., Zotter, P.,
Shen, R.-R., Schaefer, K., Shao, L., Prevot, A. S. H., and Szidat, S.:
Source Apportionment of Elemental Carbon in Beijing, China: Insights from
Radiocarbon and Organic Marker Measurements, Environ. Sci. Technol., 49,
8408–8415, https://doi.org/10.1021/acs.est.5b01944, 2015.
Zhang, Y.-L., Kawamura, K., Cao, F., and Lee, M.: Stable carbon isotopic
compositions of low-molecular-weight dicarboxylic acids, oxocarboxylic
acids, α-dicarbonyls, and fatty acids: Implications for atmospheric
processing of organic aerosols, J. Geophys. Res.-Atmos., 121, 3707–3717,
https://doi.org/10.1002/2015jd024081, 2016.
Zhao, B., Zheng, H., Wang, S., Smith, K. R., Lu, X., Aunan, K., Gu, Y.,
Wang, Y., Ding, D., Xing, J., Fu, X., Yang, X., Liou, K.-N., and Hao, J.:
Change in household fuels dominates the decrease in PM2.5 exposure and premature
mortality in China in 2005–2015, P. Natl. Acad. Sci. USA, 115,
12401–12406, https://doi.org/10.1073/pnas.1812955115, 2018.
Zhao, S., Tian, L., Zou, Z., Liu, X., Zhong, G., Mo, Y., Wang, Y., Tian, Y.,
Li, J., Guo, H., and Zhang, G.: Probing Legacy and Alternative Flame
Retardants in the Air of Chinese Cities, Environ. Sci. Technol., 55, 9450–9459,
https://doi.org/10.1021/acs.est.0c07367, 2021.
Zhu, S., Ding, P., Wang, N., Shen, C., Jia, G., and Zhang, G.: The compact
AMS facility at Guangzhou Institute of Geochemistry, Chinese Academy of
Sciences, Nucl. Instrum. Meth. B, 361, 72–75,
https://doi.org/10.1016/j.nimb.2015.06.040, 2015.
Short summary
We analyzed compound-specific dual-carbon isotope signatures (Δ14C and δ13C) of dominant secondary organic aerosol (SOA) tracer molecules (i.e., oxalic acid) to investigate the fates of SOAs in the atmosphere at five emission hotspots in China. The results indicated that SOA carbon sources and chemical processes producing SOAs vary spatially and seasonally, and these variations need to be included in Chinese climate projection models and air quality management practices.
We analyzed compound-specific dual-carbon isotope signatures (Δ14C and δ13C) of dominant...
Altmetrics
Final-revised paper
Preprint