High secondary aerosol contribution to particulate pollution during haze events in China (original) (raw)

Nature volume 514, pages 218–222 (2014)Cite this article

Subjects

Abstract

Rapid industrialization and urbanization in developing countries has led to an increase in air pollution, along a similar trajectory to that previously experienced by the developed nations1. In China, particulate pollution is a serious environmental problem that is influencing air quality, regional and global climates, and human health[2](/articles/nature13774#ref-CR2 "Wang, Y., Zhang, R. Y. & Saravanan, R. Asian pollution climatically modulates mid-latitude cyclones following hierarchical modeling and observational analysis. Nature Commun. 5, http://dx.doi.org/10.1038/ncomms4098

             (2014)"),[3](/articles/nature13774#ref-CR3 "Cao, J. J. Pollution status and control strategies of PM2. 5 in China. J. Earth Environ. 3, 1030–1036 (2012)"). In response to the extremely severe and persistent haze pollution experienced by about 800 million people during the first quarter of 2013 (refs [4](/articles/nature13774#ref-CR4 "China National Environmental Monitoring Centre. Air Quality Report in 74 Chinese Cities in March and the First Quarter 2013 (
              http://www.cnemc.cn/publish/106/news/news_34605.html
              
             (in Chinese), accessed on, 11 June 2013)"), [5](/articles/nature13774#ref-CR5 "Chen, R. J., Zhao, Z. H. & Kan, H. D. Heavy smog and hospital visits in Beijing, China. Am. J. Respir. Crit. Care Med. 188, 1170–1171 (2013)")), the Chinese State Council announced its aim to reduce concentrations of PM2.5 (particulate matter with an aerodynamic diameter less than 2.5 micrometres) by up to 25 per cent relative to 2012 levels by 2017 (ref. [6](/articles/nature13774#ref-CR6 "Chinese State Council. Atmospheric Pollution Prevention and Control Action Plan (
              http://www.gov.cn/zwgk/2013-09/12/content_2486773.htm
              
             (in Chinese), accessed on, 12 September 2013)")). Such efforts however require elucidation of the factors governing the abundance and composition of PM2.5, which remain poorly constrained in China[3](/articles/nature13774#ref-CR3 "Cao, J. J. Pollution status and control strategies of PM2. 5 in China. J. Earth Environ. 3, 1030–1036 (2012)"),[7](/articles/nature13774#ref-CR7 "Zhang, Q., He, K. B. & Huo, H. Cleaning China’s air. Nature 484, 161–162 (2012)"),[8](/articles/nature13774#ref-CR8 "Yang, F. et al. Characteristics of PM2. 5 speciation in representative megacities and across China. Atmos. Chem. Phys. 11, 5207–5219 (2011)"). Here we combine a comprehensive set of novel and state-of-the-art offline analytical approaches and statistical techniques to investigate the chemical nature and sources of particulate matter at urban locations in Beijing, Shanghai, Guangzhou and Xi’an during January 2013\. We find that the severe haze pollution event was driven to a large extent by secondary aerosol formation, which contributed 30–77 per cent and 44–71 per cent (average for all four cities) of PM2.5 and of organic aerosol, respectively. On average, the contribution of secondary organic aerosol (SOA) and secondary inorganic aerosol (SIA) are found to be of similar importance (SOA/SIA ratios range from 0.6 to 1.4). Our results suggest that, in addition to mitigating primary particulate emissions, reducing the emissions of secondary aerosol precursors from, for example, fossil fuel combustion and biomass burning is likely to be important for controlling China’s PM2.5 levels and for reducing the environmental, economic and health impacts resulting from particulate pollution.

This is a preview of subscription content, access via your institution

Access options

Subscribe to this journal

Receive 51 print issues and online access

$199.00 per year

only $3.90 per issue

Buy this article

Prices may be subject to local taxes which are calculated during checkout

Additional access options:

Similar content being viewed by others

References

  1. Seinfeld, J. H. Air pollution: a half century of progress. Am. Inst. Chem. Eng. J. 50, 1096–1108 (2004)
    Article CAS Google Scholar
  2. Wang, Y., Zhang, R. Y. & Saravanan, R. Asian pollution climatically modulates mid-latitude cyclones following hierarchical modeling and observational analysis. Nature Commun. 5, http://dx.doi.org/10.1038/ncomms4098 (2014)
  3. Cao, J. J. Pollution status and control strategies of PM2. 5 in China. J. Earth Environ. 3, 1030–1036 (2012)
    Google Scholar
  4. China National Environmental Monitoring Centre. Air Quality Report in 74 Chinese Cities in March and the First Quarter 2013 (http://www.cnemc.cn/publish/106/news/news_34605.html (in Chinese), accessed on, 11 June 2013)
  5. Chen, R. J., Zhao, Z. H. & Kan, H. D. Heavy smog and hospital visits in Beijing, China. Am. J. Respir. Crit. Care Med. 188, 1170–1171 (2013)
    Article Google Scholar
  6. Chinese State Council. Atmospheric Pollution Prevention and Control Action Plan (http://www.gov.cn/zwgk/2013-09/12/content_2486773.htm (in Chinese), accessed on, 12 September 2013)
  7. Zhang, Q., He, K. B. & Huo, H. Cleaning China’s air. Nature 484, 161–162 (2012)
    Article ADS CAS Google Scholar
  8. Yang, F. et al. Characteristics of PM2. 5 speciation in representative megacities and across China. Atmos. Chem. Phys. 11, 5207–5219 (2011)
    Article ADS CAS Google Scholar
  9. Wuebbles, D. J., Lei, H. & Lin, J. T. Intercontinental transport of aerosols and photochemical oxidants from Asia and its consequences. Environ. Pollut. 150, 65–84 (2007)
    Article CAS Google Scholar
  10. Jimenez, J. L. et al. Evolution of organic aerosols in the atmosphere. Science 326, 1525–1529 (2009)
    Article ADS CAS Google Scholar
  11. Watson, J. G. et al. CMB8 Applications and Validation Protocol for PM2.5 and VOCs (US Environmental Protection Agency and Desert Research Institute, Reno, Nevada, 1998)
  12. Canonaco, F., Crippa, M., Slowik, J. G., Baltensperger, U. & Prévôt, A. S. H. SoFi, an IGOR-based interface for the efficient use of the generalized multilinear engine (ME-2) for source apportionment: ME-2 application to aerosol mass spectrometer data. Atmos. Meas. Tech. 6, 3649–3661 (2013)
    Article Google Scholar
  13. DeCarlo, P. F. et al. Field-deployable, high-resolution, time-of-flight aerosol mass spectrometer. Anal. Chem. 78, 8281–8289 (2006)
    Article CAS Google Scholar
  14. Orasche, J., Schnelle-Kreis, J., Abbaszade, G. & Zimmermann, R. Technical note: in-situ derivatization thermal desorption GC-TOFMS for direct analysis of particle-bound non-polar and polar organic species. Atmos. Chem. Phys. 11, 8977–8993 (2011)
    Article ADS CAS Google Scholar
  15. Zhang, Y. L. et al. On the isolation of OC and EC and the optimal strategy of radiocarbon-based source apportionment of carbonaceous aerosols. Atmos. Chem. Phys. 12, 10841–10856 (2012)
    Article ADS CAS Google Scholar
  16. Cao, J. J. et al. On the potential high acid deposition in northeastern China. J. Geophys. Res. 118, 4834–4846 (2013)
    Google Scholar
  17. Robinson, A. L. et al. Rethinking organic aerosols: semivolatile emissions and photochemical aging. Science 315, 1259–1262 (2007)
    Article ADS CAS Google Scholar
  18. Zheng, M. et al. Seasonal trends in PM2. 5 source contributions in Beijing, China. Atmos. Environ. 39, 3967–3976 (2005)
    Article ADS CAS Google Scholar
  19. Wang, G. H. et al. High loadings and source strengths of organic aerosols in China. Geophys. Res. Lett. 33, L22801 (2006)
    Article ADS Google Scholar
  20. Atkinson, R. & Arey, J. Atmospheric degradation of volatile organic compounds. Chem. Rev. 103, 4605–4638 (2003)
    Article CAS Google Scholar
  21. Wang, X. F. et al. The secondary formation of inorganic aerosols in the droplet mode through heterogeneous aqueous reactions under haze conditions. Atmos. Environ. 63, 68–76 (2012)
    Article ADS CAS Google Scholar
  22. Ervens, B., Turpin, B. J. & 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 (2011)
    Article ADS CAS Google Scholar
  23. Seinfeld, J. H. & Pandis, S. N. Atmospheric Chemistry and Physics: From Air Pollution to Climate Change 2nd edn (Wiley, 2006)
    Google Scholar
  24. Hallquist, M. et al. The formation, properties and impact of secondary organic aerosol: current and emerging issues. Atmos. Chem. Phys. 9, 5155–5236 (2009)
    Article ADS CAS Google Scholar
  25. Wang, X. et al. Characterization of organic aerosol produced during pulverized coal combustion in a drop tube furnace. Atmos. Chem. Phys. 13, 10919–10932 (2013)
    Article ADS Google Scholar
  26. Wang, Y., Zhang, Q. Q., He, K., Zhang, Q. & Chai, L. Sulfate-nitrate-ammonium aerosols over China: response to 2000–2015 emission changes of sulfur dioxide, nitrogen oxides, and ammonia. Atmos. Chem. Phys. 13, 2635–2652 (2013)
    Article ADS Google Scholar
  27. Xing, J. et al. Projections of air pollutant emissions and its impacts on regional air quality in China in 2020. Atmos. Chem. Phys. 11, 3119–3136 (2011)
    Article ADS CAS Google Scholar
  28. Tiwari, S. et al. Diurnal and seasonal variations of black carbon and PM2.5 over New Delhi, India: Influence of meteorology. Atmos. Res. 125–126, 50–62 (2013)
    Article Google Scholar
  29. The United Nations Environment Program (UNEP). Africa Environment Outlook 3: Our Environment, Our Health (2013); available at http://www.unep.org/pdf/aeo3.pdf
  30. The World Health Organization (WHO). 7 Million Premature Deaths Annually Linked to Air Pollution (published online 25 March 2014); available at http://www.who.int/mediacentre/news/releases/2014/air-pollution/en/

Download references

Acknowledgements

The research leading to these results received funding from the European Community’s Seventh Framework Programme (FP7/2007-2013) under grant agreement no. 290605, the Swiss National Science Foundation (SAPMAV, no.200021_13016, WOOSHI, no. 200021L_140590, and Ambizione, PZ00P2_131673), the Swiss Competence Centers Environment and Sustainability as well as Energy and Mobility under project OPTIWARES, the National Science Foundation of China (no. 40925009), the “Strategic Priority Research Program” of the Chinese Academy of Sciences (XDA05100402), and the Helmholtz Virtual Institute of Complex Molecular Systems in Environmental Health – Aerosol and Health (HICE). The help of G. Salazar (University of Bern) during 14C analysis is acknowledged.

Author information

Author notes

  1. Monica Crippa
    Present address: Present address: European Commission, Joint Research Centre, Institute for Environment and Sustainability, Air and Climate Unit, Via Fermi, 2749, 21027 Ispra, Italy.,
  2. Ru-Jin Huang and Imad El Haddad: These authors contributed equally to this work.

Authors and Affiliations

  1. Laboratory of Atmospheric Chemistry, Paul Scherrer Institute (PSI), 5232 Villigen, Switzerland,
    Ru-Jin Huang, Carlo Bozzetti, Kaspar R. Daellenbach, Jay G. Slowik, Stephen M. Platt, Francesco Canonaco, Peter Zotter, Robert Wolf, Simone M. Pieber, Emily A. Bruns, Monica Crippa, Giancarlo Ciarelli, Urs Baltensperger, Imad El Haddad & André S. H. Prévôt
  2. State Key Laboratory of Loess and Quaternary Geology (SKLLQG), and Key Laboratory of Aerosol Chemistry and Physics, Institute of Earth Environment, Chinese Academy of Sciences, Xi’an, 710075, China
    Ru-Jin Huang, Jun-Ji Cao, Yongming Han & Zhisheng An
  3. Department of Chemistry and Biochemistry, and Oeschger Centre for Climate Change Research, University of Bern, 3012 Bern, Switzerland,
    Yanlin Zhang, Margit Schwikowski & Sönke Szidat
  4. Laboratory of Radiochemistry and Environmental Chemistry, Paul Scherrer Institute (PSI), 5232 Villigen, Switzerland,
    Yanlin Zhang & Margit Schwikowski
  5. The Jockey Club School of Public Health and Primary Care, The Chinese University of Hong Kong, Hong Kong, China
    Kin-Fai Ho
  6. Department of Earth and Environmental Sciences, University of Milano Bicocca, Piazza della Scienza 1, Milan 20126, Italy,
    Andrea Piazzalunga
  7. Helmholtz Zentrum München, German Research Center for Environmental Health (GmbH), Joint Mass Spectrometry Centre, Cooperation Group Comprehensive Molecular Analytics and Helmholtz Virtual Institute of Complex Molecular Systems in Environmental Health — Aerosol and Health (HICE), 85764 Neuherberg, Germany,
    Gülcin Abbaszade, Jürgen Schnelle-Kreis & Ralf Zimmermann
  8. University of Rostock, Joint Mass Spectrometry Centre, Institute of Chemistry, Analytical Chemistry, 18015 Rostock, Germany,
    Ralf Zimmermann

Authors

  1. Ru-Jin Huang
    You can also search for this author inPubMed Google Scholar
  2. Yanlin Zhang
    You can also search for this author inPubMed Google Scholar
  3. Carlo Bozzetti
    You can also search for this author inPubMed Google Scholar
  4. Kin-Fai Ho
    You can also search for this author inPubMed Google Scholar
  5. Jun-Ji Cao
    You can also search for this author inPubMed Google Scholar
  6. Yongming Han
    You can also search for this author inPubMed Google Scholar
  7. Kaspar R. Daellenbach
    You can also search for this author inPubMed Google Scholar
  8. Jay G. Slowik
    You can also search for this author inPubMed Google Scholar
  9. Stephen M. Platt
    You can also search for this author inPubMed Google Scholar
  10. Francesco Canonaco
    You can also search for this author inPubMed Google Scholar
  11. Peter Zotter
    You can also search for this author inPubMed Google Scholar
  12. Robert Wolf
    You can also search for this author inPubMed Google Scholar
  13. Simone M. Pieber
    You can also search for this author inPubMed Google Scholar
  14. Emily A. Bruns
    You can also search for this author inPubMed Google Scholar
  15. Monica Crippa
    You can also search for this author inPubMed Google Scholar
  16. Giancarlo Ciarelli
    You can also search for this author inPubMed Google Scholar
  17. Andrea Piazzalunga
    You can also search for this author inPubMed Google Scholar
  18. Margit Schwikowski
    You can also search for this author inPubMed Google Scholar
  19. Gülcin Abbaszade
    You can also search for this author inPubMed Google Scholar
  20. Jürgen Schnelle-Kreis
    You can also search for this author inPubMed Google Scholar
  21. Ralf Zimmermann
    You can also search for this author inPubMed Google Scholar
  22. Zhisheng An
    You can also search for this author inPubMed Google Scholar
  23. Sönke Szidat
    You can also search for this author inPubMed Google Scholar
  24. Urs Baltensperger
    You can also search for this author inPubMed Google Scholar
  25. Imad El Haddad
    You can also search for this author inPubMed Google Scholar
  26. André S. H. Prévôt
    You can also search for this author inPubMed Google Scholar

Contributions

R.-J.H., I.E.H. and C.B. wrote the paper. R.-J.H., J.-J.C. and A.S.H.P. designed the study. R.-J.H., I.E.H., C.B. and K.R.D. performed the offline AMS analysis. Y.Z., P.Z. and S. S. performed the 14C analysis. M.S. performed the IC analysis. G.A. and J.S.-K. performed the TD-GC-MS analysis. R.-J.H., I.E.H., C.B. and A.S.H.P. analysed the data. All authors reviewed and commented on the paper.

Corresponding authors

Correspondence toJun-Ji Cao or André S. H. Prévôt.

Ethics declarations

Competing interests

The authors declare no competing financial interests.

Supplementary information

Supplementary Information

This file contains additional information on the sample collection and sampling sites (Section 1); details of the chemical analysis (Section 2); extensive evaluation of a set of environmentally optimal solutions for source apportionment of PM2.5 and OC using the CMB and ME-2 models (Section 3); evaluation of model uncertainty and the sensitivity of the results to model inputs as well as the estimate of the contribution of fossil and non-fossil sources to secondary organic aerosol (Section 4); examination of potentially unidentified sources (Section 5); representativeness of the measurement sites (Section 6) and relevance of SOA formation (Section 7). The Supplementary Information also includes Supplementary Figures S1-S30, Supplementary Tables S1-S3 and additional references. (PDF 2634 kb)

PowerPoint slides

Source data

Rights and permissions

About this article

Cite this article

Huang, RJ., Zhang, Y., Bozzetti, C. et al. High secondary aerosol contribution to particulate pollution during haze events in China.Nature 514, 218–222 (2014). https://doi.org/10.1038/nature13774

Download citation

This article is cited by

Editorial Summary

What caused China's atmospheric haze?

Air pollution is an important environmental problem in China, but the factors contributing to the high levels of particulate matter present during haze pollution events remain poorly understood. This paper investigates the chemical nature and sources of particulate matter at urban locations in four Chinese cities during the severe haze pollution event of January 2013, and finds that the event was driven to a large extent by secondary aerosol formation. This indicates that mitigation strategies focused on primary particulate emissions alone are unlikely to be fully effective. Additional measures such as controlling emissions of volatile organic compounds from fossil fuel combustion (mostly coal and traffic) and biomass burning may be required if China's particulate pollution is to be reduced.