A large contribution of anthropogenic organo-nitrates to secondary organic aerosol in the Alberta oil sands
-
Published:2019-10-02
Issue:19
Volume:19
Page:12209-12219
-
ISSN:1680-7324
-
Container-title:Atmospheric Chemistry and Physics
-
language:en
-
Short-container-title:Atmos. Chem. Phys.
Author:
Lee Alex K. Y., Adam Max G., Liggio John, Li Shao-MengORCID, Li KunORCID, Willis Megan D.ORCID, Abbatt Jonathan P. D.ORCID, Tokarek Travis W., Odame-Ankrah Charles A., Osthoff Hans D.ORCID, Strawbridge Kevin, Brook Jeffery R.
Abstract
Abstract. The oil sands industry in Alberta, Canada, represents a large anthropogenic
source of secondary organic aerosol (SOA). Atmospheric emissions from oil
sands operations are a complex mixture of gaseous and particulate
pollutants. Their interaction can affect the formation and characteristics
of SOA during plume dispersion, but their chemical evolution remains poorly
understood. Oxidative processing of organic vapours in the presence of
NOx can lead to particulate organo-nitrate (pON) formation, with
important impacts on the SOA budgets, the nitrogen cycle and human health.
We provide the first direct field evidence, from ground- and aircraft-based
real-time aerosol mass spectrometry, that anthropogenic pON contributed up
to half of SOA mass that was freshly produced within the emission plumes of
oil sands facilities. Using a top-down emission-rate retrieval algorithm
constrained by aircraft measurements, we estimate the production rate of pON
in the oil sands region to be ∼15.5 t d−1. We
demonstrate that pON formation occurs via photo-oxidation of
intermediate-volatility organic compounds (IVOCs) in high-NOx
environments, providing observational constraints to improve current SOA
modelling frameworks. Our ambient observations are supported by laboratory
photo-oxidation experiments of IVOCs from bitumen vapours under high-NOx
conditions, which demonstrate that pON can account for 30 %–55 % of the
observed SOA mass depending on the degree of photochemical ageing. The large
contribution of pON to freshly formed anthropogenic SOA illustrates the
central role of pON in SOA production from the oil and gas industry, with
relevance for other urban and industrial regions with significant
anthropogenic IVOC and NOx emissions.
Publisher
Copernicus GmbH
Subject
Atmospheric Science
Reference46 articles.
1. Alberta Energy Regulator: Alberta's Energy Reserves 2014 and Supply/Demand
Outlook 2015–2024, 2014. 2. Boyd, C. M., Sanchez, J., Xu, L., Eugene, A. J., Nah, T., Tuet, W. Y., Guzman, M. I., and Ng, N. L.: Secondary organic aerosol formation from the β-pinene + NO3 system: effect of humidity and peroxy radical fate, Atmos. Chem. Phys., 15, 7497–7522, https://doi.org/10.5194/acp-15-7497-2015, 2015. 3. Brown, S. S., Talukdar, R. K., and Ravishankara, A. R.: Rate constants for
the reaction OH + NO2 +M->HNO3 + M under atmospheric
conditions, Chem. Phys. Lett., 299, 277–284, https://doi.org/10.1016/s0009-2614(98)01283-4,
1999. 4. Cappa, C. D., Onasch, T. B., Massoli, P., Worsnop, D. R., Bates, T. S.,
Cross, E. S., Davidovits, P., Hakala, J., Hayden, K. L., Jobson, B. T.,
Kolesar, K. R., Lack, D. A., Lerner, B. M., Li, S. M., Mellon, D., Nuaaman,
I., Olfert, J. S., Petaja, T., Quinn, P. K., Song, C., Subramanian, R.,
Williams, E. J., and Zaveri, R. A.: Radiative Absorption Enhancements Due to
the Mixing State of Atmospheric Black Carbon, Science, 337, 1078–1081,
https://doi.org/10.1126/science.1223447, 2012. 5. Ehn, M., Thornton, J. A., Kleist, E., Sipila, M., Junninen, H., Pullinen,
I., Springer, M., Rubach, F., Tillmann, R., Lee, B., Lopez-Hilfiker, F.,
Andres, S., Acir, I. H., Rissanen, M., Jokinen, T., Schobesberger, S.,
Kangasluoma, J., Kontkanen, J., Nieminen, T., Kurten, T., Nielsen, L. B.,
Jorgensen, S., Kjaergaard, H. G., Canagaratna, M., Dal Maso, M., Berndt, T.,
Petaja, T., Wahner, A., Kerminen, V. M., Kulmala, M., Worsnop, D. R., Wildt,
J., and Mentel, T. F.: A large source of low-volatility secondary organic
aerosol, Nature, 506, 476–479, https://doi.org/10.1038/nature13032, 2014.
Cited by
16 articles.
订阅此论文施引文献
订阅此论文施引文献,注册后可以免费订阅5篇论文的施引文献,订阅后可以查看论文全部施引文献
|
|