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Discussion papers
https://doi.org/10.5194/acp-2018-1177
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2018-1177
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 11 Jan 2019

Research article | 11 Jan 2019

Review status
This discussion paper is a preprint. It is a manuscript under review for the journal Atmospheric Chemistry and Physics (ACP).

A Large Contribution of Anthropogenic Organo-Nitrates to Secondary Organic Aerosol in the Alberta Oil Sands

Alex K. Y. Lee1,2, Max G. Adam2, John Liggio3, Shao-Meng Li3, Kun Li3, Megan D. Willis4,a, Jonathan P. D. Abbatt4, Travis W. Tokarek5, Charles A. Odame-Ankrah5, Hans D. Osthoff5, Kevin Strawbridge3, and Jeffery R. Brook3 Alex K. Y. Lee et al.
  • 1Department of Civil and Environmental Engineering, National University of Singapore, Singapore
  • 2NUS Environmental Research Institute, National University of Singapore, Singapore
  • 3Air Quality Process Research Section, Environment and Climate Change Canada, Toronto, ON, Canada
  • 4Department of Chemistry, University of Toronto, Toronto, ON, Canada
  • 5Department of Department of Chemistry, University of Calgary, Calgary, AB, Canada
  • anow at: Lawrence Berkeley National Lab, Chemical Sciences Division, Berkeley, CA, USA

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 for 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 tonnes/day. We demonstrate that pON formation occurs via photooxidation 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 photooxidation 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 aging. 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 IVOC and NOx emissions.

Alex K. Y. Lee et al.
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Short summary
This work provides the first direct field evidence that anthropogenic organo-nitrate contributed up to half of secondary organic aerosol (SOA) mass that was freshly produced within the emission plumes of oil sands facilities in Alberta, Canada. The finding illustrates the central role of organo-nitrate in SOA production from the oil and gas industry, with relevance for other urban and industrial regions with significant intermediate-volatility organic compounds (IVOCs) and NOx emissions.
This work provides the first direct field evidence that anthropogenic organo-nitrate contributed...
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