Dataset Information

Nitrate radicals and biogenic volatile organic compounds: oxidation, mechanisms, and organic aerosol.

ABSTRACT: Oxidation of biogenic volatile organic compounds (BVOC) by the nitrate radical (NO₃) represents one of the important interactions between anthropogenic emissions related to combustion and natural emissions from the biosphere. This interaction has been recognized for more than 3 decades, during which time a large body of research has emerged from laboratory, field, and modeling studies. NO₃-BVOC reactions influence air quality, climate and visibility through regional and global budgets for reactive nitrogen (particularly organic nitrates), ozone, and organic aerosol. Despite its long history of research and the significance of this topic in atmospheric chemistry, a number of important uncertainties remain. These include an incomplete understanding of the rates, mechanisms, and organic aerosol yields for NO₃-BVOC reactions, lack of constraints on the role of heterogeneous oxidative processes associated with the NO₃ radical, the difficulty of characterizing the spatial distributions of BVOC and NO₃ within the poorly mixed nocturnal atmosphere, and the challenge of constructing appropriate boundary layer schemes and non-photochemical mechanisms for use in state-of-the-art chemical transport and chemistry-climate models. This review is the result of a workshop of the same title held at the Georgia Institute of Technology in June 2015. The first half of the review summarizes the current literature on NO₃-BVOC chemistry, with a particular focus on recent advances in instrumentation and models, and in organic nitrate and secondary organic aerosol (SOA) formation chemistry. Building on this current understanding, the second half of the review outlines impacts of NO₃-BVOC chemistry on air quality and climate, and suggests critical research needs to better constrain this interaction to improve the predictive capabilities of atmospheric models.

SUBMITTER: Ng NL

PROVIDER: S-EPMC6104845 | biostudies-literature | 2017

REPOSITORIES: biostudies-literature

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Nitrate radicals and biogenic volatile organic compounds: oxidation, mechanisms, and organic aerosol.

Ng Nga Lee NL Brown Steven S SS Archibald Alexander T AT Atlas Elliot E Cohen Ronald C RC Crowley John N JN Day Douglas A DA Donahue Neil M NM Fry Juliane L JL Fuchs Hendrik H Griffin Robert J RJ Guzman Marcelo I MI Herrmann Hartmut H Hodzic Alma A Iinuma Yoshiteru Y Jimenez José L JL Kiendler-Scharr Astrid A Lee Ben H BH Luecken Deborah J DJ Mao Jingqiu J McLaren Robert R Mutzel Anke A Osthoff Hans D HD Ouyang Bin B Picquet-Varrault Benedicte B Platt Ulrich U Pye Havala O T HOT Rudich Yinon Y Schwantes Rebecca H RH Shiraiwa Manabu M Stutz Jochen J Thornton Joel A JA Tilgner Andreas A Williams Brent J BJ Zaveri Rahul A RA

Atmospheric chemistry and physics 20170101 3

Oxidation of biogenic volatile organic compounds (BVOC) by the nitrate radical (NO<sub>3</sub>) represents one of the important interactions between anthropogenic emissions related to combustion and natural emissions from the biosphere. This interaction has been recognized for more than 3 decades, during which time a large body of research has emerged from laboratory, field, and modeling studies. NO<sub>3</sub>-BVOC reactions influence air quality, climate and visibility through regional and glo ...[more]

PMID: 30147712

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Project description:The nitrate radical (NO3) oxidation of isoprene is an important contributor to secondary organic aerosol (SOA). Isoprene has two double bonds which allow for multigeneration oxidation to occur. The effects of multigeneration chemistry on the gas- and particle-phase product distributions of the isoprene + NO3 system are not fully understood. In this study, we conduct chamber experiments by varying the ratio of N2O5 (precursor of NO3) to isoprene concentration from 1:1 to 14:1 to investigate the formation of products in both phases under different oxidation levels. Multigeneration chemistry leads to the formation of gas-phase products which then partition into particle phase depending on the product volatility; first-generation products (15-36% of total SOA) such as C5H9NO5 and C10H16N2O9 have volatility (log10C* = 1.0-3.0 using the partitioning method and log10C* = 2.6-4.5 using the formula method) 1-5 orders of magnitude higher than second-generation products (37-57% of total SOA, log10C* = -0.8-2.1 using the partitioning method and log10C* = -3.7-1.8 using the formula method) such as C5H8,10N2O8, C5H9N3O10, and C10H17N3O13. The fast reaction rate constants of first-generation products (estimated to be on the order of 10-13 cm3 molecules-1 s-1 at 295 K) and the lower volatility of second-generation products result in increased SOA yields when NO3 availability increases and multigeneration chemistry is enhanced. Specifically, an increase of up to 300% in SOA yield is observed when the N2O5/isoprene ratio increases from 1:1 to 3:1; from 5.7% (organic aerosol mass concentration, ΔM o = 4.2 μg/m3) to 16.3% (ΔM o = 11.9 μg/m3) when the reacted isoprene concentration is 25 ppb and from 3.1% (ΔM o = 1.2 μg/m3) to 12.4% (ΔM o = 5.4 μg/m3) when the reacted isoprene concentration is 15 ppb. The maximum SOA yield occurs when the N2O5/isoprene ratio is greater than or equal to 3:1 as a combined result of multigeneration chemistry and peroxy radicals (RO2) fate. We encourage future studies to consider both factors, which can vary under different laboratory and ambient conditions, when comparing SOA yields to better understand any differences observed. Our results highlight that multigeneration chemistry and the updated parameters including reaction rate constants and volatility distribution of products should be considered to enable a more comprehensive representation and prediction of SOA formation from NO3 oxidation of isoprene in atmospheric models.

Dataset Information

Nitrate radicals and biogenic volatile organic compounds: oxidation, mechanisms, and organic aerosol.

Publications

Nitrate radicals and biogenic volatile organic compounds: oxidation, mechanisms, and organic aerosol.

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