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Controlled Nitric Oxide Production via O(1D) + N2O Reactions for Use in Oxidation Flow Reactor StudiesOxidation flow reactors that use low-pressure mercury lamps to produce hydroxyl (OH) radicals are an emerging technique for studying the oxidative aging of organic aerosols. Here, ozone (O3) is photolyzed at 254 nm to produce O(1D) radicals, which react with water vapor to produce OH. However, the need to use parts-per-million levels of O3 hinders the ability of oxidation flow reactors to simulate NOx-dependent secondary organic aerosol (SOA) formation pathways. Simple addition of nitric oxide (NO) results in fast conversion of NOx (NO+NO2) to nitric acid (HNO3), making it impossible to sustain NOx at levels that are sufficient to compete with hydroperoxy (HO2) radicals as a sink for organic peroxy (RO2) radicals. We developed a new method that is well suited to the characterization of NOx-dependent SOA formation pathways in oxidation flow reactors. NO and NO2 are produced via the reaction O(1D)+N2O->2NO, followed by the reaction NO+O3->NO2+O2. Laboratory measurements coupled with photochemical model simulations suggest that O(1D)+N2O reactions can be used to systematically vary the relative branching ratio of RO2 +NO reactions relative to RO2 +HO2 and/or RO2+RO2 reactions over a range of conditions relevant to atmospheric SOA formation. We demonstrate proof of concept using high-resolution time-of-flight chemical ionization mass spectrometer (HR-ToF-CIMS) measurements with nitrate (NO-3 ) reagent ion to detect gas-phase oxidation products of isoprene and -pinene previously observed in NOx-influenced environments and in laboratory chamber experiments.
Document ID
20170008764
Acquisition Source
Langley Research Center
Document Type
Reprint (Version printed in journal)
Authors
Lambe, Andrew
(Aerodyne Research, Inc. Billerica, MA, United States)
Massoli, Paola
(Aerodyne Research, Inc. Billerica, MA, United States)
Zhang, Xuan
(Aerodyne Research, Inc. Billerica, MA, United States)
Canagaratna, Manjula
(Aerodyne Research, Inc. Billerica, MA, United States)
Nowak, John
(NASA Langley Research Center Hampton, VA, United States)
Daube, Conner
(Aerodyne Research, Inc. Billerica, MA, United States)
Yan, Chao
(Helsinki Univ. Helsinki, Finland)
Nie, Wei
(Nanjing Univ. China)
Onasch, Timothy
(Aerodyne Research, Inc. Billerica, MA, United States)
Jayne, John
(Aerodyne Research, Inc. Billerica, MA, United States)
Kolb, Charles
(Aerodyne Research, Inc. Billerica, MA, United States)
Davidovits, Paul
(Boston Coll. Chestnut Hill, MA, United States)
Worsnop, Douglas
(Aerodyne Research, Inc. Billerica, MA, United States)
Brune, William
(Pennsylvania State Univ. University Park, PA, United States)
Date Acquired
September 14, 2017
Publication Date
June 22, 2017
Publication Information
Publication: Atmospheric Measurement Techniques
Publisher: Copernicus Publications
Volume: 10
Issue: 6
e-ISSN: 1867-8548
Subject Category
Chemistry And Materials (General)
Report/Patent Number
NF1676L-25951
Funding Number(s)
WBS: WBS 281945.02.39.03.03
Distribution Limits
Public
Copyright
Other

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