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Title: Controlled nitric oxide production via O(1D) + N2O reactions for use in oxidation flow reactor studies

Abstract

Oxidation 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) measurementsmore » with nitrate (NO3−) reagent ion to detect gas-phase oxidation products of isoprene and α-pinene previously observed in NOx-influenced environments and in laboratory chamber experiments.« less

Authors:
; ; ORCiD logo; ; ORCiD logo; ; ORCiD logo; ; ORCiD logo; ; ORCiD logo; ; ;
Publication Date:
Research Org.:
Boston College, Chestnut Hill, MA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER); National Science Foundation (NSF)
OSTI Identifier:
1365443
Alternate Identifier(s):
OSTI ID: 1425615
Grant/Contract Number:  
SC0006980; SC0011935; AGS-1536939; AGS-1537446; AGS-1537009
Resource Type:
Published Article
Journal Name:
Atmospheric Measurement Techniques (Online)
Additional Journal Information:
Journal Name: Atmospheric Measurement Techniques (Online) Journal Volume: 10 Journal Issue: 6; Journal ID: ISSN 1867-8548
Publisher:
Copernicus Publications, EGU
Country of Publication:
Germany
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Lambe, Andrew, Massoli, Paola, Zhang, Xuan, Canagaratna, Manjula, Nowak, John, Daube, Conner, Yan, Chao, Nie, Wei, Onasch, Timothy, Jayne, John, Kolb, Charles, Davidovits, Paul, Worsnop, Douglas, and Brune, William. Controlled nitric oxide production via O(1D) + N2O reactions for use in oxidation flow reactor studies. Germany: N. p., 2017. Web. doi:10.5194/amt-10-2283-2017.
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Lambe, Andrew, Massoli, Paola, Zhang, Xuan, Canagaratna, Manjula, Nowak, John, Daube, Conner, Yan, Chao, Nie, Wei, Onasch, Timothy, Jayne, John, Kolb, Charles, Davidovits, Paul, Worsnop, Douglas, & Brune, William. Controlled nitric oxide production via O(1D) + N2O reactions for use in oxidation flow reactor studies. Germany. https://doi.org/10.5194/amt-10-2283-2017
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Lambe, Andrew, Massoli, Paola, Zhang, Xuan, Canagaratna, Manjula, Nowak, John, Daube, Conner, Yan, Chao, Nie, Wei, Onasch, Timothy, Jayne, John, Kolb, Charles, Davidovits, Paul, Worsnop, Douglas, and Brune, William. Thu . "Controlled nitric oxide production via O(1D) + N2O reactions for use in oxidation flow reactor studies". Germany. https://doi.org/10.5194/amt-10-2283-2017.
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@article{osti_1365443,
title = {Controlled nitric oxide production via O(1D) + N2O reactions for use in oxidation flow reactor studies},
author = {Lambe, Andrew and Massoli, Paola and Zhang, Xuan and Canagaratna, Manjula and Nowak, John and Daube, Conner and Yan, Chao and Nie, Wei and Onasch, Timothy and Jayne, John and Kolb, Charles and Davidovits, Paul and Worsnop, Douglas and Brune, William},
abstractNote = {Oxidation 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 (NO3−) reagent ion to detect gas-phase oxidation products of isoprene and α-pinene previously observed in NOx-influenced environments and in laboratory chamber experiments.},
doi = {10.5194/amt-10-2283-2017},
journal = {Atmospheric Measurement Techniques (Online)},
number = 6,
volume = 10,
place = {Germany},
year = {Thu Jun 22 00:00:00 EDT 2017},
month = {Thu Jun 22 00:00:00 EDT 2017}
}
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https://doi.org/10.5194/amt-10-2283-2017
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