4.8 Article

Highly Oxygenated Organic Nitrates Formed from NO3 Radical-Initiated Oxidation of β-Pinene

Journal

ENVIRONMENTAL SCIENCE & TECHNOLOGY
Volume 55, Issue 23, Pages 15658-15671

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.est.1c03978

Keywords

NO3 radical; biogenic volatile organic compounds; organic nitrate; secondary organic aerosol; anthropogenic-biogenic interaction; night-time oxidation

Funding

  1. National Natural Science Foundation of China [41875145]
  2. Science and Technology Commission of Shanghai Municipality [20230711400]

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The study investigated the formation of gas-phase highly oxygenated organic molecules-organic nitrates (HOM-ON) from NO3-initiated oxidation of beta-pinene in the SAPHIR chamber. Results showed a mean molar yield of HOM-ON at 4.8%, with significant contributions to SOA formation, highlighting the importance of carbonylnitrates in the process.
The reactions of biogenic volatile organic compounds (BVOC) with the nitrate radicals (NO3) are major nighttime sources of organic nitrates and secondary organic aerosols (SOA) in regions influenced by BVOC and anthropogenic emissions. In this study, the formation of gas-phase highly oxygenated organic molecules-organic nitrates (HOM-ON) from NO3-initiated oxidation of a representative monoterpene, beta-pinene, was investigated in the SAPHIR chamber (Simulation of Atmosphere PHotochemistry In a large Reaction chamber). Six monomer (C = 7-10, N = 1-2, O = 6-16) and five accretion product (C = 17-20, N = 2-4, O = 9-22) families were identified and further classified into first- or second-generation products based on their temporal behavior. The time lag observed in the peak concentrations between peroxy radicals containing odd and even number of oxygen atoms, as well as between radicals and their corresponding termination products, provided constraints on the HOM-ON formation mechanism. The HOM-ON formation can be explained by unimolecular or bimolecular reactions of peroxy radicals. A dominant portion of carbonylnitrates in HOM-ON was detected, highlighting the significance of unimolecular termination reactions by intramolecular H-shift for the formation of HOM-ON. A mean molar yield of HOM-ON was estimated to be 4.8% (-2.6%/+5.6%), suggesting significant HOM-ON contributions to the SOA formation.

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