期刊
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
卷 113, 期 6, 页码 1516-1521出版社
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1508108113
关键词
particulate organic nitrates; online measurement; lifetime calculation; high-resolution time-of-flight chemical ionization mass spectrometer; biogenic volatile organic compound oxidation
资金
- US Department of Energy Small Business Innovation and Research Program [DE-SC0004577]
- Atmospheric System Research Program [DE-SC0006867, DE-SC0011791]
- National Science Foundation (NSF) CAREER Award [ATM-0846183]
- Swedish Research Council Formas Grant [214-2010-1756]
- Academy of Finland
- National Oceanic and Atmospheric Administration Climate (NOAA)
- Global Change Postdoctoral Fellowship Program
- NSF [AGS-1120076, AGS-1352972, 1242258, 1243354, AGS 1228496, AGS-1250569]
- US Environmental Protection Agency (EPA) STAR Grants [RD-83540301, R835410]
- NOAA [NA13OAR4310063]
- US EPA STAR Research Program [R835400]
- US Department of Energy Atmospheric System Research Program
- EPA STAR Grant [835407]
- Southern Company
- Electric Power Research Institute
- EPA [673401, R835410] Funding Source: Federal RePORTER
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [1404573] Funding Source: National Science Foundation
- Directorate For Geosciences [1352972] Funding Source: National Science Foundation
- Div Atmospheric & Geospace Sciences [1352972] Funding Source: National Science Foundation
- Div Atmospheric & Geospace Sciences
- Directorate For Geosciences [1243354] Funding Source: National Science Foundation
Speciated particle-phase organic nitrates (pONs) were quantified using online chemical ionization MS during June and July of 2013 in rural Alabama as part of the Southern Oxidant and Aerosol Study. A large fraction of pONs is highly functionalized, possessing between six and eight oxygen atoms within each carbon number group, and is not the common first generation alkyl nitrates previously reported. Using calibrations for isoprene hydroxynitrates and the measured molecular compositions, we estimate that pONs account for 3% and 8% of total submicrometer organic aerosol mass, on average, during the day and night, respectively. Each of the isoprene-and monoterpenes-derived groups exhibited a strong diel trend consistent with the emission patterns of likely biogenic hydrocarbon precursors. An observationally constrained diel box model can replicate the observed pON assuming that pONs (i) are produced in the gas phase and rapidly establish gas-particle equilibrium and (ii) have a short particle-phase lifetime (similar to 2-4 h). Such dynamic behavior has significant implications for the production and phase partitioning of pONs, organic aerosol mass, and reactive nitrogen speciation in a forested environment.
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