气候变化领域集成服务门户(CCPortal): Impact of NOxon secondary organic aerosol (SOA) formation from α-pinene and β-pinene photooxidation: The role of highly oxygenated organic nitrates

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DOI	10.5194/acp-20-10125-2020
	Impact of NOxon secondary organic aerosol (SOA) formation from α-pinene and β-pinene photooxidation: The role of highly oxygenated organic nitrates
	Pullinen I.; Schmitt S.; Kang S.; Sarrafzadeh M.; Schlag P.; Andres S.; Kleist E.; Mentel T.F.; Rohrer F.; Springer M.; Tillmann R.; Wildt J.; Wu C.; Zhao D.; Wahner A.; Kiendler-Scharr A.
发表日期	2020
ISSN	1680-7316
起始页码	10125
结束页码	10147
卷号	20 期号:17
英文摘要	The formation of organic nitrates (ONs) in the gas phase and their impact on mass formation of secondary organic aerosol (SOA) was investigated in a laboratory study for a-pinene and β-pinene photooxidation. Focus was the elucidation of those mechanisms that cause the often observed suppression of SOA mass formation by NOx, and therein the role of highly oxygenated multifunctional molecules (HOMs). We observed that with increasing NOx concentration (a) the portion of HOM organic nitrates (HOM-ONs) increased, (b) the fraction of accretion products (HOM-ACCs) decreased, and (c) HOM-ACCs contained on average smaller carbon numbers. Specifically, we investigated HOM organic nitrates (HOM-ONs), arising from the termination reactions of HOM peroxy radicals with NOx, and HOM permutation products (HOM-PPs), such as ketones, alcohols, or hydroperoxides, formed by other termination reactions. Effective uptake coefficients γeff of HOMs on particles were determined. HOMs with more than six O atoms efficiently condensed on particles (γeff > 0:5 on average), and for HOMs containing more than eight O atoms, every collision led to loss. There was no systematic difference in γeff for HOM-ONs and HOM-PPs arising from the same HOM peroxy radicals. This similarity is attributed to the multifunctional character of the HOMs: as functional groups in HOMs arising from the same precursor HOM peroxy radical are identical, vapor pressures should not strongly depend on the character of the final termination group. As a consequence, the suppressing effect of NOx on SOA formation cannot be simply explained by replacement of terminal functional groups by organic nitrate groups. According to their γeff all HOM-ONs with more than six O atoms will contribute to organic bound nitrate (OrgNO3) in the particulate phase. However, the fraction of OrgNO3 stored in condensable HOMs with molecular masses > 230 Da appeared to be substantially higher than the fraction of particulate OrgNO3 observed by aerosol mass spectrometry. This result suggests losses of OrgNO3 for organic nitrates in particles, probably due to hydrolysis of OrgNO3 that releases HNO3 into the gas phase but leaves behind the organic rest in the particulate phase. However, the loss of HNO3 alone could not explain the observed suppress ing effect of NOx on particle mass formation from a-pinene and β-pinene. Instead we can attribute most of the reduction in SOA mass yields with increasing NOx to the significant suppression of gas phase HOM-ACCs, which have high molecular mass and are potentially important for SOA mass formation at lowNOx conditions. © 2020 Author(s).
语种	英语
scopus关键词	aerosol formation; concentration (composition); nitrate; organic nitrogen compound; oxygenation; photooxidation; terpene
来源期刊	Atmospheric Chemistry and Physics
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/141128
作者单位	Institute for Energy and Climate Research, IEK-8, Forschungszentrum Jülich, Jülich, 52425, Germany; Institute of Bio-and Geosciences, IBG-2, Forschungszentrum Jülich, Jülich, 52425, Germany; Centre for Atmospheric Chemistry, York University, 4700 Keele St., Toronto, ON M3J 1P3, Canada; Department of Applied Physics, University of Eastern Finland, Kuopio, Finland; Tsi GmbH, Aachen, 52068, Germany; PerkinElmer, 501 Rowntree Dairy Rd, Woodbridge, ON L4L 8H1, Canada; Shimadzu Deutschland GmbH, Duisburg, 47269, Germany; Department of Environmental Science, Stockholm University, Stockholm, 11418, Sweden; Dept. of Atmos. and Oceanic Sci., Inst. of Atmos. Sci., Fudan University, Shanghai, 200438, China
推荐引用方式 GB/T 7714	Pullinen I.,Schmitt S.,Kang S.,et al. Impact of NOxon secondary organic aerosol (SOA) formation from α-pinene and β-pinene photooxidation: The role of highly oxygenated organic nitrates[J],2020,20(17).
APA	Pullinen I..,Schmitt S..,Kang S..,Sarrafzadeh M..,Schlag P..,...&Kiendler-Scharr A..(2020).Impact of NOxon secondary organic aerosol (SOA) formation from α-pinene and β-pinene photooxidation: The role of highly oxygenated organic nitrates.Atmospheric Chemistry and Physics,20(17).
MLA	Pullinen I.,et al."Impact of NOxon secondary organic aerosol (SOA) formation from α-pinene and β-pinene photooxidation: The role of highly oxygenated organic nitrates".Atmospheric Chemistry and Physics 20.17(2020).