Reactive uptake of ammonia to secondary organic aerosols: kinetics of organonitrogen formation

CORC > 生态环境研究中心 > 中国科学院生态环境研究中心 > 环境化学与生态毒理学国家重点实验室

	Reactive uptake of ammonia to secondary organic aerosols: kinetics of organonitrogen formation
	Liu, Y.; Liggio, J.; Staebler, R.; Li, S. -M.
刊名	ATMOSPHERIC CHEMISTRY AND PHYSICS
	2015
卷号	15 期号:23 页码:13569-13584
英文摘要	As a class of brown carbon, organonitrogen compounds originating from the heterogeneous uptake of NH3 by secondary organic aerosol (SOA) have received significant attention recently. In the current work, particulate organonitrogen formation during the ozonolysis of alpha-pinene and the OH oxidation of m-xylene in the presence of ammonia (34-125 ppb) was studied in a smog chamber equipped with a high resolution time-of-flight aerosol mass spectrometer and a quantum cascade laser instrument. A large diversity of nitrogen-containing organic (NOC) fragments was observed which were consistent with the reactions between ammonia and carbonyl-containing SOA. Ammonia uptake coefficients onto SOA which led to organonitrogen compounds were reported for the first time, and were in the range of similar to 10(-3)-10(-2), decreasing significantly to <10(-5) after 6 h of reaction. At the end of experiments (similar to 6 h) the NOC mass contributed 8.9 +/- 1.7 and 31.5 +/- 4.4 wt% to the total alpha-pineneand m-xylene-derived SOA, respectively, and 4-15 wt% of the total nitrogen in the system. Uptake coefficients were also found to be positively correlated with particle acidity and negatively correlated with NH3 concentration, indicating that heterogeneous reactions were responsible for the observed NOC mass, possibly limited by liquid phase diffusion. Under these conditions, the data also indicate that the formation of NOC can compete kinetically with inorganic acid neutralization. The formation of NOC in this study suggests that a significant portion of the ambient particle associated N may be derived from NH3 heterogeneous reactions with SOA. NOC from such a mechanism may be an important and unaccounted for source of PM associated nitrogen. This mechanism may also contribute to the medium or long-range transport and wet/dry deposition of atmospheric nitrogen.
研究领域[WOS]	Meteorology & Atmospheric Sciences
WOS记录号	WOS:000367189600017
公开日期	2016-03-15
内容类型	期刊论文
源URL	[http://ir.rcees.ac.cn/handle/311016/32654]
专题	生态环境研究中心_环境化学与生态毒理学国家重点实验室
推荐引用方式 GB/T 7714	Liu, Y.,Liggio, J.,Staebler, R.,et al. Reactive uptake of ammonia to secondary organic aerosols: kinetics of organonitrogen formation[J]. ATMOSPHERIC CHEMISTRY AND PHYSICS,2015,15(23):13569-13584.
APA	Liu, Y.,Liggio, J.,Staebler, R.,&Li, S. -M..(2015).Reactive uptake of ammonia to secondary organic aerosols: kinetics of organonitrogen formation.ATMOSPHERIC CHEMISTRY AND PHYSICS,15(23),13569-13584.
MLA	Liu, Y.,et al."Reactive uptake of ammonia to secondary organic aerosols: kinetics of organonitrogen formation".ATMOSPHERIC CHEMISTRY AND PHYSICS 15.23(2015):13569-13584.