气候变化领域集成服务门户(CCPortal): Using GECKO-A to derive mechanistic understanding of secondary organic aerosol formation from the ubiquitous but understudied camphene

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DOI	10.5194/acp-21-11467-2021
	Using GECKO-A to derive mechanistic understanding of secondary organic aerosol formation from the ubiquitous but understudied camphene
	Afreh I.K.; Aumont B.; Camredon M.; Barsanti K.C.
发表日期	2021
ISSN	1680-7316
起始页码	11467
结束页码	11487
卷号	21 期号:14
英文摘要	Camphene, a dominant monoterpene emitted from both biogenic and pyrogenic sources, has been significantly understudied, particularly in regard to secondary organic aerosol (SOA) formation. When camphene represents a significant fraction of emissions, the lack of model parameterizations for camphene can result in inadequate representation of gas-phase chemistry and underprediction of SOA formation. In this work, the first mechanistic study of SOA formation from camphene was performed using the Generator for Explicit Chemistry and Kinetics of Organics in the Atmosphere (GECKO-A). GECKO-A was used to generate gas-phase chemical mechanisms for camphene and two well-studied monoterpenes, α-pinene and limonene, as well as to predict SOA mass formation and composition based on gas/particle partitioning theory. The model simulations represented observed trends in published gas-phase reaction pathways and SOA yields well under chamber-relevant photooxidation and dark ozonolysis conditions. For photooxidation conditions, 70ĝ€¯% of the simulated α-pinene oxidation products remained in the gas phase compared to 50ĝ€¯% for limonene, supporting model predictions and observations of limonene having higher SOA yields than α-pinene under equivalent conditions. The top 10 simulated particle-phase products in the α-pinene and limonene simulations represented 37ĝ€¯%-50ĝ€¯% of the SOA mass formed and 6ĝ€¯%-27ĝ€¯% of the hydrocarbon mass reacted. To facilitate comparison of camphene with α-pinene and limonene, model simulations were run under idealized atmospheric conditions, wherein the gas-phase oxidant levels were controlled, and peroxy radicals reacted equally with HO2 and NO. Metrics for comparison included gas-phase reactivity profiles, time-evolution of SOA mass and yields, and physicochemical property distributions of gas- and particle-phase products. The controlled-reactivity simulations demonstrated that (1) in the early stages of oxidation, camphene is predicted to form very low-volatility products, lower than α-pinene and limonene, which condense at low mass loadings; and (2) the final simulated SOA yield for camphene (46ĝ€¯%) was relatively high, in between α-pinene (25ĝ€¯%) and limonene (74ĝ€¯%). A 50ĝ€¯% α-pineneĝ€¯+ĝ€¯50ĝ€¯% limonene mixture was then used as a surrogate to represent SOA formation from camphene; while simulated SOA mass and yield were well represented, the volatility distribution of the particle-phase products was not. To demonstrate the potential importance of including a parameterized representation of SOA formation by camphene in air quality models, SOA mass and yield were predicted for three wildland fire fuels based on measured monoterpene distributions and published SOA parameterizations for α-pinene and limonene. Using the 50/50 surrogate mixture to represent camphene increased predicted SOA mass by 43ĝ€¯%-50ĝ€¯% for black spruce and by 56ĝ€¯%-108ĝ€¯% for Douglas fir. This first detailed modeling study of the gas-phase oxidation of camphene and subsequent SOA formation highlights opportunities for future measurement-model comparisons and lays a foundation for developing chemical mechanisms and SOA parameterizations for camphene that are suitable for air quality modeling. © 2021 Atmospheric Chemistry and Physics. All rights reserved.
语种	英语
scopus关键词	aerosol composition; aerosol formation; atmospheric chemistry; chemical composition; model validation; numerical model; parameterization; radical; trace element; Picea mariana; Pseudotsuga; Pseudotsuga menziesii
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/246694
作者单位	Dept. of Chem. and Environ. Eng. and Coll. of Eng.-Center for Environmental Research and Technology, University of California-Riverside, Riverside, CA 92507, United States; Université Paris Est Creteil and Université de Paris, CNRS, LISA, Créteil, 94010, France
推荐引用方式 GB/T 7714	Afreh I.K.,Aumont B.,Camredon M.,et al. Using GECKO-A to derive mechanistic understanding of secondary organic aerosol formation from the ubiquitous but understudied camphene[J],2021,21(14).
APA	Afreh I.K.,Aumont B.,Camredon M.,&Barsanti K.C..(2021).Using GECKO-A to derive mechanistic understanding of secondary organic aerosol formation from the ubiquitous but understudied camphene.ATMOSPHERIC CHEMISTRY AND PHYSICS,21(14).
MLA	Afreh I.K.,et al."Using GECKO-A to derive mechanistic understanding of secondary organic aerosol formation from the ubiquitous but understudied camphene".ATMOSPHERIC CHEMISTRY AND PHYSICS 21.14(2021).