气候变化领域集成服务门户(CCPortal): Global simulations of monoterpene-derived peroxy radical fates and the distributions of highly oxygenated organic molecules (HOMs) and accretion products

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DOI	10.5194/acp-22-5477-2022
	Global simulations of monoterpene-derived peroxy radical fates and the distributions of highly oxygenated organic molecules (HOMs) and accretion products
	Xu, Ruochong; Thornton, Joel A.; Lee, Ben H.; Zhang, Yanxu; Jaegle, Lyatt; Lopez-Hilfiker, Felipe D.; Rantala, Pekka; Petaja, Tuukka
发表日期	2022
ISSN	1680-7316
EISSN	1680-7324
起始页码	5477
结束页码	5494
卷号	22 期号:8 页码:18
英文摘要	We evaluate monoterpene-derived peroxy radical (MT-RO2) unimolecular autoxidation and self- and cross-reactions with other RO2 species in the GEOS-Chem global chemical transport model. The formation of associated highly oxygenated organic molecules (HOMs) and accretion products are tracked in competition with other bimolecular reactions. Autoxidation is the dominant fate up to 6-8 km for first-generation MT-RO2, which can undergo unimolecular H shifts. Reaction with NO can be a more common fate for H-shift rate constants < 0.1 s(-1) or at altitudes higher than 8 km due to the imposed Arrhenius temperature dependence of unimolecular H shifts. For MT-derived HOM-RO2, generated by multistep autoxidation of first-generation MT-RO2, reaction with other RO2 species is predicted to be the major fate throughout most of the boreal and tropical forest regions, whereas reaction with NO dominates in the temperate and subtropical forests of the Northern Hemisphere. The newly added reactions result in an approximate 4 % global average decrease in HO2 and RO2, mainly due to faster self-/cross-reactions of MT-RO2, but the impact upon HO2, OH, and NOx abundances is only important in the planetary boundary layer (PBL) over portions of tropical forests. Predicted HOM concentrations in MT-rich regions and seasons can exceed total organic aerosol predicted by the standard version of the GEOS-Chem model depending on the parameters used. Comparisons to observations reveal that large uncertainties remain for key reaction parameters and processes, especially with respect to the photochemical lifetime and volatility of HOMs as well as the rates and branching of associated RO2 accretion products. Further observations and laboratory studies related to MT-RO2-derived HOMs and gas-phase RO2 accretion product formation kinetics - especially their atmospheric fate, such as gas-particle partitioning, multiphase chemistry, and net secondary organic aerosol formation - are needed.
学科领域	Environmental Sciences; Meteorology & Atmospheric Sciences
语种	英语
WOS研究方向	Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences
WOS记录号	WOS:000787242400001
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/273744
作者单位	University of Washington; University of Washington Seattle; Nanjing University; University of Helsinki; Tsinghua University; TOFWERK AG
推荐引用方式 GB/T 7714	Xu, Ruochong,Thornton, Joel A.,Lee, Ben H.,et al. Global simulations of monoterpene-derived peroxy radical fates and the distributions of highly oxygenated organic molecules (HOMs) and accretion products[J],2022,22(8):18.
APA	Xu, Ruochong.,Thornton, Joel A..,Lee, Ben H..,Zhang, Yanxu.,Jaegle, Lyatt.,...&Petaja, Tuukka.(2022).Global simulations of monoterpene-derived peroxy radical fates and the distributions of highly oxygenated organic molecules (HOMs) and accretion products.ATMOSPHERIC CHEMISTRY AND PHYSICS,22(8),18.
MLA	Xu, Ruochong,et al."Global simulations of monoterpene-derived peroxy radical fates and the distributions of highly oxygenated organic molecules (HOMs) and accretion products".ATMOSPHERIC CHEMISTRY AND PHYSICS 22.8(2022):18.