气候变化领域集成服务门户(CCPortal): Observations and modelling of glyoxal in the tropical Atlantic marine boundary layer

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DOI	10.5194/acp-22-5535-2022
	Observations and modelling of glyoxal in the tropical Atlantic marine boundary layer
	Walker, Hannah; Stone, Daniel; Ingham, Trevor; Hackenberg, Sina; Cryer, Danny; Punjabi, Shalini; Read, Katie; Lee, James; Whalley, Lisa; Spracklen, Dominick, V; Carpenter, Lucy J.; Arnold, Steve R.; Heard, Dwayne E.
发表日期	2022
ISSN	1680-7316
EISSN	1680-7324
起始页码	5535
结束页码	5557
卷号	22 期号:8 页码:23
英文摘要	In situ field measurements of glyoxal at the surface in the tropical marine boundary layer have been made with a temporal resolution of a few minutes during two 4-week campaigns in June-July and August-September 2014 at the Cape Verde Atmospheric Observatory (CVAO; 16 degrees 52' N, 24 degrees 52' W). Using laser-induced phosphorescence spectroscopy with an instrumental detection limit of similar to 1 pptv (1 h averaging), volume mixing ratios up to similar to 10 pptv were observed, with 24 h averaged mixing ratios of 4.9 and 6.3 pptv observed during the first and second campaigns, respectively. Some diel behaviour was observed, but this was not marked. A box model using the detailed Master Chemical Mechanism (version 3.2) and constrained with detailed observations of a suite of species co-measured at the observatory was used to calculate glyoxal mixing ratios. There is a general model underestimation of the glyoxal observations during both campaigns, with mean midday (11:00-13:00) observed-to-modelled ratios for glyoxal of 3.2 and 4.2 for the two campaigns, respectively, and higher ratios at night. A rate of production analysis shows the dominant sources of glyoxal in this environment to be the reactions of OH with glycolaldehyde and acetylene, with a significant contribution from the reaction of OH with the peroxide HC(O)CH2OOH, which itself derives from OH oxidation of acetaldehyde. Increased mixing ratios of acetaldehyde, which is unconstrained and potentially underestimated in the base model, can significantly improve the agreement between the observed and modelled glyoxal during the day. Mean midday observed-to-modelled glyoxal ratios decreased to 1.3 and 1.8 for campaigns 1 and 2, respectively, on constraint to a fixed acetaldehyde mixing ratio of 200 pptv, which is consistent with recent airborne measurements near CVAO. However, a significant model under-prediction remains at night. The model showed limited sensitivity to changes in deposition rates of model intermediates and the uptake of glyoxal onto aerosol compared with sensitivity to uncertainties in chemical precursors. The midday (11:00-13:00) mean modelled glyoxal mixing ratio decreased by factors of 0.87 and 0.90 on doubling the deposition rates of model intermediates and aerosol uptake of glyoxal, respectively, and increased by factors of 1.10 and 1.06 on halving the deposition rates of model intermediates and aerosol uptake of glyoxal, respectively. Although measured levels of monoterpenes at the site (total of similar to 1 pptv) do not significantly influence the model calculated levels of glyoxal, transport of air from a source region with high monoterpene emissions to the site has the potential to give elevated mixing ratios of glyoxal from monoterpene oxidation products, but the values are highly sensitive to the deposition rates of these oxidised intermediates. A source of glyoxal derived from production in the ocean surface organic microlayer cannot be ruled out on the basis of this work and may be significant at night.
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:000787783300001
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/273743
作者单位	University of Leeds; University of Leeds; UK Research & Innovation (UKRI); Natural Environment Research Council (NERC); NERC National Centre for Atmospheric Science; University of Leeds; University of York - UK; UK Research & Innovation (UKRI); Natural Environment Research Council (NERC); NERC National Centre for Atmospheric Science; University of York - UK
推荐引用方式 GB/T 7714	Walker, Hannah,Stone, Daniel,Ingham, Trevor,et al. Observations and modelling of glyoxal in the tropical Atlantic marine boundary layer[J],2022,22(8):23.
APA	Walker, Hannah.,Stone, Daniel.,Ingham, Trevor.,Hackenberg, Sina.,Cryer, Danny.,...&Heard, Dwayne E..(2022).Observations and modelling of glyoxal in the tropical Atlantic marine boundary layer.ATMOSPHERIC CHEMISTRY AND PHYSICS,22(8),23.
MLA	Walker, Hannah,et al."Observations and modelling of glyoxal in the tropical Atlantic marine boundary layer".ATMOSPHERIC CHEMISTRY AND PHYSICS 22.8(2022):23.