干旱区生态环境知识资源中心(Arid): Unraveling the Uptake of Glyoxal on a Diversity of Natural Dusts and Surrogates: Linking Dust Composition to Glyoxal Uptake and Estimation of Atmospheric Lifetimes

Arid

DOI	10.1021/acsearthspacechem.3c00359
	Unraveling the Uptake of Glyoxal on a Diversity of Natural Dusts and Surrogates: Linking Dust Composition to Glyoxal Uptake and Estimation of Atmospheric Lifetimes
	Zogka, Antonia G.; Lostier, Anais; Papadimitriou, Vassileios C.; Thevenet, Frederic; Formenti, Paola; Rossi, Michel J.; Chen, Hui; Romanias, Manolis N.
通讯作者	Romanias, MN
来源期刊	ACS EARTH AND SPACE CHEMISTRY
ISSN	2472-3452
出版年	2024
卷号	8 期号:6 页码:1165-1178
英文摘要	The uptake of glyoxal (Gly) on 28 different samples with varying mineralogical origins, such as clays, mineral proxies, and natural dusts from the major arid regions of the Earth, was determined. Experiments were performed at ambient temperature inside a Knudsen flow reactor coupled to a molecular-beam-sampling mass spectrometer. The objective of using a such high number of mineral surfaces (screening approach) was to identify composition-activity relationships (CAR) that link the elemental composition of the mineral samples with the Gly uptake and to evaluate the impact of particle size on Gly uptake. Three parameters were measured to meet these objectives: (i) the initial uptake coefficient (gamma 0), (ii) the quasi-steady-state uptake coefficient (gamma(q-ss)), and (iii) the number of Gly molecules taken up (or uptake quantity, Ns, in molecules cm(-2)). In all of the various investigated Gly-surface systems, Gly uptake was found to be predominantly irreversible. The gamma 0 values measured indicate that Gly is selectively uptaken on surface sites terminated with hydroxyl groups. The abundance of elements, such as Ti, Al, and Ca, was evidenced to play a dominant role in the uptake of Gly on mineral dusts. In particular, the CAR trends observed were: gamma(0) = ( 0.05 +/- 0.02 ) + ( 7.2 +/- 2.0 ) x Ti/Si , gamma(q-ss) = ( 16.7 +/- 2.2 ) x 10(-7) - ( 20.0 +/- 6.5 ) x exp([( - 15 +/- 9 ) x ( Al + Ca ) / Si ]) , where the relative abundance of the elements is expressed in % wt for a constant Gly concentration of 70 ppb. Our results suggest that Gly is taken up on mineral dust particles, and thus, this heterogeneous process can contribute to the formation of secondary organic aerosols (SOA) in the atmosphere. Furthermore, our results reveal the need of composition-activity relationships for atmospheric pollutants that if implemented in atmospheric models will assist in better simulating the atmospheric aging of mineral dust. Finally, the steady-state uptake coefficients of Gly on Gobi natural dust were determined as a function of Gly concentration and results were found to be well represented by the expression gamma(q-ss) = (1.3 +/- 0.4) x 10(-6) + (5.1 +/- 0.2) x 10(-5) [Gly](-(0.85 +/- 0.04)), where [Gly] is expressed in ppb and the uptake coefficients are normalized by the specific surface area of the samples. Under atmospherically relevant Gly concentrations, the uptake coefficient values were in the range 10(-3)-10(-4), and thus its heterogeneous removal on dust particles is expected to be a significant atmospheric loss process for Gly, comparable to or even higher than gas-phase degradation by OH radicals or photolysis.
英文关键词	aging of mineral dust partitioning of oxygenated organics SOA formation VOCs transportation irreversibleuptake of glyoxal modification of mineral dust physicochemicalproperties
类型	Article
语种	英语
收录类别	SCI-E
WOS记录号	WOS:001231819500001
WOS关键词	VOLATILE ORGANIC-COMPOUNDS ; MINERAL DUST ; HETEROGENEOUS INTERACTION ; CALCIUM-CARBONATE ; PARTICLE-SIZE ; ICE SURFACES ; ACETIC-ACID ; LIGHT-DUTY ; GAS-PHASE ; CHEMISTRY
WOS类目	Chemistry, Multidisciplinary ; Geochemistry & Geophysics
WOS研究方向	Chemistry ; Geochemistry & Geophysics
资源类型	期刊论文
条目标识符	http://119.78.100.177/qdio/handle/2XILL650/402584
推荐引用方式 GB/T 7714	Zogka, Antonia G.,Lostier, Anais,Papadimitriou, Vassileios C.,et al. Unraveling the Uptake of Glyoxal on a Diversity of Natural Dusts and Surrogates: Linking Dust Composition to Glyoxal Uptake and Estimation of Atmospheric Lifetimes[J],2024,8(6):1165-1178.
APA	Zogka, Antonia G..,Lostier, Anais.,Papadimitriou, Vassileios C..,Thevenet, Frederic.,Formenti, Paola.,...&Romanias, Manolis N..(2024).Unraveling the Uptake of Glyoxal on a Diversity of Natural Dusts and Surrogates: Linking Dust Composition to Glyoxal Uptake and Estimation of Atmospheric Lifetimes.ACS EARTH AND SPACE CHEMISTRY,8(6),1165-1178.
MLA	Zogka, Antonia G.,et al."Unraveling the Uptake of Glyoxal on a Diversity of Natural Dusts and Surrogates: Linking Dust Composition to Glyoxal Uptake and Estimation of Atmospheric Lifetimes".ACS EARTH AND SPACE CHEMISTRY 8.6(2024):1165-1178.