Uptake of SO2 into Sulfuric Acid Droplets through the Oxidation by NO2 under Venus-Analogous Conditions

IF 2.9 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY
Soma Ubukata*, Hiroki Karyu*, Hiromu Nakagawa, Shungo Koyama, Rikuto Minamikawa, Takeshi Kuroda, Naoki Terada and Masao Gen*, 
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Abstract

Sulfur dioxide (SO2) is the primary sulfur-bearing gas on Venus and plays a pivotal role in its atmospheric chemistry. Observations show that SO2 concentration decreases by 3 orders of magnitude from the bottom to the top of the cloud layers. However, this SO2 depletion cannot be explained by gas-phase chemistry alone, suggesting a missing SO2 sink within the cloud layers. Here, we show for the first time that SO2 uptake and subsequent oxidation within droplets could serve as an additional sink in the Venusian cloud layers. We performed laboratory experiments to examine the uptake of SO2 by sulfuric acid (H2SO4) droplets of ∼10 μm in the presence of nitrogen dioxide (NO2) as an oxidant. We find that the size growth of H2SO4 droplets occurs only when both SO2 and NO2 are present, indicating the SO2 oxidation by NO2 in H2SO4 droplets. The growth rate increases with NO2 concentration, and the reactive uptake coefficient of SO2, γSO2, is parameterized by the number density of NO2 (cm–3), nNO2, as log10γSO2 = 0.572 × log10nNO2 – 15.03. Numerical simulations suggest that γSO2= 10–7 is required to reproduce the observed SO2 concentration at the top of the cloud layer. Our results underscore that the reactive uptake of SO2 by H2SO4 droplets may play an important role in SO2 depletion in the cloud layers, warranting future observations of oxidants in the Venusian atmosphere.

金星模拟条件下NO2氧化作用下硫酸液滴对SO2的吸收
二氧化硫(SO2)是金星上主要的含硫气体,在金星的大气化学中起着关键作用。观测结果表明,从云层底部到云层顶部,SO2浓度降低了3个数量级。然而,这种二氧化硫的消耗不能仅仅用气相化学来解释,这表明在云层中缺失了二氧化硫的吸收。在这里,我们首次表明SO2的吸收和随后在液滴内的氧化可以作为金星云层中的额外汇。我们进行了实验室实验,研究了在二氧化氮(NO2)作为氧化剂存在的情况下,10 μm的硫酸(H2SO4)液滴对SO2的吸收。我们发现,只有在SO2和NO2同时存在的情况下,H2SO4液滴的尺寸才会增长,这表明SO2在H2SO4液滴中被NO2氧化。随着NO2浓度的增加,SO2的活性吸收系数γSO2由NO2的数量密度(cm-3), nNO2表示为log10γSO2 = 0.572 × log10nNO2 - 15.03。数值模拟表明,γSO2= 10-7才能重现观测到的云顶SO2浓度。我们的研究结果强调H2SO4液滴对SO2的反应性吸收可能在云层中SO2的消耗中起重要作用,这为未来对金星大气中氧化剂的观测提供了依据。
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来源期刊
ACS Earth and Space Chemistry
ACS Earth and Space Chemistry Earth and Planetary Sciences-Geochemistry and Petrology
CiteScore
5.30
自引率
11.80%
发文量
249
期刊介绍: The scope of ACS Earth and Space Chemistry includes the application of analytical, experimental and theoretical chemistry to investigate research questions relevant to the Earth and Space. The journal encompasses the highly interdisciplinary nature of research in this area, while emphasizing chemistry and chemical research tools as the unifying theme. The journal publishes broadly in the domains of high- and low-temperature geochemistry, atmospheric chemistry, marine chemistry, planetary chemistry, astrochemistry, and analytical geochemistry. ACS Earth and Space Chemistry publishes Articles, Letters, Reviews, and Features to provide flexible formats to readily communicate all aspects of research in these fields.
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