Aqueous phase sulfate production in clouds in eastern China

Shen, Xinhua; Lee, Taehyoung; Guo, Jia; Wang, Xinfeng; Li, Penghui; Xu, Ping; Wang, Yan; Ren, Yu; Wang, Wenxing; Wang, Tao; Li, Yang; Carn, S. A.; Collett, Jeffrey L.

doi:10.1016/j.atmosenv.2012.07.079

Cited by 92 publications

(106 citation statements)

References 55 publications

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“…Hydrogen peroxide plays a central role in various important chemical processes in clouds. First, H 2 O 2 is considered the most important oxidant for the conversion of sulfite to sulfate for pH lower than 5.5, thereby contributing significantly to the acidification of clouds and precipitations (Deguillaume et al, 2005;Shen et al, 2012). Second, the photolysis of H 2 O 2 will lead to an efficient production of the hydroxyl radical HO q (Arakaki et al, 2013), and recent studies have shown that this can be a dominant aqueous source (Bianco et al, 2015).…”

Section: Introductionmentioning

confidence: 99%

H2O2 modulates the energetic metabolism of the cloud microbiome

et al. 2017

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Abstract. Chemical reactions in clouds lead to oxidation processes driven by radicals (mainly HO q , NO q 3 , or HO q 2 ) or strong oxidants such as H 2 O 2 , O 3 , nitrate, and nitrite. Among those species, hydrogen peroxide plays a central role in the cloud chemistry by driving its oxidant capacity. In cloud droplets, H 2 O 2 is transformed by microorganisms which are metabolically active. Biological activity can therefore impact the cloud oxidant capacity. The present article aims at highlighting the interactions between H 2 O 2 and microorganisms within the cloud system.First, experiments were performed with selected strains studied as a reference isolated from clouds in microcosms designed to mimic the cloud chemical composition, including the presence of light and iron. Biotic and abiotic degradation rates of H 2 O 2 were measured and results showed that biodegradation was the most efficient process together with the photo-Fenton process. H 2 O 2 strongly impacted the microbial energetic state as shown by adenosine triphosphate (ATP) measurements in the presence and absence of H 2 O 2 . This ATP depletion was not due to the loss of cell viability. Secondly, correlation studies were performed based on real cloud measurements from 37 cloud samples collected at the PUY station (1465 m a.s.l., France). The results support a strong correlation between ATP and H 2 O 2 concentrations and confirm that H 2 O 2 modulates the energetic metabolism of the cloud microbiome. The modulation of microbial metabolism by H 2 O 2 concentration could thus impact cloud chemistry, in particular the biotransformation rates of carbon compounds, and consequently can perturb the way the cloud system is modifying the global atmospheric chemistry.

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Section: Introductionmentioning

confidence: 99%

H2O2 modulates the energetic metabolism of the cloud microbiome

et al. 2017

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“…5). Meteorological back-trajectories indicate the same source region (the heavily populated, industrial South China Plain) for air masses involved in all cloud samples (Shen, 2011). Because it is difficult to both collect and to fully and continuously speciate cloud water, many studies use simple surrogate cloud water solutions to better constrain yields and reaction pathways, impeding direct comparison of our findings to the literature.…”

Section: Discussionmentioning

confidence: 97%

“…The resulting [OH] aq was quantified in the cloud samples (and deionized water for comparison purposes) via absorption spectroscopy of 202 nm light by salicylic acid, which was below detection limit in the cloud samples, preceded by reverse phase liquid chromatography separation to prevent measurement interference from other absorbing species (N = 3; accounting for salicylic acid direct photolysis and using the secondorder rate constant of 1.6 × 10 10 M -1 s -1 ; see Boris et al, 2014); these measurements yielded 1.9 × 10 −14 M OH within the cloud water and 5.4 ± 0.5 × 10 −14 M OH within pure water (Boris et al, 2014). Before hydrogen peroxide addition, these ambient cloud samples contained [HOOH] aq = 1-100 µM (Shen, 2011) (Jacob, 1986;Arakaki and Faust, 1998;Ervens et al, 2003b;Deguillaume et al, 2005;Ervens and Volkamer, 2010), 1-2 orders of magnitude lower than used in similar laboratory experiments (Lim et al, 2010;Lee et al, 2011a). These solutions are among the most atmospherically relevant used in the laboratory to date; methodological assessment of evaporative cycling effects and OH exposure is discussed further in supplement Section S4.…”

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confidence: 99%

Aqueous Secondary Organic Aerosol Formation in Ambient Cloud Water Photo-Oxidations

Schurman

Boris

Desyaterik

et al. 2018

Aerosol Air Qual. Res.

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The current understanding of aqueous secondary organic aerosol (aqSOA) formation is based largely on laboratory investigations of very simple surrogate cloud water solutions that aid mechanistic understanding of aqueous oxidation but may not accurately reflect the influence of the complex ambient matrix present in authentic cloud waters on organic chemistry. In this study, unaltered ambient cloud water and 'biogenically influenced' ambient cloud water (with added pinonic acid) were photo-oxidized, atomized, and dried to simulate the formation of aqSOA in clouds, then analyzed using an Aerodyne Aerosol Mass Spectrometer. Two major chemical regimes were identified: in the first, particle organic mass is gained, then lost; sustained increases in highly oxidized fragments indicate overall organic acid formation, while increases in nominally volatile fragments suggest that evaporation may contribute to the observed mass decrease. In the second regime, the oxidation level of cloud water organic matter decreases as mass decreases, suggesting that oxidized functional groups are fragmented and lost to evaporation. Overall, the rate of aqSOA production in unaltered cloud water decreases as oxygenation increases, until organic mass loss beginning at consistent values of f44 > 0.23 ± 0.05 and O:C > 0.61 ± 0.05. We hypothesize that there may be a parameterizable 'maximum oxidation level' for cloud water above which functional group fragmentation is dominant. These experiments are among the first to quantify organic mass production in ambient cloud water and employ the most atmospherically relevant oxidant concentrations to date.

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“…The secondary inorganic species (nitrate, sulfate and ammonium) appeared to rapidly increase because the atmospheric environment exists at a high RH, and the aqueous-phase oxidation is much faster than gas-phase oxidation processes (Seinfeld and Pandis, 2006). The oxidation state in the aqueous-phase relies on droplet pH and mass concentrations of oxidants (Shen et al, 2012). Similar to NR-PM 1 species, the OA components presented synchronous enhancements at high RH levels, especially the OOA, which accounted for 36% of OA and showed the largest enhancement (from 3.5 µg m -3 increased to 8.9 µg m -3 ).…”

Section: Relative Humidity (Rh) Effects On Chemical Componentsmentioning

confidence: 89%

Evaluating the Effects of Springtime Dust Storms over Beijing and the Associated Characteristics of Sub-Micron Aerosol

Zhang

et al. 2017

Aerosol Air Qual. Res.

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In order to understand the characteristics, sources and processes of non-refractory submicron particles (NR-PM 1 ), an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was deployed to acquire observational data during the spring (April 1 to 30) in Beijing, China, in 2012. Based on PM 10 , PM 2.5 and NR-PM 1 mass concentrations observation, satellite images and the back trajectory analysis, one haze and dust storm episodes were recorded during the campaign, in addition, one clean episodes was also added to the comparison as a reference. The NR-PM 1 mass concentration was 97 µg m -3 during the haze episodes, while it was approximately 12 times and 1.7 times that on the clean and dust episodes, respectively. In addition, the secondary inorganic aerosol (sulfate, nitrate and ammonium) contributed the largest fraction of NR-PM 1 (69%) during the haze episodes. The dust storms originated from the northwestern caused the PM 10 peaking at 826 µg m ) and OOA (6 µg m -3 ). The backward trajectory clustering analysis indicated the air mass from the southeast (at a frequency more than 30%) contained the higher NR-PM 1 concentration (more than 80 µg m -3 ) corresponding to the higher sulfate, nitrate and ammonium contributions.

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Aqueous phase sulfate production in clouds in eastern China

Cited by 92 publications

References 55 publications

H<sub>2</sub>O<sub>2</sub> modulates the energetic metabolism of the cloud microbiome

H<sub>2</sub>O<sub>2</sub> modulates the energetic metabolism of the cloud microbiome

Aqueous Secondary Organic Aerosol Formation in Ambient Cloud Water Photo-Oxidations

Evaluating the Effects of Springtime Dust Storms over Beijing and the Associated Characteristics of Sub-Micron Aerosol

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Aqueous phase sulfate production in clouds in eastern China

Cited by 92 publications

References 55 publications

H&lt;sub&gt;2&lt;/sub&gt;O&lt;sub&gt;2&lt;/sub&gt; modulates the energetic metabolism of the cloud microbiome

H&lt;sub&gt;2&lt;/sub&gt;O&lt;sub&gt;2&lt;/sub&gt; modulates the energetic metabolism of the cloud microbiome

Aqueous Secondary Organic Aerosol Formation in Ambient Cloud Water Photo-Oxidations

Evaluating the Effects of Springtime Dust Storms over Beijing and the Associated Characteristics of Sub-Micron Aerosol

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H<sub>2</sub>O<sub>2</sub> modulates the energetic metabolism of the cloud microbiome

H<sub>2</sub>O<sub>2</sub> modulates the energetic metabolism of the cloud microbiome