Investigating the evolution of water-soluble organic carbon in evaporating cloud water

Pratap, Vikram; Christiansen, Amy; Carlton, Annmarie G.; Lance, Sara; Casson, P.; Dukett, Jed; Hassan, Hesham; Schwab, James J.; Hennigan, Christopher J.

doi:10.1039/d0ea00005a

Cited by 3 publications

(2 citation statements)

References 82 publications

(169 reference statements)

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“…Aqueous‐phase processing of partitioned organic gases in fogs and clouds have been shown to be a significant contributor to SOA (Ervens, 2015; Herckes et al., 2013; Lamkaddam et al., 2021). Prior work from our group found that a fraction of WSOC dissolved in cloud water evaporated when dried, mimicking the process that occurs during cloud cycling (Pratap et al., 2021). Our present results suggest that ionic strength, pH, and composition of cloud droplets affect the partitioning of WSOC g during cloud cycling.…”

Section: Atmospheric Implicationsmentioning

confidence: 79%

Partitioning of Ambient Organic Gases to Inorganic Salt Solutions: Influence of Salt Identity, Ionic Strength, and pH

Pratap

Carlton

Christiansen

et al. 2021

Geophysical Research Letters

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It is well established that the identity and concentration of inorganic salts play a determining role in organic solubility. For example, in the 19th century, Hofmeister observed a repeatable salt pattern that describes the ability of ions to cause proteins (organic molecules) to "salt in" or "salt out," (Gurau et al., 2004;Kunz et al., 2004) though controlling mechanisms are still debated (Y. Zhang & Cremer, 2006).Despite the ubiquity and importance, accurate quantitative description of the partitioning of atmospheric water-soluble organic gases to liquid water in pre-existing particulate matter remains difficult. Most ambient water-soluble organic gases are not identified at the molecular level. In addition, the salting behavior of only a limited number of atmospherically relevant organic compounds has been studied in the past (Kampf et al., 2013;

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Section: Atmospheric Implicationsmentioning

confidence: 79%

Partitioning of Ambient Organic Gases to Inorganic Salt Solutions: Influence of Salt Identity, Ionic Strength, and pH

Pratap

Carlton

Christiansen

et al. 2021

Geophysical Research Letters

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“…This has been demonstrated for systems such as secondary organic aerosols formed in the presence of reduced nitrogen species undergoing rapid drying and radical chemistry at elevated ionic strength. 11,56,57 We have demonstrated that in the case of the nucleophilic mechanism for BrC formation from glyoxal and ammonia, bulk solutions with the highest feasible concentration of ammonium sulfate and organic content indicate that the nature of the organic content (i.e., functional group composition) has large effects on BrC yields. Kinetic analysis leads us to the conclusion that small changes in equilibria prior to the rate-determining step cause these yield effects.…”

Section: Atmospheric Implicationsmentioning

confidence: 93%

Effects of Organic Matrices on Nucleophilic Aqueous Aerosol Chemistry: Yields and Mechanistic Insight for Brown Carbon Formation from Glyoxal and Ammonia

Drozd

Brown

Karp

2022

ACS Earth Space Chem.

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Climate forcing effects of tropospheric aerosols are determined by their relative abilities to absorb and scatter light and also their effects on cloud properties and lifetime, which may lead to net warming or cooling of the atmosphere. Many details of the formation and lifecycle of organic content that contributes to aerosol light absorption, termed brown carbon (BrC), remain uncertain after extensive study. The reactive species that form BrC make up only a small fraction of total aerosol organic content, and the overwhelming remainder of organic content could greatly influence the rate of BrC formation. One significant route to BrC formation is the reaction of water-soluble carbonyl species to form larger conjugated and/or aromatic compounds, such as the reaction of di-aldehydes (e.g., glyoxal) with reduced nitrogen species (ammonia or amines) to form imidazole derivatives. In this study, we work to further address the complexity of atmospheric aerosols by adding a matrix of organic content to the glyoxal–ammonium system. We find that the addition of a broad range of organic species (alcohols, ketones, organic acids, etc.) to BrC-forming reaction mixtures can both increase and decrease the rate of BrC formation. The rate of BrC formation is shown to vary by more than an order of magnitude depending on the composition of the organic matrix present. UV–vis kinetic measurements and HPLC-ToF-MS product analysis of aqueous solutions with qualities similar to atmospheric aerosols reveal the specific steps in BrC formation affected by the presence of organic content. Our method of systematically adding complexity also proves a useful tool for mechanistic evaluation, and we provide evidence that the proposed cis-di-imine mechanism for the reaction of ammonia and glyoxal is unlikely, with amine species reacting instead.

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Characterization of two aerosol carbon analyzers based on temperature programmed oxidation: TCA08 and FATCAT

Corbin,

Clavel,

Smallwood

2024

Aerosol Science and Technology

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Investigating the evolution of water-soluble organic carbon in evaporating cloud water

Abstract: Cloud cycling plays a key role in the evolution of atmospheric particles and gases, producing secondary aerosol mass and transforming the optical properties and impacts of aerosols globally.

Cited by 3 publications

References 82 publications

Partitioning of Ambient Organic Gases to Inorganic Salt Solutions: Influence of Salt Identity, Ionic Strength, and pH

Partitioning of Ambient Organic Gases to Inorganic Salt Solutions: Influence of Salt Identity, Ionic Strength, and pH

Effects of Organic Matrices on Nucleophilic Aqueous Aerosol Chemistry: Yields and Mechanistic Insight for Brown Carbon Formation from Glyoxal and Ammonia

Characterization of two aerosol carbon analyzers based on temperature programmed oxidation: TCA08 and FATCAT

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