Volatility of Organic Aerosol: Evaporation of Ammonium Sulfate/Succinic Acid Aqueous Solution Droplets

Condensation and evaporation modify the properties and effects of atmospheric aerosol particles. We studied the evaporation of aqueous succinic acid and succinic acid/ammonium sulfate droplets to obtain insights on the effect of ammonium sulfate on the gas/particle partitioning of atmospheric organic acids. Droplet evaporation in a laminar flow tube was measured in a Tandem Differential Mobility Analyzer setup. A wide range of droplet compositions was investigated, and for some of the experiments the composition was tracked using an Aerosol Mass Spectrometer. The measured evaporation was compared to model predictions where the ammonium sulfate was assumed not to directly affect succinic acid evaporation. The model captured the evaporation rates for droplets with large organic content but overestimated the droplet size change when the molar concentration of succinic acid was similar to or lower than that of ammonium sulfate, suggesting that ammonium sulfate enhances the partitioning of dicarboxylic acids to aqueous particles more than currently expected from simple mixture thermodynamics. If extrapolated to the real atmosphere, these results imply enhanced partitioning of secondary organic compounds to particulate phase in environments dominated by inorganic aerosol.

[1]  A. Zardini,et al.  Atmospheric sugar alcohols: evaporation rates and saturation vapor pressures , 2014 .

[2]  T. Peter,et al.  Vapor pressures of substituted polycarboxylic acids are much lower than previously reported , 2013 .

[3]  A. Laskin,et al.  Tropospheric chemistry of internally mixed sea salt and organic particles: Surprising reactivity of NaCl with weak organic acids , 2012 .

[4]  Douglas R. Worsnop,et al.  The contribution of organics to atmospheric nanoparticle growth , 2012 .

[5]  Julia Laskin,et al.  Formation of nitrogen- and sulfur-containing light-absorbing compounds accelerated by evaporation of water from secondary organic aerosols , 2012 .

[6]  M. Glasius,et al.  Organosulfates and oxidation products from biogenic hydrocarbons in fine aerosols from a forest in North West Europe during spring , 2011 .

[7]  A. Laskin,et al.  Spectroscopic evidence of keto-enol tautomerism in deliquesced malonic acid particles. , 2011, The journal of physical chemistry. A.

[8]  A. Zardini,et al.  The vapor pressures and activities of dicarboxylic acids reconsidered: the impact of the physical state of the aerosol , 2010 .

[9]  B. Turpin,et al.  Aqueous chemistry and its role in secondary organic aerosol (SOA) formation , 2010 .

[10]  R. A. Cox,et al.  Studies of single aerosol particles containing malonic acid, glutaric acid, and their mixtures with sodium chloride. II. Liquid-state vapor pressures of the acids. , 2010, The journal of physical chemistry. A.

[11]  I. Riipinen,et al.  Evaporation of ternary inorganic/organic aqueous droplets: Sodium chloride, succinic acid and water , 2010 .

[12]  R Anthony Cox,et al.  Studies of single aerosol particles containing malonic acid, glutaric acid, and their mixtures with sodium chloride. I. Hygroscopic growth. , 2010, The journal of physical chemistry. A.

[13]  D. R. Worsnop,et al.  Evolution of Organic Aerosols in the Atmosphere , 2009, Science.

[14]  Laura Mitchem,et al.  Comparative thermodynamic studies of aqueous glutaric acid, ammonium sulfate and sodium chloride aerosol at high humidity. , 2008, The journal of physical chemistry. A.

[15]  T. Peter,et al.  A combined particle trap/HTDMA hygroscopicity study of mixed inorganic/organic aerosol particles , 2008 .

[16]  I. Riipinen,et al.  Thermodynamic properties of malonic, succinic, and glutaric acids: evaporation rates and saturation vapor pressures. , 2007, Environmental science & technology.

[17]  A. Goldstein,et al.  Known and Unexplored Organic Constituents in the Earth's Atmosphere , 2007 .

[18]  S. Sjogrena,et al.  Hygroscopic growth and water uptake kinetics of two-phase aerosol particles consisting of ammonium sulfate, adipic and humic acid mixtures , 2007 .

[19]  Birgitta Svenningsson,et al.  A method for determining thermophysical properties of organic material in aqueous solutions: Succinic acid , 2006 .

[20]  Maria Cristina Facchini,et al.  Surface tensions of multi-component mixed inorganic/organic aqueous systems of atmospheric significance: measurements, model predictions and importance for cloud activation predictions , 2006 .

[21]  Katrin Fuhrer,et al.  Field-deployable, high-resolution, time-of-flight aerosol mass spectrometer. , 2006, Analytical chemistry.

[22]  John H Seinfeld,et al.  Thermodynamic models of aqueous solutions containing inorganic electrolytes and dicarboxylic acids at 298.15 K. 2. Systems including dissociation equilibria. , 2006, The journal of physical chemistry. A.

[23]  John H Seinfeld,et al.  Thermodynamic models of aqueous solutions containing inorganic electrolytes and dicarboxylic acids at 298.15 K. 1. The acids as nondissociating components. , 2006, The journal of physical chemistry. A.

[24]  H. Lihavainen,et al.  Surface Tensions and Densities of Oxalic, Malonic, Succinic, Maleic, Malic, and cis-Pinonic Acids , 2006 .

[25]  B. Luo,et al.  Densities of liquid H+/NH4+/SO42-/NO3-/H2O solutions at tropospheric temperatures , 2006 .

[26]  Jens Abildskov,et al.  UNIFAC Parameters for Four New Groups , 2002 .

[27]  C. Chan,et al.  The hygroscopic properties of dicarboxylic and multifunctional acids: measurements and UNIFAC predictions. , 2001, Environmental science & technology.

[28]  Peter Brimblecombe,et al.  Thermodynamic modelling of aqueous aerosols containing electrolytes and dissolved organic compounds , 2001 .

[29]  Hans-Christen Hansson,et al.  Inorganic, organic and macromolecular components of fine aerosol in different areas of Europe in relation to their water solubility , 1999 .

[30]  Peter Brimblecombe,et al.  Thermodynamic Model of the System H+−NH4+−SO42-−NO3-−H2O at Tropospheric Temperatures , 1998 .

[31]  T. Vesala,et al.  Models for condensational growth and evaporation of binary aerosol particles , 1997 .

[32]  Jen‐Ping Chen Theory of deliquescence and modified Köhler curves , 1994 .

[33]  Glen R. Cass,et al.  Quantification of urban organic aerosols at a molecular level: Identification, abundance and seasonal variation , 1993 .

[34]  T. Vesala,et al.  Condensation in the continuum regime , 1991 .

[35]  Aage Fredenslund,et al.  Vapor−Liquid Equilibria by UNIFAC Group Contribution. 6. Revision and Extension , 1979 .

[36]  Aage Fredenslund,et al.  Group‐contribution estimation of activity coefficients in nonideal liquid mixtures , 1975 .

[37]  N. Fuchs,et al.  HIGH-DISPERSED AEROSOLS , 1971 .

[38]  O. Redlich,et al.  Algebraic Representation of Thermodynamic Properties and the Classification of Solutions , 1948 .