Images reveal that atmospheric particles can undergo liquid-liquid phase separations

Proceedings of the National Academy of Sciences of the United States of America

Volumn 109, Issue 33, 2012, Pages 13188-13193

  You, Yuan ^a   Renbaum Wolff, Lindsay ^a   Carreras Sospedra, Marc ^b   Hanna, Sarah J ^a   Hiranuma, Naruki ^c   Kamal, Saeid ^a   Smith, Mackenzie L ^d   Zhang, Xiaolu ^e   Weber, Rodney J ^e   Shilling, John E ^f   Dabdub, Donald ^b   Martin, Scot T ^d,g   Bertram, Allan K ^a  

^a UNIVERSITY OF BRITISH COLUMBIA   (Canada)

^b University of California at Irvine   (United States)

^c KARLSRUHE INSTITUTE OF TECHNOLOGY   (Germany)

^d HARVARD UNIVERSITY   (United States)

^e GEORGIA INSTITUTE OF TECHNOLOGY   (United States)

^f PACIFIC NORTHWEST NATIONAL LABORATORY   (United States)

^g HARVARD UNIVERSITY   (United States)

Author keywords

Ambient aerosol; Atmospheric chemistry; Chemistry; Physical state; Secondary organic aerosol

Indexed keywords

DINITROGEN PENTOXIDE; NITRATE; ORGANIC COMPOUND;

AEROSOL; ARTICLE; ATMOSPHERE; CRYSTALLIZATION; FLUORESCENCE MICROSCOPY; LIQUID LIQUID PHASE SEPARATION; MICROSCOPY; PHASE SEPARATION; PRIORITY JOURNAL; SIMULATION; UNITED STATES; URBAN AREA;

EID: 84865165579     PISSN: 00278424     EISSN: 10916490     Source Type: Journal    
DOI: 10.1073/pnas.1206414109     Document Type: Article

References (43)

1. Murphy DM, et al. (2006) Single-particle mass spectrometry of tropospheric aerosol particles. J Geophys Res 111:D23S32.
2. Pratt KA, Prather KA (2010) Aircraft measurements of vertical profiles of aerosol mixing states. J Geophys Res Atmos 115:D11305.
3. Seinfeld JH, Pandis SN (2006) Atmospheric Chemistry and Physics (Wiley Interscience, Hoboken, NJ).
4. Finlayson-Pitts BJ, Pitts JN (2000) Chemistry of the Upper and Lower Atmosphere: Theory, Experiments and Applications (Academic, San Diego, London).
5. Hallquist M, et al. (2009) The formation, properties and impact of secondary organic aerosol: Current and emerging issues. Atmos Chem Phys 9:5155-5236.
6. Zuend A, Marcolli C, Peter T, Seinfeld JH (2010) Computation of liquid-liquid equilibria and phase stabilities: Implications for RH-dependent gas/particle partitioning of organic-inorganic aerosols. Atmos Chem Phys 10:7795-7820.
7. Chang EI, Pankow JF (2006) Prediction of activity coefficients in liquid aerosol particles containing organic compounds, dissolved inorganic salts, and water - Part 2: Consideration of phase separation effects by an X-UNIFAC model. Atmos Environ 40:6422-6436. (Pubitemid 44332996)
8. Martin ST (2000) Phase transitions of aqueous atmospheric particles. Chem Rev 100:3403-3454.
9. Pankow JF (2003) Gas/particle partitioning of neutral and ionizing compounds to single and multi-phase aerosol particles. 1. Unified modeling framework. Atmos Environ 37:3323-3333.
10. Marcolli C, Krieger UK (2006) Phase changes during hygroscopic cycles of mixed organic/ inorganic model systems of tropospheric aerosols. J Phys Chem A 110:1881-1893. (Pubitemid 43343006)
11. Buajarern J, Mitchem L, Reid JP (2007) Characterizing multiphase organic/inorganic/ aqueous aerosol droplets. J Phys Chem A 111:9054-9061. (Pubitemid 47522557)
12. Clegg SL, Seinfeld JH, Brimblecombe P (2001) Thermodynamic modelling of aqueous aerosols containing electrolytes and dissolved organic compounds. J Aerosol Sci 32:713-738. (Pubitemid 32401578)
13. Bertram AK, et al. (2011) Predicting the relative humidities of liquid-liquid phase separation, efflorescence, and deliquescence of mixed particles of ammonium sulfate, organic material, and water using the organic-to-sulfate mass ratio of the particle and the oxygen-to-carbon elemental ratio of the organic component. Atmos Chem Phys 11:10995-11006.
14. Ciobanu VG, Marcolli C, Krieger UK, Weers U, Peter T (2009) Liquid-liquid phase separation in mixed organic/inorganic aerosol particles. J Phys ChemA 113:10966-10978.
15. Erdakos GB, Asher WE, Seinfeld JH, Pankow JF (2006) Prediction of activity coefficients in liquid aerosol particles containing organic compounds, dissolved inorganic salts, and water - Part 1: Organic compounds and water by consideration of short- and long-range effects using X-UNIFAC.1. Atmos Environ 40:6410-6421. (Pubitemid 44332995)
16. Song M, et al. (2012) Liquid-liquid phase separation and morphology of internally mixed dicarboxylic acids/ammonium sulfate/water particles. Atmos Chem Phys 12:2691-2712.
17. Anttila T, Kiendler-Scharr A, Mentel TF, Tillmann R (2007) Size dependent partitioning of organic material: Evidence for the formation of organic coatings on aqueous aerosols. J Atmos Chem 57:215-237. (Pubitemid 47036959)
18. Smith ML, Kuwata M, Martin ST (2011) Secondary organic material produced by the dark ozonolysis of alpha-pinene minimally affects the deliquescence and efflorescence of ammonium sulfate. Aerosol Sci Technol 45:225-242.
19. Prisle NL, Engelhart GJ, Bilde M, Donahue NM (2010) Humidity influence on gasparticle phase partitioning of alpha-pinene + O(3) secondary organic aerosol. Geophys Res Lett 37:L01802.
20. Zuend A, Seinfeld JH (2012) Modeling the gas-particle partitioning of secondary organic aerosol: The importance of liquid-liquid phase separation. Atmos Chem Phys Discuss 12:2199-2258.
21. Odum JR, Jungkamp TP, Griffin RJ, Flagan RC, Seinfeld JH (1997) The atmospheric aerosol-forming potential of whole gasoline vapor. Science 276:96-99.
22. Reinhardt A, et al. (2007) Ultrahigh mass resolution and accurate mass measurements as a tool to characterize oligomers in secondary organic aerosols. Anal Chem 79:4074-4082. (Pubitemid 46903156)
23. Ng NL, et al. (2010) Organic aerosol components observed in Northern Hemispheric datasets from Aerosol Mass Spectrometry. Atmos Chem Phys 10:4625-4641.
24. Jimenez JL, et al. (2009) Evolution of organic aerosols in the atmosphere. Science 326:1525-1529.
25. Zhang Q, et al. (2007) Ubiquity and dominance of oxygenated species in organic aerosols in anthropogenically-influenced Northern Hemisphere midlatitudes. Geophys Res Lett 34:L13801.
26. Pant A, Parsons MT, Bertram AK (2006) Crystallization of aqueous ammonium sulfate particles internally mixed with soot and kaolinite: Crystallization relative humidities and nucleation rates. J Phys Chem A 110:8701-8709. (Pubitemid 44187370)
27. Bodsworth A, Zobrist B, Bertram AK (2010) Inhibition of efflorescence in mixed organic-inorganic particles at temperatures less than 250 K. Phys Chem Chem Phys 12:12259-12266.
28. Weber RJ, et al. (2007) A study of secondary organic aerosol formation in the anthropogenic-influenced southeastern United States. J Geophys Res Atmos 112:D13302.
29. Lee SH, Murphy DM, Thomson DS, Middlebrook AM (2002) Chemical components of single particles measured with Particle Analysis by Laser Mass Spectrometry (PALMS) during the Atlanta SuperSite Project: Focus on organic/sulfate, lead, soot, and mineral particles. J Geophys Res Atmos 107(D1):4003.
30. Liu DY, Wenzel RJ, Prather KA (2003) Aerosol time-of-flight mass spectrometry during the Atlanta Supersite Experiment: 1. Measurements. J Geophys Res Atmos 108:8426.
31. Martin ST, et al. (2004) Effects of the physical state of tropospheric ammoniumsulfate- nitrate particles on global aerosol direct radiative forcing. Atmos Chem Phys 4(1):183-214. (Pubitemid 39073757)
32. Anttila T, Kiendler-Scharr A, Tillmann R, Mentel TF (2006) On the reactive uptake of gaseous compounds by organic-coated aqueous aerosols: Theoretical analysis and application to the heterogeneous hydrolysis of N2O5. J Phys Chem A 110:10435-10443. (Pubitemid 44412534)
33. Folkers M, Mentel TF, Wahner A (2003) Influence of an organic coating on the reactivity of aqueous aerosols probed by the heterogeneous hydrolysis of N2O5. Geophys Res Lett 30:1644.
34. Riemer N, et al. (2009) Relative importance of organic coatings for the heterogeneous hydrolysis of N2O5 during summer in Europe. J Geophys Res Atmos 114:D17307.
35. Escorcia EN, Sjostedt SJ, Abbatt JPD (2010) Kinetics of N(2)O(5) hydrolysis on secondary organic aerosol and mixed ammonium bisulfate-secondary organic aerosol particles. J Phys Chem A 114:13113-13121.
36. Brown SS, et al. (2006) Variability in nocturnal nitrogen oxide processing and its role in regional air quality. Science 311:67-70. (Pubitemid 43063058)
37. Riemer N, et al. (2003) Impact of the heterogeneous hydrolysis of N2O5 on chemistry and nitrate aerosol formation in the lower troposphere under photosmog conditions. J Geophys Res Atmos 108:4144.
38. Kwamena NOA, Buajarern J, Reid JP (2010) Equilibrium morphology of mixed organic/inorganic/aqueous aerosol droplets: Investigating the effect of relative humidity and surfactants. J Phys Chem A 114:5787-5795.
39. Reid JP, et al. (2011) The morphology of aerosol particles consisting of hydrophobic and hydrophilic phases: Hydrocarbons, alcohols and fatty acids as the hydrophobic component. Phys Chem Chem Phys 13:15559-15572.
40. Shilling JE, et al. (2008) Particle mass yield in secondary organic aerosol formed by the dark ozonolysis of alpha-pinene. Atmos Chem Phys 8:2073-2088.
41. Aiken AC, et al. (2008) O/C and OM/OC ratios of primary, secondary, and ambient organic aerosols with high-resolution time-of-flight aerosol mass spectrometry. Environ Sci Technol 42:4478-4485. (Pubitemid 351842394)
42. DeCarlo PF, et al. (2006) Field-deployable, high-resolution, time-of-flight aerosol mass spectrometer. Anal Chem 78:8281-8289. (Pubitemid 44927604)
43. Parsons MT, Mak J, Lipetz SR, Bertram AK (2004) Deliquescence of malonic, succinic, glutaric, and adipic acid particles. J Geophys Res 109:D06212.