Articles | Volume 21, issue 13
https://doi.org/10.5194/acp-21-10215-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-21-10215-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
07 Jul 2021
Research article |
| 07 Jul 2021
| 07 Jul 2021
Viscosity and phase state of aerosol particles consisting of sucrose mixed with inorganic salts
Young-Chul Song
Department of Earth and Environmental Sciences, Jeonbuk National University, Jeonju, Republic of Korea
The Earth and Environmental Science System Research Center, Jeonbuk National University, Jeonju, Republic of Korea
Joseph Lilek
Department of Atmospheric and Oceanic Sciences, McGill University, Montréal, Quebec, Canada
Jae Bong Lee
Innovative System Safety Research Division, Korea Atomic Energy Research Institute, Daejeon, Republic of Korea
Man Nin Chan
Earth System Science Programme, Faculty of Science, The Chinese University of Hong Kong, Hong Kong, China
The Institute of Environment, Energy, and Sustainability, The Chinese University of Hong Kong, Hong Kong, China
Zhijun Wu
Key Joint Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing, China
Andreas Zuend
Department of Atmospheric and Oceanic Sciences, McGill University, Montréal, Quebec, Canada
Mijung Song
CORRESPONDING AUTHOR
Department of Earth and Environmental Sciences, Jeonbuk National University, Jeonju, Republic of Korea
The Earth and Environmental Science System Research Center, Jeonbuk National University, Jeonju, Republic of Korea
Department of Environment and Energy, Jeonbuk National University, Jeonju, Republic of Korea
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Huan Song, Keding Lu, Can Ye, Huabin Dong, Shule Li, Shiyi Chen, Zhijun Wu, Mei Zheng, Limin Zeng, Min Hu, and Yuanhang Zhang
Atmos. Chem. Phys., 21, 13713–13727, https://doi.org/10.5194/acp-21-13713-2021, https://doi.org/10.5194/acp-21-13713-2021, 2021
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Yu Wang, Aristeidis Voliotis, Yunqi Shao, Taomou Zong, Xiangxinyue Meng, Mao Du, Dawei Hu, Ying Chen, Zhijun Wu, M. Rami Alfarra, and Gordon McFiggans
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Gang Zhao, Yishu Zhu, Zhijun Wu, Taomou Zong, Jingchuan Chen, Tianyi Tan, Haichao Wang, Xin Fang, Keding Lu, Chunsheng Zhao, and Min Hu
Atmos. Chem. Phys., 21, 9995–10004, https://doi.org/10.5194/acp-21-9995-2021, https://doi.org/10.5194/acp-21-9995-2021, 2021
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Tianyi Tan, Min Hu, Zhuofei Du, Gang Zhao, Dongjie Shang, Jing Zheng, Yanhong Qin, Mengren Li, Yusheng Wu, Limin Zeng, Song Guo, and Zhijun Wu
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Laurent Poulain, Benjamin Fahlbusch, Gerald Spindler, Konrad Müller, Dominik van Pinxteren, Zhijun Wu, Yoshiteru Iinuma, Wolfram Birmili, Alfred Wiedensohler, and Hartmut Herrmann
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Jingchuan Chen, Zhijun Wu, Jie Chen, Naama Reicher, Xin Fang, Yinon Rudich, and Min Hu
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Weigang Wang, Ting Lei, Andreas Zuend, Hang Su, Yafang Cheng, Yajun Shi, Maofa Ge, and Mingyuan Liu
Atmos. Chem. Phys., 21, 2179–2190, https://doi.org/10.5194/acp-21-2179-2021, https://doi.org/10.5194/acp-21-2179-2021, 2021
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Hoi Ki Lam, Rongshuang Xu, Jack Choczynski, James F. Davies, Dongwan Ham, Mijung Song, Andreas Zuend, Wentao Li, Ying-Lung Steve Tse, and Man Nin Chan
Atmos. Chem. Phys., 21, 2053–2066, https://doi.org/10.5194/acp-21-2053-2021, https://doi.org/10.5194/acp-21-2053-2021, 2021
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This work demonstrates that organic compounds present at or near the surface of aerosols can be subjected to oxidation initiated by gas-phase oxidants, such as hydroxyl radicals (OH). The heterogeneous reactivity is sensitive to their surface concentrations, which are determined by the phase separation behavior. This results of this work emphasize the effects of phase separation and potentially distinct aerosol morphologies on the chemical transformation of atmospheric aerosols.
Li Wu, Clara Becote, Sophie Sobanska, Pierre-Marie Flaud, Emilie Perraudin, Eric Villenave, Young-Chul Song, and Chul-Un Ro
Atmos. Chem. Phys., 20, 14103–14122, https://doi.org/10.5194/acp-20-14103-2020, https://doi.org/10.5194/acp-20-14103-2020, 2020
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Chao Peng, Yu Wang, Zhijun Wu, Lanxiadi Chen, Ru-Jin Huang, Weigang Wang, Zhe Wang, Weiwei Hu, Guohua Zhang, Maofa Ge, Min Hu, Xinming Wang, and Mingjin Tang
Atmos. Chem. Phys., 20, 13877–13903, https://doi.org/10.5194/acp-20-13877-2020, https://doi.org/10.5194/acp-20-13877-2020, 2020
Yujue Wang, Min Hu, Nan Xu, Yanhong Qin, Zhijun Wu, Liwu Zeng, Xiaofeng Huang, and Lingyan He
Atmos. Chem. Phys., 20, 13721–13734, https://doi.org/10.5194/acp-20-13721-2020, https://doi.org/10.5194/acp-20-13721-2020, 2020
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Field straw residue burning is a widespread type of biomass burning in Asia, while its emissions are poorly understood. In this study, we designed lab-controlled experiments to comprehensively investigate the emission factors, chemical compositions and light absorption properties of both water-soluble and water-insoluble carbonaceous aerosols emitted from straw burning. The results clearly highlight the significant influences of burning conditions and combustion efficiency on the emissions.
Young-Chul Song, Ariana G. Bé, Scot T. Martin, Franz M. Geiger, Allan K. Bertram, Regan J. Thomson, and Mijung Song
Atmos. Chem. Phys., 20, 11263–11273, https://doi.org/10.5194/acp-20-11263-2020, https://doi.org/10.5194/acp-20-11263-2020, 2020
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We report the liquid–liquid phase separation (LLPS) of organic aerosol consisting of α-pinene- and β-caryophyllene-derived ozonolysis products and commercial organic compounds. As compositional complexity increased from one to two organic species, LLPS occurred over a wider range of average O : C values (increasing from 0.44 to 0.67). These results provide further evidence that LLPS is likely frequent in organic aerosol particles in the troposphere, even in the absence of inorganic salt.
Cited articles
Abdulagatov, I. M., Zeinalova, A. A., and Azizov, N. D.:
Viscosity of the aqueous Ca(NO3)2 solutions at temperatures from 298 to 573 K and at pressures up to 40 MPa,
J. Chem. Eng. Data,
49, 1444–1450, https://doi.org/10.1021/je049853n, 2004.
Athanasiadis, A., Fitzgerald, C., Davidson, N. M., Giorio, C., Botchway, S. W., Ward, A. D., Kalberer, M., Pope, F. D., and Kuimova, M. K.:
Dynamic viscosity mapping of the oxidation of squalene aerosol particles,
Phys. Chem. Chem. Phys.,
18, 30385–30393, https://doi.org/10.1039/C6CP05674A, 2016.
Bateman, A. P., Bertram, A. K., and Martin, S. T.:
Hygroscopic influence on the semisolid-to-liquid transition of secondary organic materials,
J. Phys. Chem. A,
119, 4386–4395, https://doi.org/10.1021/jp508521c, 2015.
Bateman, A. P., Gong, Z., Harder, T. H., de Sá, S. S., Wang, B., Castillo, P., China, S., Liu, Y., O'Brien, R. E., Palm, B. B., Shiu, H.-W., Cirino, G. G., Thalman, R., Adachi, K., Alexander, M. L., Artaxo, P., Bertram, A. K., Buseck, P. R., Gilles, M. K., Jimenez, J. L., Laskin, A., Manzi, A. O., Sedlacek, A., Souza, R. A. F., Wang, J., Zaveri, R., and Martin, S. T.: Anthropogenic influences on the physical state of submicron particulate matter over a tropical forest, Atmos. Chem. Phys., 17, 1759–1773, https://doi.org/10.5194/acp-17-1759-2017, 2017.
Berkemeier, T., Steimer, S. S., Krieger, U. K., Peter, T., Pöschl, U., Ammann, M., and Shiraiwa, M.:
Ozone uptake on glassy, semi-solid and liquid organic matter and the role of reactive oxygen intermediates in atmospheric aerosol chemistry,
Phys. Chem. Chem. Phys.,
18, 12662–12674, 2016.
Bertram, A. K., Martin, S. T., Hanna, S. J., Smith, M. L., Bodsworth, A., Chen, Q., Kuwata, M., Liu, A., You, Y., and Zorn, S. R.: 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, https://doi.org/10.5194/acp-11-10995-2011, 2011.
Bhattarai, G., Lee, J. B., Kim, M. H., Ham, S., So, H. S., Oh, S.,
Sim, H. J., Lee, J. C., Song, M., and Kook, S. H.: Maternal exposure
to fine particulate matter during pregnancy induces progressive
senescence of hematopoietic stem cells under preferential
30 impairment of the bone marrow microenvironment and aids development
of myeloproliferative disease, Leukemia 34, 1481–1484, https://doi.org/10.1038/s41375-019-0665-8, 2020
Cheng, Z., Luo, L., Wang, S., Wang, Y., Sharma, S., Shimadera, H., Wang, X., Bressi, M., de Miranda, R. M., Jiang, J., Zhou, W., Fajardo, O., Yan, N., and Hao, J.:
Status and characteristics of ambient PM2.5 pollution in global megacities,
Environ. Int.,
89–90, 212–221, https://doi.org/10.1016/j.envint.2016.02.003, 2016.
Davies, J. F. and Wilson, K. R.:
Nanoscale interfacial gradients formed by the reactive uptake of OH radicals onto viscous aerosol surfaces,
Chem. Sci.,
6, 7020–7027, https://doi.org/10.1039/C5SC02326B, 2015.
George, I. J. and Abbatt, J. P. D.: Heterogeneous oxidation of atmospheric aerosol particles by gas-phase radicals, Nat. Chem., 2, 713–722, 2010.
Gervasi, N. R., Topping, D. O., and Zuend, A.: A predictive group-contribution model for the viscosity of aqueous organic aerosol, Atmos. Chem. Phys., 20, 2987–3008, https://doi.org/10.5194/acp-20-2987-2020, 2020.
Grayson, J. W., Song, M., Sellier, M., and Bertram, A. K.: Validation of the poke-flow technique combined with simulations of fluid flow for determining viscosities in samples with small volumes and high viscosities, Atmos. Meas. Tech., 8, 2463–2472, https://doi.org/10.5194/amt-8-2463-2015, 2015.
Grayson, J. W., Zhang, Y., Mutzel, A., Renbaum-Wolff, L., Böge, O., Kamal, S., Herrmann, H., Martin, S. T., and Bertram, A. K.: Effect of varying experimental conditions on the viscosity of α-pinene derived secondary organic material, Atmos. Chem. Phys., 16, 6027–6040, https://doi.org/10.5194/acp-16-6027-2016, 2016.
Grayson, J. W., Evoy, E., Song, M., Chu, Y., Maclean, A., Nguyen, A., Upshur, M. A., Ebrahimi, M., Chan, C. K., Geiger, F. M., Thomson, R. J., and Bertram, A. K.: The effect of hydroxyl functional groups and molar mass on the viscosity of non-crystalline organic and organic–water particles, Atmos. Chem. Phys., 17, 8509–8524, https://doi.org/10.5194/acp-17-8509-2017, 2017.
Guo, L., Gu, W., Peng, C., Wang, W., Li, Y. J., Zong, T., Tang, Y., Wu, Z., Lin, Q., Ge, M., Zhang, G., Hu, M., Bi, X., Wang, X., and Tang, M.: A comprehensive study of hygroscopic properties of calcium- and magnesium-containing salts: implication for hygroscopicity of mineral dust and sea salt aerosols, Atmos. Chem. Phys., 19, 2115–2133, https://doi.org/10.5194/acp-19-2115-2019, 2019.
Gupta, D., Eom, H.-J., Cho, H.-R., and Ro, C.-U.: Hygroscopic behavior of NaCl–MgCl2 mixture particles as nascent sea-spray aerosol surrogates and observation of efflorescence during humidification, Atmos. Chem. Phys., 15, 11273–11290, https://doi.org/10.5194/acp-15-11273-2015, 2015.
Ham, S., Babar, Z. B., Lee, J. B., Lim, H.-J., and Song, M.: Liquid–liquid phase separation in secondary organic aerosol particles produced from α-pinene ozonolysis and α-pinene photooxidation with/without ammonia, Atmos. Chem. Phys., 19, 9321–9331, https://doi.org/10.5194/acp-19-9321-2019, 2019.
Hao, L. Q., Kortelainen, A., Romakkaniemi, S., Portin, H., Jaatinen, A., Leskinen, A., Komppula, M., Miettinen, P., Sueper, D., Pajunoja, A., Smith, J. N., Lehtinen, K. E. J., Worsnop, D. R., Laaksonen, A., and Virtanen, A.: Atmospheric submicron aerosol composition and particulate organic nitrate formation in a boreal forestland–urban mixed region, Atmos. Chem. Phys., 14, 13483–13495, https://doi.org/10.5194/acp-14-13483-2014, 2014.
Haynes, W. M.:
CRC handbook of chemistry and physics, 97rd edn.,
CRC Press, New York, 2015.
Hinks, M. L., Brady, M. V, Lignell, H., Song, M., Grayson, J. W., Bertram, A. K., Lin, P., Laskin, A., Laskin, J., and Nizkorodov, S. A.:
Effect of viscosity on photodegradation rates in complex secondary organic aerosol materials,
Phys. Chem. Chem. Phys.,
18, 8785–8793, https://doi.org/10.1039/c5cp05226b, 2016.
Hosny, N. A., Fitzgerald, C., Tong, C., Kalberer, M., Kuimova, M. K., and Pope, F. D.: Fluorescent lifetime imaging of atmospheric aerosols: a direct probe of aerosol viscosity, Faraday Discuss., 165, 343–356, https://doi.org/10.1039/C3FD00041A, 2013.
Hosny, N. A., Fitzgerald, C., Vysniauskas, A., Athanasiadis, T., Berkemeier, T., Uygur, N., Pöschl, U., Shiraiwa, M., Kalberer, M., Pope, F. D., and Kuimova, M. K.:
Direct imaging of changes in aerosol particle viscosity upon hydration and chemical aging,
Chem. Sci.,
7, 1357–1367, https://doi.org/10.1039/C5SC02959G, 2016.
Huang, R. J., Zhang, Y., Bozzetti, C., Ho, K. F., Cao, J. J., Han, Y., Daellenbach, K. R., Slowik, J. G., Platt, S. M., Canonaco, F., Zotter, P., Wolf, R., Pieber, S. M., Bruns, E. A., Crippa, M., Ciarelli, G., Piazzalunga, A., Schwikowski, M., Abbaszade, G., Schnelle-Kreis, J., Zimmermann, R., An, Z., Szidat, S., Baltensperger, U., El Haddad, I., and Prévôt, A. S. H.:
High secondary aerosol contribution to particulate pollution during haze events in China,
Nature,
514, 218–222, https://doi.org/10.1038/nature13774, 2015.
Huang, Y., Mahrt, F., Xu, S., Shiraiwa, M., Zuend, A., and Bertram, A. K.:
Coexistence of three liquid phases in individual atmospheric aerosol particles,
P. Natl. Acad. Sci. USA,
118, e2102512118, https://doi.org/10.1073/pnas.2102512118, 2021.
Ji, Z. R., Zhang, Y., Pang, S. F., and Zhang, Y. H.: Crystal nucleation and crystal growth and mass transfer in internally mixed sucrose/NaNO3 particles, J. Phys. Chem. A, 121, 7968–7975, https://doi.org/10.1021/acs.jpca.7b08004, 2017.
Kanakidou, M., Seinfeld, J. H., Pandis, S. N., Barnes, I., Dentener, F. J., Facchini, M. C., Van Dingenen, R., Ervens, B., Nenes, A., Nielsen, C. J., Swietlicki, E., Putaud, J. P., Balkanski, Y., Fuzzi, S., Horth, J., Moortgat, G. K., Winterhalter, R., Myhre, C. E. L., Tsigaridis, K., Vignati, E., Stephanou, E. G., and Wilson, J.: Organic aerosol and global climate modelling: a review, Atmos. Chem. Phys., 5, 1053–1123, https://doi.org/10.5194/acp-5-1053-2005, 2005.
Kaufman, Y. J., Tanré, D., and Boucher, O.:
A satellite view of aerosols in the climate system,
Nature,
419, 215–223, 2002.
Kidd, C., Perraud, V., Wingen, L. M., and Finlayson-Pitts, B. J.:
Integrating phase and composition of secondary organic aerosol from the ozonolysis of α-pinene,
P. Natl. Acad. Sci. USA,
111, 7552–7, https://doi.org/10.1073/pnas.1322558111, 2014.
Kim, Y., Sartelet, K., and Couvidat, F.: Modeling the effect of non-ideality, dynamic mass transfer and viscosity on SOA formation in a 3-D air quality model, Atmos. Chem. Phys., 19, 1241–1261, https://doi.org/10.5194/acp-19-1241-2019, 2019.
Knopf, D. A., Alpert, P., and Wang, B.:
The role of organic aerosol in atmospheric ice nucleation – A Review,
ACS Earth Sp. Chem.,
2, 168–202, https://doi.org/10.1021/acsearthspacechem.7b00120, 2018.
Koop, T., Bookhold, J., Shiraiwa, M., and Pöschl, U.:
Glass transition and phase state of organic compounds: dependency on molecular properties and implications for secondary organic aerosols in the atmosphere,
Phys. Chem. Chem. Phys.,
13, 19238–19255, https://doi.org/10.1039/c1cp22617g, 2011.
Kulmala, M., Asmi, A., Lappalainen, H. K., Baltensperger, U., Brenguier, J.-L., Facchini, M. C., Hansson, H.-C., Hov, Ø., O'Dowd, C. D., Pöschl, U., Wiedensohler, A., Boers, R., Boucher, O., de Leeuw, G., Denier van der Gon, H. A. C., Feichter, J., Krejci, R., Laj, P., Lihavainen, H., Lohmann, U., McFiggans, G., Mentel, T., Pilinis, C., Riipinen, I., Schulz, M., Stohl, A., Swietlicki, E., Vignati, E., Alves, C., Amann, M., Ammann, M., Arabas, S., Artaxo, P., Baars, H., Beddows, D. C. S., Bergström, R., Beukes, J. P., Bilde, M., Burkhart, J. F., Canonaco, F., Clegg, S. L., Coe, H., Crumeyrolle, S., D'Anna, B., Decesari, S., Gilardoni, S., Fischer, M., Fjaeraa, A. M., Fountoukis, C., George, C., Gomes, L., Halloran, P., Hamburger, T., Harrison, R. M., Herrmann, H., Hoffmann, T., Hoose, C., Hu, M., Hyvärinen, A., Hõrrak, U., Iinuma, Y., Iversen, T., Josipovic, M., Kanakidou, M., Kiendler-Scharr, A., Kirkevåg, A., Kiss, G., Klimont, Z., Kolmonen, P., Komppula, M., Kristjánsson, J.-E., Laakso, L., Laaksonen, A., Labonnote, L., Lanz, V. A., Lehtinen, K. E. J., Rizzo, L. V., Makkonen, R., Manninen, H. E., McMeeking, G., Merikanto, J., Minikin, A., Mirme, S., Morgan, W. T., Nemitz, E., O'Donnell, D., Panwar, T. S., Pawlowska, H., Petzold, A., Pienaar, J. J., Pio, C., Plass-Duelmer, C., Prévôt, A. S. H., Pryor, S., Reddington, C. L., Roberts, G., Rosenfeld, D., Schwarz, J., Seland, Ø., Sellegri, K., Shen, X. J., Shiraiwa, M., Siebert, H., Sierau, B., Simpson, D., Sun, J. Y., Topping, D., Tunved, P., Vaattovaara, P., Vakkari, V., Veefkind, J. P., Visschedijk, A., Vuollekoski, H., Vuolo, R., Wehner, B., Wildt, J., Woodward, S., Worsnop, D. R., van Zadelhoff, G.-J., Zardini, A. A., Zhang, K., van Zyl, P. G., Kerminen, V.-M., S Carslaw, K., and Pandis, S. N.: General overview: European Integrated project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI) – integrating aerosol research from nano to global scales, Atmos. Chem. Phys., 11, 13061–13143, https://doi.org/10.5194/acp-11-13061-2011, 2011.
Kuwata, M. and Martin, S. T.:
Phase of atmospheric secondary organic material affects its reactivity,
P. Natl. Acad. Sci. USA,
109, 17354-17359, 2012.
Ladino, L. A., Zhou, S., Yakobi-Hancock, J. D., Aljawhary, D., and Abbatt, J. P. D.:
Factors controlling the ice nucleating abilities of α-pinene SOA particles,
J. Geophys. Res.,
119, 9041–9051, https://doi.org/10.1002/2014JD021578, 2014.
Laliberté, M.:
Model for calculating the viscosity of aqueous aolutions,
J. Chem. Eng. Data,
52, 1507–1508, https://doi.org/10.1021/je700232s, 2007.
Laliberté, M.:
A model for calculating the heat capacity of aqueous solutions, with updated density and viscosity data,
J. Chem. Eng. Data,
54, 1725–1760, https://doi.org/10.1021/je8008123, 2009.
Laskin, A., Iedema, M. J., Ichkovich, A., Graber, E. R., Taraniuk, I., and Rudich, Y.:
Direct observation of completely processed calcium carbonate dust particles,
Faraday Discuss.,
130, 453–468, https://doi.org/10.1039/b417366j, 2005.
Li, J., Forrester, S. M., and Knopf, D. A.: Heterogeneous oxidation of amorphous organic aerosol surrogates by O3, NO3, and OH at typical tropospheric temperatures, Atmos. Chem. Phys., 20, 6055–6080, https://doi.org/10.5194/acp-20-6055-2020, 2020.
Li, X. H., Zhao, L. J., Dong, J. L., Xiao, H. S., and Zhang, Y. H.:
Confocal raman studies of Mg(NO3)2 aerosol particles deposited on a quartz substrate: supersaturated structures and complicated phase transitions,
J. Phys. Chem. B,
112, 5032–5038, https://doi.org/10.1021/jp709938x, 2008.
Liu, Y., Wu, Z., Huang, X., Shen, H., Bai, Y., Qiao, K., Meng, X., Hu, W., Tang, M., and He, L.: Aerosol Phase State and Its Link to Chemical Composition and Liquid Water Content in a Subtropical Coastal Megacity, Environ. Sci. Technol., 53, 5027–5033, https://doi.org/10.1021/acs.est.9b01196, 2019.
Lilek, J. and Zuend, A.: A predictive viscosity model for aqueous electrolytes and mixed organic–inorganic aerosol phase,
in preparation, 2021.
Liu, Y. J., Zhu, T., Zhao, D. F., and Zhang, Z. F.: Investigation of the hygroscopic properties of Ca(NO3)2 and internally mixed Ca(NO3)2
Maclean, A. M., Smith, N. R., Li, Y., Huang, Y., Hettiyadura, A. P. S., Crescenzo, G. V., Shiraiwa, M., Laskin, A., Nizkorodov, S. A., and Bertram, A. K.:
Humidity-Dependent Viscosity of Secondary Organic Aerosol from Ozonolysis of β-Caryophyllene: Measurements, Predictions, and Implications,
ACS Earth Sp. Chem.,
5, 305–318, https://doi.org/10.1021/acsearthspacechem.0c00296, 2021.
Mikhailov, E., Vlasenko, S., Martin, S. T., Koop, T., and Pöschl, U.: Amorphous and crystalline aerosol particles interacting with water vapor: conceptual framework and experimental evidence for restructuring, phase transitions and kinetic limitations, Atmos. Chem. Phys., 9, 9491–9522, https://doi.org/10.5194/acp-9-9491-2009, 2009.
Murphy, D. M., Cziczo, D. J., Froyd, K. D., Hudson, P. K., Matthew, B. M., Middlebrook, A. M., Peltier, R. E., Sullivan, A., Thomson, D. S., and Weber, R. J.:
Single-peptide mass spectrometry of tropospheric aerosol particles,
J. Geophys. Res.-Atmos.,
111, 1–15, https://doi.org/10.1029/2006JD007340, 2006.
Murray, B. J.: Inhibition of ice crystallisation in highly viscous aqueous organic acid droplets, Atmos. Chem. Phys., 8, 5423–5433, https://doi.org/10.5194/acp-8-5423-2008, 2008.
Murray, B. J., Wilson, T. W., Dobbie, S., Cui, Z., Al-Jumur, S. M. R. K., Möhler, O., Schnaiter, M., Wagner, R., Benz, S., Niemand, M., Saathoff, H., Ebert, V., Wagner, S., and Kärcher, B.:
Heterogeneous nucleation of ice particles on glassy aerosols under cirrus conditions,
Nat. Geosci.,
3, 233–237, https://doi.org/10.1038/ngeo817, 2010.
Murray, B. J., Haddrell, A. E., Peppe, S., Davies, J. F., Reid, J. P., O'Sullivan, D., Price, H. C., Kumar, R., Saunders, R. W., Plane, J. M. C., Umo, N. S., and Wilson, T. W.: Glass formation and unusual hygroscopic growth of iodic acid solution droplets with relevance for iodine mediated particle formation in the marine boundary layer, Atmos. Chem. Phys., 12, 8575–8587, https://doi.org/10.5194/acp-12-8575-2012, 2012.
Pan, X., Uno, I., Wang, Z., Nishizawa, T., Sugimoto, N., Yamamoto, S., Kobayashi, H., Sun, Y., Fu, P., Tang, X., and Wang, Z.:
Real-time observational evidence of changing Asian dust morphology with the mixing of heavy anthropogenic pollution,
Sci. Rep.-UK,
7, 1–8, https://doi.org/10.1038/s41598-017-00444-w, 2017.
Pant, A., Parsons, M. T., and Bertram, A. K.: 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, https://doi.org/10.1021/Jp060985s, 2006.
Petters, S. S., Kreidenweis, S. M., Grieshop, A. P., Ziemann, P. J., and Petters, M. D.:
Temperature- and humidity-dependent phase states of secondary organic aerosols,
Geophys. Res. Lett.,
46, 1005–1013, https://doi.org/10.1029/2018GL080563, 2019.
Power, R. M., Simpson, S. H., Reid, J. P., and Hudson, A. J.:
The Transition from liquid to solid-like behaviour in ultrahigh viscosity aerosol particles,
Chem. Sci.,
4, 2597–2604, https://doi.org/10.1039/c3sc50682g, 2013.
Reid, J. P., Bertram, A. K., Topping, D. O., Laskin, A., Martin, S. T., Petters, M. D., Pope, F. D., and Rovelli, G.:
The viscosity of atmospherically relevant organic particles,
Nat. Commun.,
9, 956, https://doi.org/10.1038/s41467-018-03027-z, 2018.
Renbaum-Wolff, L., Grayson, J. W., Bateman, A. P., Kuwata, M., Sellier, M., Murray, B. J., Shilling, J. E., Martin, S. T., and Bertram, A. K.:
Viscosity of α-pinene secondary organic material and implications for particle growth and reactivity,
P. Natl. Acad. Sci. USA,
110, 8014–9, https://doi.org/10.1073/pnas.1219548110, 2013.
Richards, D. S., Trobaugh, K. L., Hajek-Herrera, J., Price, C. L., Sheldon, C. S., Davies, J. F., and Davis, R. D.:
Ion-molecule interactions enable unexpected phase transitions in organic-inorganic aerosol,
Science Advances,
6, 1–12. https://doi.org/10.1126/sciadv.abb5643, 2020a.
Richards, D. S., Trobaugh, K. L., Hajek-Herrera, J., and Davis, R. D.:
Dual-Balance Electrodynamic Trap as a Microanalytical Tool for Identifying Gel Transitions and Viscous Properties of Levitated Aerosol Particles,
Anal. Chem.,
92, 3086–3094, https://doi.org/10.1021/acs.analchem.9b04487, 2020b.
Rothfuss, N. E. and Petters, M. D.:
Influence of functional groups on the viscosity of organic aerosol,
Environ. Sci. Technol.,
51, 271–279, https://doi.org/10.1021/acs.est.6b04478, 2017.
Rovelli, G., Song, Y. C., Maclean, A. M., Topping, D. O., Bertram, A. K., and Reid, J. P.:
Comparison of approaches for measuring and predicting the viscosity of ternary component aerosol particles,
Anal. Chem.,
91, 5074–5082, https://doi.org/10.1021/acs.analchem.8b05353, 2019.
Russell, P. B., Kinne, S. A., and Bergstrom, R. W.:
Aerosol climate effects: local radiative forcing and column closure experiments,
J. Geophys. Res.-Atmos.,
102, 9397–9407, https://doi.org/10.1029/97jd00112, 1997.
Saukko, E., Lambe, A. T., Massoli, P., Koop, T., Wright, J. P., Croasdale, D. R., Pedernera, D. A., Onasch, T. B., Laaksonen, A., Davidovits, P., Worsnop, D. R., and Virtanen, A.: Humidity-dependent phase state of SOA particles from biogenic and anthropogenic precursors, Atmos. Chem. Phys., 12, 7517–7529, https://doi.org/10.5194/acp-12-7517-2012, 2012.
Schmedding, R., Rasool, Q. Z., Zhang, Y., Pye, H. O. T., Zhang, H., Chen, Y., Surratt, J. D., Lopez-Hilfiker, F. D., Thornton, J. A., Goldstein, A. H., and Vizuete, W.: Predicting secondary organic aerosol phase state and viscosity and its effect on multiphase chemistry in a regional-scale air quality model, Atmos. Chem. Phys., 20, 8201–8225, https://doi.org/10.5194/acp-20-8201-2020, 2020.
Sellier, M., Grayson, J. W., Renbaum-Wolff, L., Song, M., and Bertram, A. K.: Estimating the viscosity of a highly viscous liquid droplet through the relaxation time of a dry spot, J. Rheol., 59, 733–750, https://doi.org/10.1122/1.4917240, 2015.
Shi, Z., Zhang, D., Hayashi, M., Ogata, H., Ji, H., and Fujiie, W.:
Influences of sulfate and nitrate on the hygroscopic behaviour of coarse dust particles,
Atmos. Environ.,
42, 822–827, https://doi.org/10.1016/j.atmosenv.2007.10.037, 2008.
Shiraiwa, M. and Seinfeld, J. H.:
Equilibration timescale of atmospheric secondary organic aerosol partitioning,
Geophys. Res. Lett.,
39, L24801, https://doi.org/10.1029/2012GL054008, 2012.
Shiraiwa, M., Yee, L. D., Schilling, K. A., Loza, C. L., Craven, J. S., Zuend, A., Ziemann, P. J., and Seinfeld, J. H.: Size distribution dynamics reveal particle-phase chemistry in organic aerosol formation, P. Natl. Acad. Sci. USA, 110, 11746–11750, https://doi.org/10.1073/pnas.1307501110, 2013.
Slade, J. H. and Knopf, D. A.:
Multiphase OH oxidation kinetics of organic aerosol: The role of particle phase state and relative humidity,
Geophys. Res. Lett.,
41, 5297–5306. https://doi.org/10.1002/2014GL060582, 2014.
Song, M., Marcolli, C., Krieger, U. K., Zuend, A., and Peter, T.: Liquid-liquid phase separation and morphology of internally mixed dicarboxylic acids/ammonium sulfate/water particles, Atmos. Chem. Phys., 12, 2691–2712, https://doi.org/10.5194/acp-12-2691-2012, 2012.
Song, M., Liu, P. F., Hanna, S. J., Li, Y. J., Martin, S. T., and Bertram, A. K.: Relative humidity-dependent viscosities of isoprene-derived secondary organic material and atmospheric implications for isoprene-dominant forests, Atmos. Chem. Phys., 15, 5145–5159, https://doi.org/10.5194/acp-15-5145-2015, 2015.
Song, M., Liu, P. F., Hanna, S. J., Zaveri, R. A., Potter, K., You, Y., Martin, S. T., and Bertram, A. K.:
Relative humidity-dependent viscosity of secondary organic material from toluene photo-oxidation and possible implications for organic particulate matter over megacities, Atmos. Chem. Phys., 16, 8817–8830, https://doi.org/10.5194/acp-16-8817-2016, 2016.
Song, M., Maclean, A. M., Huang, Y., Smith, N. R., Blair, S. L., Laskin, J., Laskin, A., DeRieux, W.-S. W., Li, Y., Shiraiwa, M., Nizkorodov, S. A., and Bertram, A. K.:
Liquid–liquid phase separation and viscosity within secondary organic aerosol generated from diesel fuel vapors, Atmos. Chem. Phys., 19, 12515–12529, https://doi.org/10.5194/acp-19-12515-2019, 2019.
Song, Y. C., Ryu, J., Malek, M. A., Jung, H. J., and Ro, C. U.:
Chemical speciation of individual airborne particles by the combined use of quantitative energy-dispersive electron probe X-ray microanalysis and attenuated total reflection Fourier transform-infrared imaging techniques,
Anal. Chem.,
82, 7987–7998, https://doi.org/10.1021/ac1014113, 2010.
Song, Y.-C., Eom, H.-J., Jung, H.-J., Malek, M. A., Kim, H. K., Geng, H., and Ro, C.-U.: Investigation of aged Asian dust particles by the combined use of quantitative ED-EPMA and ATR-FTIR imaging, Atmos. Chem. Phys., 13, 3463–3480, https://doi.org/10.5194/acp-13-3463-2013, 2013.
Song, Y. C., Haddrell, A. E., Bzdek, B. R., Reid, J. P., Bannan, T., Topping, D. O., Percival, C., and Cai, C.:
Measurements and pedictions of binary component aerosol particle viscosity,
J. Phys. Chem. A,
120, 8123–8137, https://doi.org/10.1021/acs.jpca.6b07835, 2016.
Song, Y. C., Ingram, S., Arbon, R. E., Topping, D. O., Glowacki, D. R., and Reid, J. P.: Transient Cavity Dynamics and Divergence from the Stokes-Einstein Equation in Organic Aerosol, Chem. Sci., 11, 2999–3006, https://doi.org/10.1039/C9SC06228A, 2020.
Steimer, S. S., Berkemeier, T., Gilgen, A., Krieger, K. U., Peter, T., Shiraiwa, M., and Ammann, M.:
Shikimic acid ozonolysis kinetics in the transition from liquid aqueous solution to highly viscous glass,
Phys. Chem. Chem. Phys.,
17, 31101–31109, https://doi.org/10.1039/C5CP04544D, 2015.
Stokes, R. H. and Robinson, R. A.:
Interactions in aqueous nonelectrolyte solutions .i. solute-solvent equilibria,
J. Phys. Chem.,
70, 2126–2130, 1966.
Sullivan, R. C., Guazzotti, S. A., Sodeman, D. A., and Prather, K. A.: Direct observations of the atmospheric processing of Asian mineral dust, Atmos. Chem. Phys., 7, 1213–1236, https://doi.org/10.5194/acp-7-1213-2007, 2007.
Usher, C. R., Michel, A. E., and Grassian, V. H.:
Reactions on mineral dust,
Chem. Rev.,
103, 4883–4939, https://doi.org/10.1021/cr020657y, 2003.
Vaden, T. D., Imre, D., Beranek, J., Shrivastava, M., and Zelenyuk, A.:
Evaporation kinetics and phase of laboratory and ambient secondary organic aerosol,
P. Natl. Acad. Sci. USA,
108, 2190–2195, https://doi.org/10.1073/pnas.1013391108, 2011.
Virtanen, A., Joutsensaari, J., Koop, T., Kannosto, J., Yli-Pirilä, P., Leskinen, J., Mäkelä, J. M., Holopainen, J. K., Pöschl, U., Kulmala, M., Worsnop, D. R., and Laaksonen, A.:
An amorphous solid state of biogenic secondary organic aerosol particles,
Nature,
467, 824–827, https://doi.org/10.1038/nature09455, 2010.
Wahab, A., Mahiuddin, S., Hefter, G., and Kunz, W.:
Densities, ultrasonic velocities, viscosities, and electrical conductivities of aqueous solutions of Mg(OAc)2 and Mg(NO3)2,
J. Chem. Eng. Data,
51, 1609–1616, https://doi.org/10.1021/je060107n, 2006.
Wallace, B. J. and Preston, T. C.:
Water Uptake and Loss in Viscous Aerosol Particles with Concentration-Dependent Diffusivities,
J. Phys. Chem. A,
123, 3374–3382, https://doi.org/10.1021/acs.jpca.9b00907, 2019.
Wang, G., Zhang, R., Gomez, M. E., Yang, L., Levy Zamora, M., Hu, M., Lin, Y., Peng, J., Guo, S., Meng, J., Li, J., Cheng, C., Hu, T., Ren, Y., Wang, Y., Gao, J., Cao, J., An, Z., Zhou, W., Li, G., Wang, J., Tian, P., Marrero-Ortiz, W., Secrest, J., Du, Z., Zheng, J., Shang, D., Zeng, L., Shao, M., Wang, W., Huang, Y., Wang, Y., Zhu, Y., Li, Y., Hu, J., Pan, B., Cai, L., Cheng, Y., Ji, Y., Zhang, F., Rosenfeld, D., Liss, P. S., Duce, R. A., Kolb, C. E., and Molina, M. J.:
Persistent sulfate formation from London fog to Chinese haze,
P. Natl. Acad. Sci. USA,
113, 13630–13635, https://doi.org/10.1073/pnas.1616540113, 2016.
Wang, L. N., Cai, C., and Zhang, Y. H.: Kinetically determined hygroscopicity and efflorescence of sucrose-ammonium sulfate aerosol droplets under lower RH, J. Phys. Chem. B, 121, 8551–8557, https://doi.org/10.1021/acs.jpcb.7b05551, 2017.
Wang, S., Nan, J., Shi, C., Fu, Q., Gao, S., Wang, D., Cui, H., Saiz-Lopez, A., and Zhou, B.:
Atmospheric ammonia and its impacts on regional air quality over the megacity of Shanghai, China,
Sci. Rep.-UK,
5, 1–13, https://doi.org/10.1038/srep15842, 2015a.
Wang, Y., Ma, J. B., Zhou, Q., Pang, S. F., and Zhang, Y. H.:
Hygroscopicity of mixed glycerol
Winston, P. W. and Bates, D. H.:
Saturated solutions for the control of humidity in biological research,
Ecology,
41, 232–237, 1960.
Xiao, S. and Bertram, A. K.:
Reactive uptake kinetics of NO3 on multicomponent and multiphase organic mixtures containing unsaturated and saturated organics,
Phys. Chem. Chem. Phys,
13, 6628–6636, 2011.
Xu, R., Lam, H. K., Wilson, K. R., Davies, J. F., Song, M., Li, W., Tse, Y.-L. S., and Chan, M. N.: Effect of inorganic-to-organic mass ratio on the heterogeneous OH reaction rates of erythritol: implications for atmospheric chemical stability of 2-methyltetrols, Atmos. Chem. Phys., 20, 3879–3893, https://doi.org/10.5194/acp-20-3879-2020, 2020.
Yli-Juuti, T., Pajunoja, A., Tikkanen, O. P., Buchholz, A., Faiola, C., Väisänen, O., Hao, L., Kari, E., Peräkylä, O., Garmash, O., Shiraiwa, M., Ehn, M., Lehtinen, K., and Virtanen, A.:
Factors controlling the evaporation of secondary organic aerosol from α-pinene ozonolysis,
Geophys. Res. Lett.,
44, 2562–2570, https://doi.org/10.1002/2016GL072364, 2017.
Zaveri, R. A., Easter, R. C., Shilling, J. E., and Seinfeld, J. H.: Modeling kinetic partitioning of secondary organic aerosol and size distribution dynamics: representing effects of volatility, phase state, and particle-phase reaction, Atmos. Chem. Phys., 14, 5153–5181, https://doi.org/10.5194/acp-14-5153-2014, 2014.
Zaveri, R. A., Shilling, J. E., Zelenyuk, A., Liu, J. M., Bell, D. M., D'Ambro, E. L., Gaston, C., Thornton, J. A., Laskin, A., Lin, P., Wilson, J., Easter, R. C., Wang, J., Bertram, A. K., Martin, S. T., Seinfeld, J. H., and Worsnop, D. R.: Growth kinetics and size distribution dynamics of viscous secondary organic aerosol, Environ. Sci. Technol., 52, 3, 1191–1199, https://doi.org/10.1021/acs.est.7b04623, 2018.
Zdanovskii, A. B.:
Trudy Solyanoi Laboratorii (Transactions of the Salt Laboratory),
Akad. Nauk SSSR,
6, 5–70, 1936.
Zdanovskii, A. B.:
New methods of calculating solubilities of electrolytes in multicomponent systems,
Zh. Fiz. Khim+.,
22, 1478–1485, 1948.
Zhang, Q., Jimenez, J. L., Canagaratna, M. R., Allan, J. D., Coe, H., Ulbrich, I., Alfarra, M. R., Takami, A., Middlebrook, A. M., Sun, Y. L., Dzepina, K., Dunlea, E., Docherty, K., DeCarlo, P. F., Salcedo, D., Onasch, T., Jayne, J. T., Miyoshi, T., Shimono, A., Hatakeyama, S., Takegawa, N., Kondo, Y., Schneider, J., Drewnick, F., Borrmann, S., Weimer, S., Demerjian, K., Williams, P., Bower, K., Bahreini, R., Cottrell, L., Griffin, R. J., Rautiainen, J., Sun, J. Y., Zhang, Y. M., and Worsnop, D. R.:
Ubiquity and dominance of oxygenated species in organic aerosols in anthropogenically-influenced Northern Hemisphere midlatitudes,
Geophys. Res. Lett.,
34, 1–6, https://doi.org/10.1029/2007GL029979, 2007.
Zhang, R., Wang, G., Guo, S., Zamora, M. L., Ying, Q., Lin, Y., Wang, W., Hu, M., and Wang, Y.:
Formation of urban fine particulate matter,
Chem. Rev.,
115, 3803–3855, https://doi.org/10.1021/acs.chemrev.5b00067, 2015.
Zhang, Y., Sanchez, M. S., Douet, C., Wang, Y., Bateman, A. P., Gong, Z., Kuwata, M., Renbaum-Wolff, L., Sato, B. B., Liu, P. F., Bertram, A. K., Geiger, F. M., and Martin, S. T.: Changing shapes and implied viscosities of suspended submicron particles, Atmos. Chem. Phys., 15, 7819–7829, https://doi.org/10.5194/acp-15-7819-2015, 2015.
Zieger, P., Vaisanen, O., Corbin, J. C., Partridge, D. G., Bastelberger, S., Mousavi-Fard, M., Rosati, B., Gysel, M., Krieger, U. K., Leck, C., Nenes, A., Riipinen, I., Virtanen, A., and Salter, M. E.:
Revising the hygroscopicity of inorganic sea salt particles,
Nat. Commun.,
8, 15883, https://doi.org/10.1038/ncomms15883, 2017.
Zobrist, B., Marcolli, C., Pedernera, D. A., and Koop, T.: Do atmospheric aerosols form glasses?, Atmos. Chem. Phys., 8, 5221–5244, https://doi.org/10.5194/acp-8-5221-2008, 2008.
Zobrist, B., Soonsin, V., Luo, B. P., Krieger, U. K., Marcolli, C., Peter, T., and Koop, T.:
Ultra-slow water diffusion in aqueous sucrose glasses,
Phys. Chem. Chem. Phys.,
13, 3514–26, https://doi.org/10.1039/c0cp01273d, 2011.
Zuend, A., Marcolli, C., Luo, B. P., and Peter, T.: A thermodynamic model of mixed organic-inorganic aerosols to predict activity coefficients, Atmos. Chem. Phys., 8, 4559–4593, https://doi.org/10.5194/acp-8-4559-2008, 2008.
Zuend, A., Marcolli, C., Booth, A. M., Lienhard, D. M., Soonsin, V., Krieger, U. K., Topping, D. O., McFiggans, G., Peter, T., and Seinfeld, J. H.: New and extended parameterization of the thermodynamic model AIOMFAC: calculation of activity coefficients for organic-inorganic mixtures containing carboxyl, hydroxyl, carbonyl, ether, ester, alkenyl, alkyl, and aromatic functional groups, Atmos. Chem. Phys., 11, 9155–9206, https://doi.org/10.5194/acp-11-9155-2011, 2011.
Short summary
We report viscosity of binary mixtures of organic material / H2O and inorganic salts / H2O, as well as ternary mixtures of organic material / inorganic salts/ H2O, over the atmospheric relative humidity (RH) range. The viscosity measurements indicate that the studied mixed organic–inorganic particles range in phase state from liquid to semi-solid or even solid across the atmospheric RH range at a temperature of 293 K.
We report viscosity of binary mixtures of organic material / H2O and inorganic salts / H2O, as...
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