Crystal Nucleation and Crystal Growth and Mass Transfer in Internally Mixed Sucrose/NaNO3 Particles

Ji, Zhi-Ru; Zhang, Yunhong; Pang, Shu-Feng; Yun-hong, Zhang

doi:10.1021/acs.jpca.7b08004

Cited by 20 publications

(18 citation statements)

References 56 publications

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“…Despite the abundant mass of inorganic species in the atmosphere (Jimenez et al, 2009;Cheng et al, 2016), few studies have reported the viscosity of single particles consisting of inorganic species covering the RH range to high salt concentrations (Power et al, 2013;Rovelli et al, 2019). Herein, the RH-dependent viscosity was quantified for particles consisting of Mg(NO 3 ) 2 / H 2 O or Ca(NO 3 ) 2 / H 2 O determined at 293 ± 1 K upon dehydration using the bead-mobility and poke-and-flow techniques.…”

Section: Viscosities Of Particles Consisting Ofmentioning

confidence: 99%

“…Aerosol particles are emitted from various natural (e.g., the ocean and plants) and anthropogenic (e.g., transportation and fuel combustion) sources, as well as being produced by gas-to-particle conversion and equilibration processes due to chemical processing of gaseous species in the atmosphere (e.g., sulfur dioxide, nitrogen oxides, ammonia, and volatile organic compounds). Submicron-sized aerosol particles mainly consist of organic materials and inorganic salts (Jimenez et al, 2009;Huang et al, 2015;Cheng et al, 2016). Depending on the location and the season, the organic mass fraction of submicron particles ranges from ∼ 20 % up to ∼ 90 % (Zhang et al, 2007;Jimenez et al, 2009;Hao et al, 2014;Huang et al, 2015;Cheng et al, 2016;Wang et al, 2016).…”

Section: Introductionmentioning

confidence: 99%

“…Submicron-sized aerosol particles mainly consist of organic materials and inorganic salts (Jimenez et al, 2009;Huang et al, 2015;Cheng et al, 2016). Depending on the location and the season, the organic mass fraction of submicron particles ranges from ∼ 20 % up to ∼ 90 % (Zhang et al, 2007;Jimenez et al, 2009;Hao et al, 2014;Huang et al, 2015;Cheng et al, 2016;Wang et al, 2016). Field measurements have shown that organic materials and inorganic salts are often internally mixed in an aerosol particle (Murphy et al, 2006;Y.…”

Section: Introductionmentioning

confidence: 99%

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Viscosity and phase state of aerosol particles consisting of sucrose mixed with inorganic salts

et al. 2021

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Abstract. Research on the viscosity and phase state of aerosol particles is essential because of their significant influence on the particle growth rate, equilibration times, and related evolution of mass concentration as well as heterogeneous reactions. So far, most studies of viscosity and phase state have been focused on organic aerosol particles, yet data on how viscosity can vary when the organic materials are mixed with inorganic salts remain scarce. Herein, using bead-mobility and poke-and-flow techniques, we quantified viscosities at 293 ± 1 K for 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. Sucrose as the organic species and calcium nitrate (Ca(NO3)2) or magnesium nitrate (Mg(NO3)2) as the inorganic salts were examined. For binary sucrose / H2O particles, the viscosities gradually increased from ∼ 3 × 10−2 to ≳1 × 108 Pa s as RH decreased from ∼ 75 % to ∼ 25 %. Compared with the results for the sucrose / H2O particles, binary Ca(NO3)2/H2O and Mg(NO3)2/H2O particles showed drastic enhancements to ≳1 × 108 Pa s at low RH close to the efflorescence RH. For ternary mixtures of sucrose / Ca(NO3)2 / H2O or sucrose / Mg(NO3)2 / H2O, with organic-to-inorganic mass ratios of 1:1, the viscosities of the particles gradually increased from ∼ 3 × 10−2 to greater than ∼ 1 × 108 Pa s for RH values from ∼ 75 % to ∼ 5 %. Compared to the viscosities of the Ca(NO3)2/H2O particles, higher viscosities were observed for the ternary sucrose / Ca(NO3)2 / H2O particles, with values increased by about 1 order of magnitude at 50 % RH and about 6 orders of magnitude at 35 % RH. Moreover, we applied a thermodynamics-based group-contribution model (AIOMFAC-VISC, Aerosol Inorganic–Organic Mixtures Functional groups Activity Coefficients Viscosity) to predict aerosol viscosities for the studied systems. The model predictions and viscosity measurements show good agreement within ∼ 1 order of magnitude in viscosity. 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. These results support our understanding that organic / inorganic / H2O particles can exist in a liquid, semisolid, or even a solid state in the troposphere.

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Section: Viscosities Of Particles Consisting Ofmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Viscosity and phase state of aerosol particles consisting of sucrose mixed with inorganic salts

et al. 2021

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“…These VOCs can be oxidized in the atmosphere, and the oxidized products can form secondary organic aerosol (SOA) (Hallquist et al, 2009;Ervens et al, 2011). SOA accounts for 20 %-80 % of the mass of atmospheric aerosol particles (Zhang et al, 2007;Jimenez et al, 2009) and plays an important role in climate, air quality, and public health (Kanakidou et al, 2005;Jang et al, 2006;Solomon, 2007;Baltensperger et al, 2008;Murray et al, 2010;Wang et al, 2012;Pöschl and Shiraiwa, 2015;Shiraiwa et al, 2017;Shrivastava et al, 2017a, b). Despite the importance of SOA, many of the physicochemical properties of SOA remain poorly understood.…”

Section: Introductionmentioning

confidence: 99%

Liquid–liquid phase separation and viscosity within secondary organic aerosol generated from diesel fuel vapors

et al. 2019

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Abstract. Information on liquid–liquid phase separation (LLPS) and viscosity (or diffusion) within secondary organic aerosol (SOA) is needed to improve predictions of particle size, mass, reactivity, and cloud nucleating properties in the atmosphere. Here we report on LLPS and viscosities within SOA generated by the photooxidation of diesel fuel vapors. Diesel fuel contains a wide range of volatile organic compounds, and SOA generated by the photooxidation of diesel fuel vapors may be a good proxy for SOA from anthropogenic emissions. In our experiments, LLPS occurred over the relative humidity (RH) range of ∼70 % to ∼100 %, resulting in an organic-rich outer phase and a water-rich inner phase. These results may have implications for predicting the cloud nucleating properties of anthropogenic SOA since the presence of an organic-rich outer phase at high-RH values can lower the supersaturation with respect to water required for cloud droplet formation. At ≤10 % RH, the viscosity was ≥1×108 Pa s, which corresponds to roughly the viscosity of tar pitch. At 38 %–50 % RH, the viscosity was in the range of 1×108 to 3×105 Pa s. These measured viscosities are consistent with predictions based on oxygen to carbon elemental ratio (O:C) and molar mass as well as predictions based on the number of carbon, hydrogen, and oxygen atoms. Based on the measured viscosities and the Stokes–Einstein relation, at ≤10 % RH diffusion coefficients of organics within diesel fuel SOA is ≤5.4×10-17 cm2 s−1 and the mixing time of organics within 200 nm diesel fuel SOA particles (τmixing) is 50 h. These small diffusion coefficients and large mixing times may be important in laboratory experiments, where SOA is often generated and studied using low-RH conditions and on timescales of minutes to hours. At 38 %–50 % RH, the calculated organic diffusion coefficients are in the range of 5.4×10-17 to 1.8×10-13 cm2 s−1 and calculated τmixing values are in the range of ∼0.01 h to ∼50 h. These values provide important constraints for the physicochemical properties of anthropogenic SOA.

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“…Diffusion rates within SOA can also affect multi-phase reactions (Shiraiwa et al, 2011;Zhou et al, 2013;Steimer et al, 2014;Houle et al, 2015;Li et al, 2018), the extent of long-range transport of pollutants (Zelenyuk et al, 2012;Zhou et al, 2013;Mu et al, 2018), ice nucleation (Murray et al, 2010;Wang et al, 2012;Wilson et al, 2012;Ladino et al, 2014;Schill et al, 2014;Knopf et al, 2018), and crystalline of salts (Murray, 2008;Murray and Bertram, 2008;Bodsworth et al, 2010;Song et al, 2013;Ji et al, 2017;.…”

mentioning

confidence: 99%

Liquid-liquid phase separation and viscosity within secondary organic aerosol generated from diesel fuel vapors

Song¹,

Maclean²,

Huang³

et al. 2019

Preprint

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Abstract. Information on liquid-liquid phase separation (LLPS) and viscosity (or diffusion) within secondary organic aerosol (SOA) is needed to improve predictions of particle size, mass, reactivity, and cloud nucleating properties in the atmosphere. Here we report on LLPS and viscosities within SOA generated by the photooxidation of diesel fuel vapors. Diesel fuel contains a wide range of volatile organic compounds, and SOA generated by the photooxidation of diesel fuel vapors may be a good proxy for SOA from anthropogenic emissions. In our experiments, LLPS occurred over the relative humidity (RH) range of ~&#8201;70&#8201;% to ~&#8201;100&#8201;%, resulting in an organic-rich outer phase and a water-rich inner phase. These results may have implications for predicting the cloud nucleating properties of anthropogenic SOA since the organic-rich outer phase can lower the kinetic barrier for activation to a cloud droplet. At &#8804;&#8201;10&#8201;% RH, the viscosity was in the range of &#8805;&#8201;1&#8201;&#215;&#8201;108&#8201;Pa&#8201;s, which corresponds to roughly the viscosity of tar pitch. At 38&#8211;50&#8201;% RH the viscosity was in the range of 1&#8201;&#215;&#8201;108&#8211;3&#8201;&#215;&#8201;105&#8201;Pa&#8201;s. These measured viscosities are consistent with predictions based on oxygen to carbon elemental ratio (O&#8201;:&#8201;C) and molar mass as well as predictions based on the number of carbon, hydrogen, and oxygen atoms. Based on the measured viscosities and the Stokes&#8211;Einstein relation, at &#8804;&#8201;10&#8201;% RH diffusion coefficients of organics within diesel fuel SOA is &#8804;&#8201;5.4&#8201;&#215;&#8201;10&#8722;17cm2&#8201;s&#8722;1 and the mixing time of organics within 200&#8201;nm diesel fuel SOA particles (&#964;mixing) is &#8819;&#8201;50&#8201;h. These small diffusion coefficients and large mixing times may be important in laboratory experiments, where SOA is often generated and studied using low RH conditions and on time scales of minutes to hours. At 38&#8211;50&#8201;% RH, the calculated organic diffusion coefficients are in the range of 5.4&#8201;&#215;&#8201;10&#8722;17 to 1.8&#8201;&#215;&#8201;10&#8722;13&#8201;cm2&#8201;s&#8722;1 and calculated &#964;mixing values are in the range of ~&#8201;0.01&#8201;h to ~&#8201;50&#8201;h. These values provide important constraints for the physicochemical properties of anthropogenic SOA.

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Crystal Nucleation and Crystal Growth and Mass Transfer in Internally Mixed Sucrose/NaNO₃ Particles

Cited by 20 publications

References 56 publications

Viscosity and phase state of aerosol particles consisting of sucrose mixed with inorganic salts

Viscosity and phase state of aerosol particles consisting of sucrose mixed with inorganic salts

Liquid–liquid phase separation and viscosity within secondary organic aerosol generated from diesel fuel vapors

Liquid-liquid phase separation and viscosity within secondary organic aerosol generated from diesel fuel vapors

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