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Plane microscopic observation on instability of double emulsion clusters

  • Department of Thermal Science and Energy Engineering, University of Science and Technology of China, Hefei 230027, China

Cite this:
https://doi.org/10.52396/JUST-2020-0023
  • Received Date: 19 December 2020
  • Rev Recd Date: 04 February 2021
  • Publish Date: 30 April 2021
    Abstract

  • Abstract

    Double emulsions have huge potential applications in many fields, but their wide use is limited by the instability. We have established a plane experimental observation method based on the microscope observation on the instability of double emulsion clusters to understand the key factors that affect the instability of droplets. A glass capillary device was used to produce the uniform monodisperse double emulsion droplets, and the dynamic information of the double emulsions was recorded through a microscope. We found that the instability of the double emulsions was caused together by diffusion and coalescence. And through the light curing experiment, the coalescence phenomenon of the internal droplets and the outer phase became visible. The experimental results show that the thicker the oil film thickness of the W/O/W droplets, the more difficult the coalescence of the inner droplets and the outer phase, and the more stable the double emulsions. The effect of glycerol on the stability of double emulsions was studied by changing the concentration of glycerol in the outer phase. We found that the stability time of the double emulsions increased with the decrease of the glycerol concentration, but when the glycerol concentration was reduced to 10 wt%, the stability of the double emulsions became worse. When the glycerol concentration was not less than 40 wt%, the instability of the double emulsions was more caused by the conversion of W/O/W droplets to O/W droplets. When the glycerol concentration was not more than 30 wt%, the instability of the double emulsions was more caused by the conversion of W/O/W droplets to W/W droplets. In addition, by using different surfactants, it was found that the double emulsions formulated with polyvinyl alcohol (PVA) had higher yield and a longer stable time.

    Abstract

    Double emulsions have huge potential applications in many fields, but their wide use is limited by the instability. We have established a plane experimental observation method based on the microscope observation on the instability of double emulsion clusters to understand the key factors that affect the instability of droplets. A glass capillary device was used to produce the uniform monodisperse double emulsion droplets, and the dynamic information of the double emulsions was recorded through a microscope. We found that the instability of the double emulsions was caused together by diffusion and coalescence. And through the light curing experiment, the coalescence phenomenon of the internal droplets and the outer phase became visible. The experimental results show that the thicker the oil film thickness of the W/O/W droplets, the more difficult the coalescence of the inner droplets and the outer phase, and the more stable the double emulsions. The effect of glycerol on the stability of double emulsions was studied by changing the concentration of glycerol in the outer phase. We found that the stability time of the double emulsions increased with the decrease of the glycerol concentration, but when the glycerol concentration was reduced to 10 wt%, the stability of the double emulsions became worse. When the glycerol concentration was not less than 40 wt%, the instability of the double emulsions was more caused by the conversion of W/O/W droplets to O/W droplets. When the glycerol concentration was not more than 30 wt%, the instability of the double emulsions was more caused by the conversion of W/O/W droplets to W/W droplets. In addition, by using different surfactants, it was found that the double emulsions formulated with polyvinyl alcohol (PVA) had higher yield and a longer stable time.
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    • References(36)
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    Niepa T H R, Hou L, Jiang H, et al. Microbial nanoculture as an artificial microniche. Sci Rep-Uk, 2016, 6(1): 30578.
    [2]
    Oh M J, Ryu T K, Choi S W. Hollow polydimethylsiloxane beads with a porous structure for cell encapsulation. Macromol Rapid Comm, 2013, 34(21): 1728-1733.
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    Tao Y, Rotem A, Zhang H, et al. Rapid, targeted and culture-free viral infectivity assay in drop-based microfluidics. Lab on a Chip, 2015, 15(19): 3934-3940.
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    Windbergs M, Zhao Y, Heyman J, et al. Biodegradable core-shell carriers for simultaneous encapsulation of synergistic actives. J. Am. Chem. Soc., 2013, 135(21): 7933-7937.
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    Kim S H, Park J G, Choi T M, et al. Osmotic-pressure-controlled concentration of colloidal particles in thin-shelled capsules. Nat. Commun., 2014, 5(1): 3068.
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    Yeo S J, Tu F, Kim S H, et al. Angle- and strain-independent coloured free-standing films incorporating non-spherical colloidal photonic crystals. Soft Matter, 2015, 11(8): 1582-1588.
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    Chen H, Zhao Y, Li J, et al. Reactions in double emulsions by flow-controlled coalescence of encapsulated drops. Lab on a Chip, 2011, 11(14): 2312-2315.
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    Guan X, Hou L, Ren Y, et al. A dual-core double emulsion platform for osmolarity-controlled microreactor triggered by coalescence of encapsulated droplets. Biomicrofluidics, 2016, 10(3): 034111.
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    Lee T Y, Praveenkumar R, Oh Y K, et al. Alginate microgels created by selective coalescence between core drops paired with an ultrathin shell. J. Mater. Chem. B, 2016, 4(19): 3232-3238.
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    Kim J H, Jeon T Y, Choi T M, et al. Droplet microfluidics for producing functional microparticles. Langmuir, 2014, 30(6): 1473-1488.
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    Abbaspourrad A, Carroll N J, Kim S H, et al. Polymer microcapsules with programmable active release. J. Am. Chem. Soc., 2013, 135(20): 7744-7750.
    [13]
    Abbaspourrad A, Datta S S, Weitz D A. Controlling release from pH-responsive microcapsules. Langmuir, 2013, 29(41): 12697-12702.
    [14]
    Amstad E, Kim S H, Weitz D A. Photo-and thermoresponsive polymersomes for triggered release. Angewandte Chemie International Edition, 2012, 51(50): 12499-12503.
    [15]
    Dilauro A M, Abbaspourrad A, Weitz D A, et al. Stimuli-responsive core-shell microcapsules with tunable rates of release by using a depolymerizable poly(phthalaldehyde) Membrane. Macromolecules, 2013, 46(9): 3309-3313.
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    Lensen D, Gelderblom E C, Vriezema D M, et al. Biodegradable polymeric microcapsules for selective ultrasound-triggered drug release. Soft Matter, 2011, 7(11): 5417-5422.
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    Florence A T, Whitehill D. The formulation and stability of multiple emulsions. Int J Pharm, 1982, 11(4): 277-308.
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    Garti N. Double emulsions—scope, limitations and new achievements. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 1997, 123-124: 233-246.
    [19]
    Okushima S, Nisisako T, Torii T, et al. Controlled production of monodisperse double emulsions by two-step droplet breakup in microfluidic devices. Langmuir, 2004, 20(23): 9905-9908.
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    Chu L Y, Utada A S, Shah R K, et al. Controllable monodisperse multiple emulsions. Angewandte Chemie International Edition, 2007, 46(47): 8970-8974.
    [21]
    Utada A S, Lorenceau E, Link D R, et al. Monodisperse double emulsions generated from a microcapillary device. Science, 2005, 308(5721): 537.
    [22]
    Ficheux M F, Bonakdar L, Leal-Calderon F, et al. Some stability criteria for double emulsions. Langmuir, 1998, 14(10): 2702-2706.
    [23]
    Schmidts T, Dobler D, Nissing C, et al. Influence of hydrophilic surfactants on the properties of multiple W/O/W emulsions. J. Colloid. Interf. Sci., 2009, 338(1): 184-192.
    [24]
    Hou L, Ren Y, Jia Y, et al. Osmolarity-controlled swelling behaviors of dual-cored double-emulsion drops. Microfluid Nanofluid, 2017, 21(4): 60.
    [25]
    Bouyer E, Mekhloufi G, Rosilio V, et al. Proteins, polysaccharides, and their complexes used as stabilizers for emulsions: Alternatives to synthetic surfactants in the pharmaceutical field? Int. J. Pharm., 2012, 436(1): 359-378.
    [26]
    Zhu Q, Qiu S, Zhang H, et al. Physical stability, microstructure and micro-rheological properties of water-in-oil-in-water (W/O/W) emulsions stabilized by porcine gelatin. Food Chem., 2018, 253: 63-70.
    [27]
    Frasch-Melnik S, Norton I T, Spyropoulos F. Fat-crystal stabilised W/O emulsions for controlled salt release. J. Food Eng., 2010, 98(4): 437-442.
    [28]
    Pawlik A, Cox P W, Norton I T. Food grade duplex emulsions designed and stabilised with different osmotic pressures. J. Colloid. Interf. Sci., 2010, 352(1): 59-67.
    [29]
    Márquez A L, Medrano A, Panizzolo L A, et al. Effect of calcium salts and surfactant concentration on the stability of water-in-oil (W/O) emulsions prepared with polyglycerol polyricinoleate. J. Colloid. Interf. Sci., 2010, 341(1): 101-108.
    [30]
    Florence A T, Whitehill D. Stabilization of water/oil/water multiple emulsions by polymerization of the aqueous phases. Journal of Pharmacy and Pharmacology, 1982, 34(11): 687-691.
    [31]
    Koroleva M Y, Yurtov E V. Effect of ionic strength of dispersed phase on ostwald ripening in water-in-oil emulsions. Colloid Journal, 2003, 65(1): 40-43.
    [32]
    Oron A, Davis S H, Bankoff S G. Long-scale evolution of thin liquid films. Reviews of Modern Physics, 1997, 69(3): 931-980.
    [33]
    González-Ochoa H, Ibarra-Bracamontes L, Arauz-Lara J L. Two-stage coalescence in double emulsions. Langmuir, 2003, 19(19): 7837-7840.
    [34]
    Takamura K, Fischer H, Morrow N R. Physical properties of aqueous glycerol solutions. J. Petrol. Sci. Eng., 2012, 98-99: 50-60.
    [35]
    Oppermann A K L, Noppers J M E, Stieger M, et al. Effect of outer water phase composition on oil droplet size and yield of (W1/O/W2) double emulsions. Food Res. Int., 2018, 107: 148-157.
    [36]
    Magdassi S, Frank S G.Formation of oil-in-glycerol/water emulsions. J. Disper. Sci. Technol., 1986, 7(5): 599-612.
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    [1]
    Niepa T H R, Hou L, Jiang H, et al. Microbial nanoculture as an artificial microniche. Sci Rep-Uk, 2016, 6(1): 30578.
    [2]
    Oh M J, Ryu T K, Choi S W. Hollow polydimethylsiloxane beads with a porous structure for cell encapsulation. Macromol Rapid Comm, 2013, 34(21): 1728-1733.
    [3]
    Tao Y, Rotem A, Zhang H, et al. Rapid, targeted and culture-free viral infectivity assay in drop-based microfluidics. Lab on a Chip, 2015, 15(19): 3934-3940.
    [4]
    Windbergs M, Zhao Y, Heyman J, et al. Biodegradable core-shell carriers for simultaneous encapsulation of synergistic actives. J. Am. Chem. Soc., 2013, 135(21): 7933-7937.
    [5]
    Kim S H, Park J G, Choi T M, et al. Osmotic-pressure-controlled concentration of colloidal particles in thin-shelled capsules. Nat. Commun., 2014, 5(1): 3068.
    [6]
    Yeo S J, Tu F, Kim S H, et al. Angle- and strain-independent coloured free-standing films incorporating non-spherical colloidal photonic crystals. Soft Matter, 2015, 11(8): 1582-1588.
    [7]
    Chen H, Zhao Y, Li J, et al. Reactions in double emulsions by flow-controlled coalescence of encapsulated drops. Lab on a Chip, 2011, 11(14): 2312-2315.
    [8]
    Guan X, Hou L, Ren Y, et al. A dual-core double emulsion platform for osmolarity-controlled microreactor triggered by coalescence of encapsulated droplets. Biomicrofluidics, 2016, 10(3): 034111.
    [9]
    Lee T Y, Praveenkumar R, Oh Y K, et al. Alginate microgels created by selective coalescence between core drops paired with an ultrathin shell. J. Mater. Chem. B, 2016, 4(19): 3232-3238.
    [10]
    Brugarolas T, Park B J, Lee M H, et al. Generation ofamphiphilic Janus Bubbles and their behavior at an air-water interface. Adv. Funct. Mater., 2011, 21(20): 3924-3931.
    [11]
    Kim J H, Jeon T Y, Choi T M, et al. Droplet microfluidics for producing functional microparticles. Langmuir, 2014, 30(6): 1473-1488.
    [12]
    Abbaspourrad A, Carroll N J, Kim S H, et al. Polymer microcapsules with programmable active release. J. Am. Chem. Soc., 2013, 135(20): 7744-7750.
    [13]
    Abbaspourrad A, Datta S S, Weitz D A. Controlling release from pH-responsive microcapsules. Langmuir, 2013, 29(41): 12697-12702.
    [14]
    Amstad E, Kim S H, Weitz D A. Photo-and thermoresponsive polymersomes for triggered release. Angewandte Chemie International Edition, 2012, 51(50): 12499-12503.
    [15]
    Dilauro A M, Abbaspourrad A, Weitz D A, et al. Stimuli-responsive core-shell microcapsules with tunable rates of release by using a depolymerizable poly(phthalaldehyde) Membrane. Macromolecules, 2013, 46(9): 3309-3313.
    [16]
    Lensen D, Gelderblom E C, Vriezema D M, et al. Biodegradable polymeric microcapsules for selective ultrasound-triggered drug release. Soft Matter, 2011, 7(11): 5417-5422.
    [17]
    Florence A T, Whitehill D. The formulation and stability of multiple emulsions. Int J Pharm, 1982, 11(4): 277-308.
    [18]
    Garti N. Double emulsions—scope, limitations and new achievements. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 1997, 123-124: 233-246.
    [19]
    Okushima S, Nisisako T, Torii T, et al. Controlled production of monodisperse double emulsions by two-step droplet breakup in microfluidic devices. Langmuir, 2004, 20(23): 9905-9908.
    [20]
    Chu L Y, Utada A S, Shah R K, et al. Controllable monodisperse multiple emulsions. Angewandte Chemie International Edition, 2007, 46(47): 8970-8974.
    [21]
    Utada A S, Lorenceau E, Link D R, et al. Monodisperse double emulsions generated from a microcapillary device. Science, 2005, 308(5721): 537.
    [22]
    Ficheux M F, Bonakdar L, Leal-Calderon F, et al. Some stability criteria for double emulsions. Langmuir, 1998, 14(10): 2702-2706.
    [23]
    Schmidts T, Dobler D, Nissing C, et al. Influence of hydrophilic surfactants on the properties of multiple W/O/W emulsions. J. Colloid. Interf. Sci., 2009, 338(1): 184-192.
    [24]
    Hou L, Ren Y, Jia Y, et al. Osmolarity-controlled swelling behaviors of dual-cored double-emulsion drops. Microfluid Nanofluid, 2017, 21(4): 60.
    [25]
    Bouyer E, Mekhloufi G, Rosilio V, et al. Proteins, polysaccharides, and their complexes used as stabilizers for emulsions: Alternatives to synthetic surfactants in the pharmaceutical field? Int. J. Pharm., 2012, 436(1): 359-378.
    [26]
    Zhu Q, Qiu S, Zhang H, et al. Physical stability, microstructure and micro-rheological properties of water-in-oil-in-water (W/O/W) emulsions stabilized by porcine gelatin. Food Chem., 2018, 253: 63-70.
    [27]
    Frasch-Melnik S, Norton I T, Spyropoulos F. Fat-crystal stabilised W/O emulsions for controlled salt release. J. Food Eng., 2010, 98(4): 437-442.
    [28]
    Pawlik A, Cox P W, Norton I T. Food grade duplex emulsions designed and stabilised with different osmotic pressures. J. Colloid. Interf. Sci., 2010, 352(1): 59-67.
    [29]
    Márquez A L, Medrano A, Panizzolo L A, et al. Effect of calcium salts and surfactant concentration on the stability of water-in-oil (W/O) emulsions prepared with polyglycerol polyricinoleate. J. Colloid. Interf. Sci., 2010, 341(1): 101-108.
    [30]
    Florence A T, Whitehill D. Stabilization of water/oil/water multiple emulsions by polymerization of the aqueous phases. Journal of Pharmacy and Pharmacology, 1982, 34(11): 687-691.
    [31]
    Koroleva M Y, Yurtov E V. Effect of ionic strength of dispersed phase on ostwald ripening in water-in-oil emulsions. Colloid Journal, 2003, 65(1): 40-43.
    [32]
    Oron A, Davis S H, Bankoff S G. Long-scale evolution of thin liquid films. Reviews of Modern Physics, 1997, 69(3): 931-980.
    [33]
    González-Ochoa H, Ibarra-Bracamontes L, Arauz-Lara J L. Two-stage coalescence in double emulsions. Langmuir, 2003, 19(19): 7837-7840.
    [34]
    Takamura K, Fischer H, Morrow N R. Physical properties of aqueous glycerol solutions. J. Petrol. Sci. Eng., 2012, 98-99: 50-60.
    [35]
    Oppermann A K L, Noppers J M E, Stieger M, et al. Effect of outer water phase composition on oil droplet size and yield of (W1/O/W2) double emulsions. Food Res. Int., 2018, 107: 148-157.
    [36]
    Magdassi S, Frank S G.Formation of oil-in-glycerol/water emulsions. J. Disper. Sci. Technol., 1986, 7(5): 599-612.
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