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Molecular Interactions in Surfactant Solutions: from Micelles to Microemulsions

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Molecular Interactions in Surfactant Solutions: from Micelles to Microemulsions MOLECULAR INTERACTIONS IN SURFACTANT SOLUTIONS: FROM MICELLES TO MICROEMULSIONS By MONICA A. JAMES-SMITH A DISSERTATION PRESENTED TO THE GRADUATE SCHOOL OF THE UNIVERSITY OF FLORIDA IN PARTIAL FULFILLMENT OF THE REQUIREMENTS FOR THE DEGREE OF DOCTOR OF PHILOSOPHY UNIVERSITY OF FLORIDA 2006 1 Copyright 2006 by Monica A. James-Smith 2 To my parents who have been my #1 supporters since October 17, 1977. 3 ACKNOWLEDGMENTS I thank my Almighty Heavenly Father for allowing me to make it to this point and for seeing me through every obstacle that arose. I am forever grateful to my husband, Rod, for all of his support, love and encouragement. I sincerely thank my parents, Dan and Elaine James, for always believing in me, for their constant prayers, and for always providing the right words when the journey seemed difficult. I would like to thank Melanie, Dan, Chris, and Bruce for knowing how to make me feel like I can accomplish anything. I owe a huge debt of gratitude to my best friend, Brandi Chestang, who has been there to answer every phone call and has cheered me on all my life. I am also greatly appreciative to all of my other friends, family, and loved ones. I must also extend my sincerest appreciation to my in-laws who have taken me in as a family member and provided tremendous support as I have pursued this degree. I am forever grateful to Dr. Dinesh O. Shah for being a mentor, an advisor, and a confidant, for providing me with the highest caliber of guidance and for always pushing me towards greatness. I would like to extend sincerest thanks to Drs. Brij Moudgil, Manoj Varshney, Yakov Rabinovich, Anuj Chauhan, Oscar Crisalle, Ranga Narayanan, Donn Dennis, and Richard Dickenson for stimulating conversation and insightful comments and suggestions. I also would like to thank all of my colleagues who have been of great assistance throughout me years here at UF. Last, but definitely not least, I would like to thank Pastor Kevin W. Thorpe and the Faith Baptist Church family for showing me that my family is bigger than I think and for helping me to make it through this journey. 4 TABLE OF CONTENTS page ACKNOWLEDGMENTS ...............................................................................................................4 LIST OF TABLES...........................................................................................................................8 LIST OF FIGURES .........................................................................................................................9 ABSTRACT...................................................................................................................................12 CHAPTER 1 LITERATURE REVIEW .......................................................................................................14 1.1 Micelles.............................................................................................................................14 1.1.1 Introduction ............................................................................................................14 1.1.2 Dynamic Nature of Micellar Solutions...................................................................18 1.2 Macroemulsions................................................................................................................24 1.2.1 Emulsion Droplet Size............................................................................................26 1.2.2 Viscosity of Emulsions...........................................................................................28 1.2.3 Determination of Emulsion Type (O/W or W/O)...................................................28 1.2.4 Emulsion Stability ..................................................................................................29 1.2.4.1 Coalescence..................................................................................................29 1.2.4.2 Charge stabilization: The electrical double layer.........................................30 1.2.4.3 Phase inversion in emulsions .......................................................................31 1.2.4.4 Emulsion creaming.......................................................................................31 1.2.5 Demulsification ......................................................................................................32 1.2.6 Surfactant Selection for Emulsification..................................................................33 1.2.7 Applications of Emulsions .....................................................................................34 1.3 Microemulsions ................................................................................................................35 1.3.1 Formation of Microemulsions ................................................................................41 1.3.2 Applications of Microemulsions ............................................................................42 1.3.3 Nano-emulsions......................................................................................................42 2 A NOVEL METHOD TO ELUCIDATE THE PRESENCE OF SUB-MICELLAR AGGREGATES IN SURFACTANT SOLUTIONS..............................................................61 2.1 Introduction.......................................................................................................................61 2.2 Experimental Procedure....................................................................................................63 2.2.1 Materials.................................................................................................................63 2.2.2 Ultracentrifugation .................................................................................................63 2.2.3 Two-Phase Dye Transfer (Methylene Blue Complexation) and UV-Vis Analysis........................................................................................................................64 2.2.4 Foamability.............................................................................................................64 2.2.5 Fabric Wetting........................................................................................................65 2.2.6 Dynamic Surface Tension ......................................................................................65 5 2.3 Results and Discussion .....................................................................................................65 2.3.1 SDS Surfactant Solutions .......................................................................................65 2.3.2 Effect of Counter-Ions on Sub-Micellar Aggregate Concentration .......................73 2.3.3 Importance of Sub-Micellar Aggregates in Technological Processes....................75 2.3.3.1 Foaming........................................................................................................76 2.3.3.2 Fabric wetting...............................................................................................77 2.3.3.3 Dynamic surface tension ..............................................................................77 2.4 Conclusions.......................................................................................................................78 3 DETERMINATION OF DRUG AND FATTY ACID BINDING CAPACITY TO PLURONIC F127 IN MICROEMULSIONS FOR DETOXIFICATION..............................94 3.1 Introduction.......................................................................................................................94 3.2 Experimental Procedure....................................................................................................96 3.2.1 Materials.................................................................................................................96 3.2.2 Microemulsion Preparation ....................................................................................96 3.2.3 Turbidity Analysis..................................................................................................96 3.2.4 Dynamic Surface Tension ......................................................................................97 3.2.5 Foamability.............................................................................................................97 3.2.6 Fabric Wetting........................................................................................................98 3.2.7 Surface Tension......................................................................................................98 3.3 Results and Discussion .....................................................................................................98 3.3.1 Effect of Sodium Caprylate Concentration on Drug and Fatty Acid Binding to Microemulsions............................................................................................................98 3.3.2 Determination of Free Fatty Acid by Dynamic Processes ...................................101 3.3.3 Effect of Fatty Acid Chain Length on Drug and Fatty Acid Binging to Microemulsions..........................................................................................................104 3.3.4 Effect of the Number of Ethylene Oxide (EO) and Propylene Oxide (PO) Groups of Pluronics on Fatty Acid and Drug Binding ..............................................105 3.4 Conclusions.....................................................................................................................106 4 A Novel Method to Quantify the Amount of Surfactant at the Oil/Water Interface
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