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Hydrophobic Interactions in Salt Solutions

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Hydrophobic Interactions in Salt Solutions Hydrophobic Interactions in Salt Solutions Mehdi Azadi B.Sc., M.Sc. Chemical Engineering A thesis submitted for the degree of Doctor of Philosophy at The University of Queensland in 2016 School of Chemical Engineering Abstract The fundamental understanding of hydrophobic interactions and forces between hydrophobic (water-repellent) surfaces in water is central to many areas of daily activities in many industries. Examples are broad and range from dissolving oily drugs into aqueous solutions for delivery to the body to the coalescence or aggregation of air bubbles, droplets and solid particles dispersed in water. Recent studies show controversial effects of dissolved (hydrophobic) gases in the water on hydrophobic forces. This PhD project aims to further investigate the role of dissolved gases in hydrophobic interactions. The concentration of dissolved gases in water can be controlled using inorganic salt solutions, which possess different levels of gas solubility at different salt concentrations. The use of salt solutions can reduce the effect of the electrical repulsion between charged surfaces in water, allowing a better quantification of hydrophobic forces. Atomic Force Microscopy (AFM), with surface force measurement and surface imaging abilities, was used to study the interaction between hydrophobic surfaces. Force measurements were carried out in salt solutions and were quantified by comparing experimental data with the classical theory of colloid stability. The electrical double-layer force was quantified using numerical solutions of the Poisson-Boltzmann equation. Van der Waals forces were calculated by applying the Lifshitz-Hamaker theory, which is based on quantum mechanics. It was hypothesised that dissolved gases would accumulate at the interface between water and hydrophobic surface in the form of dense gas layer changing the structure of interfacial water molecules and their hydrogen bond network, and cause the hydrophobic attraction. The research also examined the effect of dissolved gases on the force between hydrophobic surfaces in various salt types including NaCl, LiCl, KCl, and CsCl. The results showed that increasing salt concentration, or equivalently decreasing gas solubility, decreased the range and magnitude of the force between hydrophobic surfaces. The behaviour was found to be consistent across different salts tested. There is limited evidence of the presence of an interactive force between hydrophobic solid surfaces in non-aqueous solutions. The interaction between hydrophobic surfaces was also studied in non-aqueous solutions including formamide and dimethyl sulfoxide (DMSO). The AFM force measurement results showed that there is a short-range attractive force between the hydrophobic solid surfaces in formamide, while no attraction was found in the DMSO solution. However, an attractive force was observed between the hydrophobic solid surfaces in DMSO solutions mixed ii with water at 50-50% and 25-75% DMSO-water mixtures. The results suggested that the solution bonding structure and the presence of dissolved gas molecules affect and control the interaction between the hydrophobic solid surfaces. This research provides further evidence that the short-range attraction between hydrophobic surfaces is affected by the presence of dissolved gases. The recommendations for future research include: studying the hydrophobic interactions in non-aqueous solutions, using ellipsometry to study the possibility of interfacial gas enrichment, using capillary tube and high speed camera to study hydrophobic interactions and effect of dissolved gases, and using in-situ surface enhance Raman spectroscopy to probe the possibility of presence of gas layer in the vicinity of hydrophobic surface. iii Declaration by author This thesis is composed of my original work and contains no material previously published or written by another person except where due reference has been made in the text. I have clearly stated the contribution by others to jointly-authored works that I have included in my thesis. I have clearly stated the contribution of others to my thesis as a whole, including statistical assistance, survey design, data analysis, significant technical procedures, professional editorial advice, and any other original research work used or reported in my thesis. The content of my thesis is the result of work I have carried out since the commencement of my research higher degree candidature and does not include a substantial part of work that has been submitted to qualify for the award of any other degree or diploma in any university or other tertiary institution. I have clearly stated which parts of my thesis, if any, have been submitted to qualify for another award. I acknowledge that an electronic copy of my thesis must be lodged with the University Library and, subject to the policy and procedures of The University of Queensland, the thesis be made available for research and study in accordance with the Copyright Act 1968 unless a period of embargo has been approved by the Dean of the Graduate School. I acknowledge that copyright of all material contained in my thesis resides with the copyright holder(s) of that material. Where appropriate I have obtained copyright permission from the copyright holder to reproduce material in this thesis. iv Publications during candidature Mehdi Azadi, Anh Nguyen, Gleb Yakubov (2015). "Attractive forces between hydrophobic solid surfaces measured by AFM on the first approach in salt solutions and in the presence of dissolved gases." Langmuir 31(6): 1941-1949. v Publications included in this thesis Mehdi Azadi, Anh Nguyen, Gleb Yakubov (2015). "Attractive forces between hydrophobic solid surfaces measured by AFM on the first approach in salt solutions and in the presence of dissolved gases." Langmuir 31(6): 1941-1949. 50% is incorporated in Chapter 4. Contributor Statement of contribution Mehdi Azadi (Candidate) Designed experiments (90%) Conducting the experiments (100%) Wrote the paper (60%) Anh Nguyen Designed experiments (10%) Wrote and edited paper (20%) Gleb Yakubov Wrote and edited paper (20%) vi Contributions by others to the thesis None Statement of parts of the thesis submitted to qualify for the award of another degree None vii Acknowledgements I would like to express my gratitude to my principal supervisor Professor Anh V. Nguyen. I would also like to extend my appreciation to my co-supervisor Dr Gleb Yakubov. I would not have made it this far if it was not for their support and guidance during my PhD. I would like to gratefully acknowledge the financial support from The University of Queensland with the International Postgraduate Research Scholarship (IPRS), and UQ Centennial Scholarship (UQCent). I would also like to thank my family: my mother and father for their never ending love and support during all these years, and my brother for always being there for me when I needed his support. Last but not the least, I would like to mention that I moved to Australia to do my PhD and follow my dreams for research. However, I was so fortunate to meet Alycia, a precious dream far beyond imagination. I would like to thank my dearest Alycia for her unconditional love and support during this PhD journey. I would like to dedicate this work to my parents (Zahra and Mohammadtaghi), brother (Mohsen), and Alycia. viii Keywords Hydrophobic interaction, salt, dissolved gas, AFM, IGE, DLVO, surface forces Australian and New Zealand Standard Research Classifications (ANZSRC) ANZSRC code: 090499, Chemical Engineering not elsewhere classified, 100% Fields of Research (FoR) Classification FoR code: 0904, Chemical Engineering, 100% ix Table of Contents Abstract ....................................................................................................................... ii Declaration by author ................................................................................................. iv Publications during candidature ................................................................................. v Publications included in this thesis ............................................................................. vi Contributions by others to the thesis ......................................................................... vii Statement of parts of the thesis submitted to qualify for the award of another degree .................................................................................................................................. vii Acknowledgements .................................................................................................. viii Keywords ................................................................................................................... ix Australian and New Zealand Standard Research Classifications (ANZSRC) ............. ix Fields of Research (FoR) Classification ..................................................................... ix Table of Contents ....................................................................................................... x List of Figures ........................................................................................................... xiii List of Tables .......................................................................................................... xviii Chapter 1 ................................................................................................................... 1 Introduction ...............................................................................................................
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