Self-Assembly Formation of Lipid Bilayer Coatings on Bare Aluminum Oxide: Overcoming the Force of Interfacial Water

Widely used in catalysis and biosensing applications, aluminum oxide has become popular for surface functionalization with biological macromolecules, including lipid bilayer coatings. However, it is difficult to form supported lipid bilayers on aluminum oxide, and current methods require covalent su...

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Main Authors: Jackman, Joshua Alexander, Tabaei, Seyed Ruhollah, Zhao, Zhilei, Yorulmaz, Saziye, Cho, Nam-Joon
Other Authors: School of Chemical and Biomedical Engineering
Format: Journal Article
Language:English
Published: 2016
Subjects:
Online Access:https://hdl.handle.net/10356/80930
http://hdl.handle.net/10220/40631
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author Jackman, Joshua Alexander
Tabaei, Seyed Ruhollah
Zhao, Zhilei
Yorulmaz, Saziye
Cho, Nam-Joon
author2 School of Chemical and Biomedical Engineering
author_facet School of Chemical and Biomedical Engineering
Jackman, Joshua Alexander
Tabaei, Seyed Ruhollah
Zhao, Zhilei
Yorulmaz, Saziye
Cho, Nam-Joon
author_sort Jackman, Joshua Alexander
collection NTU
description Widely used in catalysis and biosensing applications, aluminum oxide has become popular for surface functionalization with biological macromolecules, including lipid bilayer coatings. However, it is difficult to form supported lipid bilayers on aluminum oxide, and current methods require covalent surface modification, which masks the interfacial properties of aluminum oxide, and/or complex fabrication techniques with specific conditions. Herein, we addressed this issue by identifying simple and robust strategies to form fluidic lipid bilayers on aluminum oxide. The fabrication of a single lipid bilayer coating was achieved by two methods, vesicle fusion under acidic conditions and solvent-assisted lipid bilayer (SALB) formation under near-physiological pH conditions. Importantly, quartz crystal microbalance with dissipation (QCM-D) monitoring measurements determined that the hydration layer of a supported lipid bilayer on aluminum oxide is appreciably thicker than that of a bilayer on silicon oxide. Fluorescence recovery after photobleaching (FRAP) analysis indicated that the diffusion coefficient of lateral lipid mobility was up to 3-fold greater on silicon oxide than on aluminum oxide. In spite of this hydrodynamic coupling, the diffusion coefficient on aluminum oxide, but not silicon oxide, was sensitive to the ionic strength condition. Extended-DLVO model calculations estimated the thermodynamics of lipid–substrate interactions on aluminum oxide and silicon oxide, and predict that the range of the repulsive hydration force is greater on aluminum oxide, which in turn leads to an increased equilibrium separation distance. Hence, while a strong hydration force likely contributes to the difficulty of bilayer fabrication on aluminum oxide, it also confers advantages by stabilizing lipid bilayers with thicker hydration layers due to confined interfacial water. Such knowledge provides the basis for improved surface functionalization strategies on aluminum oxide, underscoring the practical importance of surface hydration.
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spelling ntu-10356/809302020-06-01T10:21:28Z Self-Assembly Formation of Lipid Bilayer Coatings on Bare Aluminum Oxide: Overcoming the Force of Interfacial Water Jackman, Joshua Alexander Tabaei, Seyed Ruhollah Zhao, Zhilei Yorulmaz, Saziye Cho, Nam-Joon School of Chemical and Biomedical Engineering School of Materials Science & Engineering Centre for Biomimetic Sensor Science Surface coating Biofunctionalization Supported lipid bilayer Interfacial forces Self-assembly Aluminum oxide Widely used in catalysis and biosensing applications, aluminum oxide has become popular for surface functionalization with biological macromolecules, including lipid bilayer coatings. However, it is difficult to form supported lipid bilayers on aluminum oxide, and current methods require covalent surface modification, which masks the interfacial properties of aluminum oxide, and/or complex fabrication techniques with specific conditions. Herein, we addressed this issue by identifying simple and robust strategies to form fluidic lipid bilayers on aluminum oxide. The fabrication of a single lipid bilayer coating was achieved by two methods, vesicle fusion under acidic conditions and solvent-assisted lipid bilayer (SALB) formation under near-physiological pH conditions. Importantly, quartz crystal microbalance with dissipation (QCM-D) monitoring measurements determined that the hydration layer of a supported lipid bilayer on aluminum oxide is appreciably thicker than that of a bilayer on silicon oxide. Fluorescence recovery after photobleaching (FRAP) analysis indicated that the diffusion coefficient of lateral lipid mobility was up to 3-fold greater on silicon oxide than on aluminum oxide. In spite of this hydrodynamic coupling, the diffusion coefficient on aluminum oxide, but not silicon oxide, was sensitive to the ionic strength condition. Extended-DLVO model calculations estimated the thermodynamics of lipid–substrate interactions on aluminum oxide and silicon oxide, and predict that the range of the repulsive hydration force is greater on aluminum oxide, which in turn leads to an increased equilibrium separation distance. Hence, while a strong hydration force likely contributes to the difficulty of bilayer fabrication on aluminum oxide, it also confers advantages by stabilizing lipid bilayers with thicker hydration layers due to confined interfacial water. Such knowledge provides the basis for improved surface functionalization strategies on aluminum oxide, underscoring the practical importance of surface hydration. NRF (Natl Research Foundation, S’pore) NMRC (Natl Medical Research Council, S’pore) 2016-06-07T07:51:29Z 2019-12-06T14:17:38Z 2016-06-07T07:51:29Z 2019-12-06T14:17:38Z 2014 Journal Article Jackman, J. A., Tabaei, S. R., Zhao, Z., Yorulmaz, S., & Cho, N.-J. (2015). Self-Assembly Formation of Lipid Bilayer Coatings on Bare Aluminum Oxide: Overcoming the Force of Interfacial Water. ACS Applied Materials & Interfaces, 7(1), 959-968. 1944-8244 https://hdl.handle.net/10356/80930 http://hdl.handle.net/10220/40631 10.1021/am507651h en ACS Applied Materials & Interfaces © 2014 American Chemical Society
spellingShingle Surface coating
Biofunctionalization
Supported lipid bilayer
Interfacial forces
Self-assembly
Aluminum oxide
Jackman, Joshua Alexander
Tabaei, Seyed Ruhollah
Zhao, Zhilei
Yorulmaz, Saziye
Cho, Nam-Joon
Self-Assembly Formation of Lipid Bilayer Coatings on Bare Aluminum Oxide: Overcoming the Force of Interfacial Water
title Self-Assembly Formation of Lipid Bilayer Coatings on Bare Aluminum Oxide: Overcoming the Force of Interfacial Water
title_full Self-Assembly Formation of Lipid Bilayer Coatings on Bare Aluminum Oxide: Overcoming the Force of Interfacial Water
title_fullStr Self-Assembly Formation of Lipid Bilayer Coatings on Bare Aluminum Oxide: Overcoming the Force of Interfacial Water
title_full_unstemmed Self-Assembly Formation of Lipid Bilayer Coatings on Bare Aluminum Oxide: Overcoming the Force of Interfacial Water
title_short Self-Assembly Formation of Lipid Bilayer Coatings on Bare Aluminum Oxide: Overcoming the Force of Interfacial Water
title_sort self assembly formation of lipid bilayer coatings on bare aluminum oxide overcoming the force of interfacial water
topic Surface coating
Biofunctionalization
Supported lipid bilayer
Interfacial forces
Self-assembly
Aluminum oxide
url https://hdl.handle.net/10356/80930
http://hdl.handle.net/10220/40631
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