Controlled vapor deposition of azide-terminated siloxane monolayers : a platform for tailoring oxide surfaces
Abstract/Contents
- Abstract
- The controlled deposition of mixed, azide-terminated siloxane monolayers onto oxide surfaces provides a platform for the covalent attachment of alkyne-terminated species such as oligonucleotides using the copper-catalyzed azide-alkyne cycloaddition (CuAAC) reaction. A convenient method for the vapor deposition of dense siloxane monolayers onto oxide surfaces was developed. A selectively deuterated silane, (CD3O)3-Si-(CH2)13-CH3, was synthesized and then vapor deposited in the presence of controlled amounts of water vapor from the in situ dehydration of MgSO4[multiplication dot]7H2O at 110°C. Monolayer densification was characterized using ellipsometry, Fourier transform infrared (FTIR) spectroscopy, water contact angle, and electrochemical capacitance measurements. The formation of dense, completely hydrolyzed monolayers required excess amounts of silane and water reactants. The optimized vapor deposition conditions were used to form mixed, azide-terminated monolayers. Dilution of the azide groups with unreactive methyl groups was achieved from the co-deposition of two silanes. Enrichment of the monolayers with the higher vapor pressure silane reactant was observed. Quantitative CuAAC reactions of the azide groups in mixed monolayers were demonstrated with azide surface compositions up to approximately 40%. Steric hindrance presumably prevented the quantitative reaction of a purely azide-terminated monolayer. Alkyne-terminated oligonucleotides were covalently attached to azide-terminated monolayers on glass followed by hybridization with complementary oligonucleotides. However, the azide-terminated monolayers were susceptible to the nonspecific adsorption of oligonucleotides even after thorough rinsing in aqueous detergents and buffers. A two-step reaction sequence was developed that involved one CuAAC reaction to attach oligonucleotides at low density followed by a second CuAAC reaction with ethynyl phosphonic acid to make the surface more resistant to nonspecific adsorption.
Description
| Type of resource | text |
|---|---|
| Form | electronic; electronic resource; remote |
| Extent | 1 online resource. |
| Publication date | 2011 |
| Issuance | monographic |
| Language | English |
Creators/Contributors
| Associated with | Lowe, Randall Dewayne, Jr |
|---|---|
| Associated with | Stanford University, Department of Chemical Engineering |
| Primary advisor | Bao, Zhenan |
| Primary advisor | Chidsey, Christopher E. D. (Christopher Elisha Dunn) |
| Thesis advisor | Bao, Zhenan |
| Thesis advisor | Chidsey, Christopher E. D. (Christopher Elisha Dunn) |
| Thesis advisor | Frank, C. W |
| Advisor | Frank, C. W |
Subjects
| Genre | Theses |
|---|
Bibliographic information
| Statement of responsibility | Randall Dewayne Lowe, Jr. |
|---|---|
| Note | Submitted to the Department of Chemical Engineering. |
| Thesis | Thesis (Ph.D.)--Stanford University, 2011. |
| Location | electronic resource |
Access conditions
- Copyright
- © 2011 by Randall Dewayne Lowe
- License
- This work is licensed under a Creative Commons Attribution Non Commercial 3.0 Unported license (CC BY-NC).
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