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12-1-2014 Master Thesis.pdf (2.08 MB)

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Ionically Crosslinked Polymer Networks for Underwater Adhesion and Long-Term Controlled Release

Lawrence, Patrick G.
http://rave.ohiolink.edu/etdc/view?acc_num=toledo1417437994

Abstract Details

2014, Master of Science, University of Toledo, Chemical Engineering.
Underwater adhesives have several potential applications in industry as well as in medicine. Much of the recent research in this area has focused on adhesive preparation from biological or custom-designed biomimetic polymers. As a simpler alternative, we have recently shown that ionically crosslinked, gel-like underwater adhesive complexes can be prepared by the mixing of the readily-available and inexpensive polyelectrolyte, poly(allylamine hydrochloride) (PAH), with commonly-used multivalent anions, pyrophosphate (PPi) and tripolyphosphate (TPP). Remarkably, these gel-like complexes adhere to both hydrophilic and hydrophobic substrates under water with tensile adhesive strength considerably greater than that of Scotch Permanent Double Sided Tape (up to ~400 kPa vs. ~85 kPa when used as a pressure-sensitive adhesives) and due to the reversible nature of the ionic crosslinks, self-heal when torn. These complexes also exhibit very high storage moduli (greater than 100 kPa), indicative of a very high crosslink density. The high crosslink density allow these gel-like complexes to also entrap and deliver small molecule payloads over multiple-month timescales. Moreover, their formation and rheological/adhesion properties can be controlled using external stimuli (pH and ionic strength). In this thesis we characterize formation and rheological/adhesion properties of gel-like PAH/PPi and PAH/TPP complexes the through the use of dynamic and electrophoretic light scattering, rheology and tensile adhesion tests. We also describe their sensitivity to pH and ionic strength, and explain how the complexes can be dissolved on demand by raising or lowering the ambient pH, and can form spontaneously by increasing the NaCl concentration (which can be used for developing injectable underwater adhesive formulations). Finally, we demonstrate the ability of these adhesives to release small molecule payloads over multiple-month timescales by characterizing their ability to take up and release small molecule dyes (Fast Green FCF and Rhodamine B).
Yakov Lapitsky, PhD (Committee Chair)
Isabel Escobar, PhD (Committee Member)
Youngwoo Seo, PhD (Committee Member)
135 p.
Chemical Engineering; Chemistry; Materials Science; Polymer Chemistry; Polymers
Ionic Crosslinking; Polyelectrolytes; Underwater Adhesion; Stimulus-Responsive; Controlled Release

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Citations

  • Lawrence, P. G. (2014). Ionically Crosslinked Polymer Networks for Underwater Adhesion and Long-Term Controlled Release [Master's thesis, University of Toledo]. OhioLINK Electronic Theses and Dissertations Center. http://rave.ohiolink.edu/etdc/view?acc_num=toledo1417437994

    APA Style (7th edition)

  • Lawrence, Patrick . Ionically Crosslinked Polymer Networks for Underwater Adhesion and Long-Term Controlled Release. 2014. University of Toledo, Master's thesis. OhioLINK Electronic Theses and Dissertations Center, http://rave.ohiolink.edu/etdc/view?acc_num=toledo1417437994.

    MLA Style (8th edition)

  • Lawrence, Patrick . "Ionically Crosslinked Polymer Networks for Underwater Adhesion and Long-Term Controlled Release." Master's thesis, University of Toledo, 2014. http://rave.ohiolink.edu/etdc/view?acc_num=toledo1417437994

    Chicago Manual of Style (17th edition)

toledo1417437994
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This open access ETD is published by University of Toledo and OhioLINK.