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Computer Simulation and Mathematical Modeling of Reversibly Associated Polymers

Wang, Shihu
http://rave.ohiolink.edu/etdc/view?acc_num=case1275488088

Abstract Details

2010, Doctor of Philosophy, Case Western Reserve University, Macromolecular Science and Engineering.
Reversible and specific interactions have been employed extensively for the preparation of smart materials and biomaterials. Using computer simulation and mathematical modeling, we studied the equilibrium properties of different polymeric systems that utilize these interactions, including metal-ligand and ligand-receptor interactions. The equilibrium properties of metallo-supramolecular micelles formed by core- and corona- blocks connected via 2:1 ligand-metal complexes were studied by analyzing the competition of 2:1 and 1:1 metal-ligand complexation in the bulk and on the core surface as well as steric interactions between neighboring corona blocks attached to the surface. We found that increasing association energy for the second metal-ligand bond or decreasing corona block length can enhance the micelle core surface coverage. 3:1 ligand-metal complexation leads to the self-assembly of linear end-functionalized oligomers in solution and formation of a metallo-supramolecular network in a limited range of metal-to-oligomer ratios and at a sufficiently large oligomer concentration. We studied the conditions of network formation and investigated the properties of metallo-supramolecular networks, such as elastic plateau modulus, mesh-size and molecular weight between effective crosslinks. The obtained results were in qualitative agreement with experimental data. We showed that cis-trans isomerization of 2:1 ligand-metal complexes being in equilibrium with 3:1 ligand-metal complexes significantly affects self-assembly and network formation of metallo-supramolecular polymers. We predicted conditions when trans-cis isomerization can trigger sol-network transition and cause a significant change in materials properties. The molecular mechanisms of network transformation upon cis-trans isomerization were discussed. Ligand-receptor interactions have been employed to enhance the targeting efficiency of nanoparticles. We systematically studied the influence of different design parameters of a spherical nanoparticle tethered with monovalent ligands on its targeting efficiency to planar cell surfaces containing mobile receptors. Predictions were made regarding the preferable nanoparticle design to achieve high affinity of a nanoparticle to cell surface. We also discussed the selectivity of nanoparticle targeting to cells with a high receptor density and made recommendations for the desirable nanoparticle design to improve targeting selectivity.
Elena E. Dormidontova, PhD (Advisor)
Ica Manas-Zloczower, PhD (Committee Member)
Alexander M. Jamieson, PhD (Committee Member)
Philip L. Taylor, PhD (Committee Member)
249 p.
Biomedical Research; Biophysics; Engineering; Materials Science; Physics; Polymers
Computer Simulation; Monte Carlo; Bond Fluctuation Model; Metal-Ligand Interaction; Metallo-Supramolecular Micelles; Metallo-Supramolecular Gels; cis-trans Isomerization; Ligand-Receptor Interaction; Nanoparticle Targeting; Targeting Efficiency

Recommended Citations

Citations

  • Wang, S. (2010). Computer Simulation and Mathematical Modeling of Reversibly Associated Polymers [Doctoral dissertation, Case Western Reserve University]. OhioLINK Electronic Theses and Dissertations Center. http://rave.ohiolink.edu/etdc/view?acc_num=case1275488088

    APA Style (7th edition)

  • Wang, Shihu. Computer Simulation and Mathematical Modeling of Reversibly Associated Polymers. 2010. Case Western Reserve University, Doctoral dissertation. OhioLINK Electronic Theses and Dissertations Center, http://rave.ohiolink.edu/etdc/view?acc_num=case1275488088.

    MLA Style (8th edition)

  • Wang, Shihu. "Computer Simulation and Mathematical Modeling of Reversibly Associated Polymers." Doctoral dissertation, Case Western Reserve University, 2010. http://rave.ohiolink.edu/etdc/view?acc_num=case1275488088

    Chicago Manual of Style (17th edition)

case1275488088
761
© 2010, all rights reserved.
This open access ETD is published by Case Western Reserve University School of Graduate Studies and OhioLINK.