Hostname: page-component-78c5997874-m6dg7 Total loading time: 0 Render date: 2024-11-19T08:43:09.222Z Has data issue: false hasContentIssue false
  • English
  • Français

Molecular Simulations of Recognitive Polymer Networks Prepared by Biomimetic Configurational Imprinting as Responsive Biomaterials

Published online by Cambridge University Press:  01 February 2011

David B. Henthorn  and
Nicholas A. Peppas
David B. Henthorn
Affiliation:
Department of Chemical Engineering, The University of Texas at Austin, Austin, TX, USA
Nicholas A. Peppas
Affiliation:
Department of Chemical Engineering, The University of Texas at Austin, Austin, TX, USA Department of Biomedical Engineering and Division of Pharmaceutics, The University of Texas at Austin, Austin, TX, USA
Get access

Abstract

Proteins, enzymes, and antibodies have the ability to discern specific molecules out of a whole host of species and selectively bind them with remarkable affinity. A route that would enable the creation of synthetic polymers with this binding ability would be a great advance with subsequent applications in chemical sensors, single-molecule separations, and even artificial enzymes. In this work we study the molecular imprinting process whereby a controlled nanostructure consisting of distinct binding sites is created in a polymer network through a templating procedure. Simulations were done to better understand the underlying network structure that gives rise to the increased uptake. An all-atom molecular dynamics simulation was coupled with a kinetic gelation approach to study network formation in the presence of a template. The monomers used were first studied with density-functional theory in order to parameterize a force field for various methacrylates. Simulation results showed three key functional group interactions that lead to successful imprinting and subsequent rebinding.

Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 787: Symposium G – Molecularly Imprinted Materials , 2003 , G2.1
Copyright
Copyright © Materials Research Society 2004

Access options

Get access to the full version of this content by using one of the access options below. (Log in options will check for institutional or personal access. Content may require purchase if you do not have access.)

References

REFERENCES

1. Ratner, B.D., The Engineering of Biomaterials Exhibiting Recognition and Specificity. J. Mol. Recognition, 1996. 9: p. 617–625.Google Scholar
2. Takeuchi, T. and Haginaka, J., Separation and Sensing Based on Molecular Recognition Using Molecularly Imprinted Polymers. J. Chromatography B., 1999. 728: p. 1–20.Google Scholar
3. Whitcombe, M.J. and Vulfson, E.N., inted Polymers. Advanced Materials, 2001. 13: p. 467–480.Google Scholar
4. Mosbauch, K. and Ramstrom, O., The Emerging Technique of Molecular Imprinting and its Future Impact on Biotechnology. Biotechnol., 1996. 14: p. 163–170.Google Scholar
5. Takeuchi, T. and Matsui, J., Molecular Imprinting: An Approach to “Tailor Made” Synthetic Polymers with Biomimetic Functions. Acta. Polym., 1996. 47: p. 471–480.Google Scholar
6. Byrne, M.E., Park, K., and Peppas, N.A., Molecular imprinting within hydrogels. Advanced Drug Delivery Reviews, 2002. 54(1): p. 149–161.Google Scholar
7. Rachkov, A. and Minoura, N., Towards Molecularly Imprinted Polymers Selective to Peptides and Proteins. The Epitope Approach. Biochimica et Biophysica Acta, 2001. 1544: p. 255–266.Google Scholar
8. Frisch, M. J., G.W.T., , Schlegel, H. B., Scuseria, G. E., Robb, M. A., Cheeseman, J. R., Zakrzewski, V. G., Montgomery, J. A. Jr, Stratmann, R. E., Burant, J. C., Dapprich, S., Millam, J. M., Daniels, A. D., Kudin, K. N., Strain, M. C., Farkas, O., Tomasi, J., Barone, V., Cossi, M., Cammi, R., Mennucci, B., Pomelli, C., Adamo, C., Clifford, S., Ochterski, J., Petersson, G. A., Ayala, P. Y., Cui, Q., Morokuma, K., Salvador, P., Dannenberg, J. J., Malick, D. K., Rabuck, A. D., Raghavachari, K., Foresman, J. B., Cioslowski, J., Ortiz, J. V., Baboul, A. G., Stefanov, B. B., Liu, G., Liashenko, A., Piskorz, P., Komaromi, I., Gomperts, R., Martin, R. L., Fox, D. J., Keith, T., Al-Laham, M. A., Peng, C. Y., Nanayakkara, A., Challacombe, M., Gill, P. M. W., Johnson, B., Chen, W., Wong, M. W., Andres, J. L., Gonzalez, C., Head-Gordon, M., Replogle, E. S., and Pople, J. A., Gaussian 98. 2001, Gaussian Inc.: Pittsburgh PA.Google Scholar
9. Boots, H., A Model for Inhomogeneous Network Formation by Chain-reaction Polymerization.Google Scholar
10. Bowman, C.N. and Peppas, N.A., Initiation and Termination Mechanisms in Kinetic Gelation Simulations. Journal of Polymer Science: Part A: Polymer Chemistry, 1991. 29: p. 1575–1583.Google Scholar
11. Reddy, M.R., Erion, M.D., and Agarwal, A., Free Energy Calculations: Use and Limitations in Predicting Ligand Binding Affinities, in Reviews in Computational Chemistry, Lipkowski, K.B. and Boyd, D.B., Editors. 2000, Wiley-VCH: New York.Google Scholar
12. Jorgensen, W.L. and Briggs, J.M., A Priori pKa Calculations and the Hydration of Organic Anions. J. Am. Chem. Soc., 1989. 111: p. 4190–4197.Google Scholar
13. Oral, E., Recognitive Polymer Networks for Therapeutic and Diagnostic Devices, in PhD Thesis, School of Chemical Engineering. 2002, Purdue University.Google Scholar