Amino acid N-carboxyanhydrides and polypeptides: Controlled polymerization, properties and applications

The goal of my Ph.D. research is to develop controlled/living polymerization techniques of α-amino acid N-carboxyanhydrides (NCAs) and synthetic polypeptides based materials. Polypeptides are a class of emerging biomaterials receiving increasing interests for various applications including drug delivery, gene therapy, antimicrobial and tissue engineering. The ring-opening polymerization (ROP) of NCAs has long been demonstrated as a powerful technique for preparation of high molecular weight (MW) synthetic polypeptides in gram scale. We developed a system utilizing organo-silicon amines, namely hexamethyldisilazane (HMDS) and N-trimethylsilyl (N-TMS) amines, for the controlled ROP of various NCAs. Predicable MWs and narrow molecular weight distributions (MWDs) of homo- and block- polypeptides can be prepared via this methodology. Our mechanism study illustrated that the polymerization involves formation of trimethylsilyl carbamate (TMS-CBM) structure at the propagation center. In addition, the system allows facile end group and side-chain functionalization of the polypeptides and integration of NCA ROP with other polymerization techniques such as ring-opening metathesis polymerization (ROMP) to prepare hybrid polypeptides materials. Finally, we discovered a new type of ionic polypeptides with unusual helical stability and demonstrated that they have great potential for gene delivery and siRNA delivery applications.

Name thesis:degree_name

Ph.D.

Level thesis:degree_level

Dissertation

Discipline thesis:degree_discipline

Materials Science & Engr

Grantor

University of Illinois at Urbana-Champaign

Year dc:date

2011

Author dc:creator

• Lu, Hua

Contributors dc:contributor

• Cheng, Jianjun
• Braun, Paul V.
• Economy, James
• Moore, Jeffrey S.

• N-carboxyanhydrides (nca)
• Polypeptides
• Controlled-polymerization
• Helix gene-delivery

Statement dc:rights

• Copyright 2011 Hua Lu

Language dc:language

en

Handle dc:identifier

http://hdl.handle.net/2142/24190

OAI identifier oai:identifier

oai:www.ideals.illinois.edu:2142/24190