Development of Robust Strategies for Polymer Syntheses and Application to the Preparation of Functionalized Macromolecular Assemblies - Responsive Janus Nanostructures

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The overarching aim of this project is to combine the core competencies of 3 research laboratories in the France, Germany and the United States to investigate the development of robust synthetic strategies for functionalized polymers and apply these novel materials/processes to the preparation of Janus macromolecular assemblies. A driving force for this effort is the application of architecturally-defined soft materials to address resource, health and energy issues. This is a transnational problem and can be addressed most efficiently with multi-national teams. The challenge of matching functional group requirements with efficient synthetic approaches is perhaps best illustrated by the synthesis of Janus macromolecules, nanoparticles and nano-objects. While these materials have great promise in a range of industrial and research settings, there is an increasing need to develop strategies for their construction. An underlying theme of this project is to develop novel synthetic approaches that rely on high yielding and user friendly chemistry, so called “click” reactions to prepare these materials in a facile and efficient manner. Not only will these efforts expand synthetic methodologies in a fundamental sense, but they will greatly increase the range of Janus structures that can be prepared while the simplified techniques will allow a much wider spectrum of researcher’s access to these important material class. We propose to combine living polymerization techniques such as anionic or controlled radical vinyl polymerization and ring opening polymerization of lactones/carbonates/lactides, etc. with efficient functionalization chemistry such as thiol-ene, azide crosslinking, etc. to access tailor-made, multifunctional Janus materials. This will dramatically impact and enhance the development of a fundamental understanding of Janus materials and their use in efficient energy generation/storage, disease detection/treatment, robust sensor systems, etc. The innovation afforded through the discovery and utilization of new synthetic reagents, programmable functional groups and novel polymeric structures is significant and if successful will greatly increase the accessibility of Janus materials to as wide a group of researchers as possible.