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

该项目的总体目标是结合法国、德国和美国的3个研究实验室的核心能力，研究功能化聚合物强大的合成策略的开发，并将这些新材料/工艺应用于JANUS大分子组装的制备。推动这一努力的一个动力是应用建筑定义的软材料来解决资源、健康和能源问题。这是一个跨国问题，可以通过多国团队最有效地解决。将官能团要求与有效的合成方法相匹配的挑战可能最好地通过Janus大分子、纳米颗粒和纳米对象的合成来说明。虽然这些材料在一系列工业和研究环境中有很大的前景，但越来越需要为它们的建造制定战略。该项目的一个基本主题是开发新的合成方法，这些方法依赖于高产率和用户友好的化学，即所谓的“点击”反应，以方便和有效的方式制备这些材料。这些努力不仅将从根本上扩展合成方法，而且将极大地增加可制备的Janus结构的范围，而简化的技术将允许更广泛的研究人员接触这些重要的材料类别。我们建议将活性聚合技术(如阴离子或可控自由基乙烯基聚合和内酯/碳酸酯/丙交酯的开环聚合等)与高效的官能化化学(如硫醇-烯、叠氮交联等)相结合，以获得量身定制的多功能Janus材料。这将极大地影响和促进对Janus材料及其在高效能源产生/储存、疾病检测/治疗、坚固的传感器系统等方面的使用的基本了解的发展。通过发现和利用新的合成试剂、可编程官能团和新型聚合物结构所带来的创新意义重大，如果成功，将极大地增加Janus材料的可获得性，使尽可能广泛的研究人员能够使用。

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.