New Molecularly Imprinted Polymers with Significantly Enhanced Properties for Chemical and Biological Analyses and Separations

0854105SpivakOne单体分子印迹聚合物(简称OMNiMIP)是由PI基团中开发的新型交联单体合成的，与传统形成的分子印迹聚合物(MIP)相比，具有根本的不同，导致了新的和增强的性能。首先，一种单体的使用最终提供了更高的每克聚合物的负载能力，这可以改进固相萃取和分析分离等应用。OMNiMIPs重结合能力的增强可能导致超出目前MIPs限制的应用，例如在固相萃取、环境净化或蛋白质纯化策略中高容量去除目标化合物。我们目前正在调查造成OMNiMIP的高容量和选择性的基本原则。更高的容量也为同时印迹几种不同的目标化合物提供了更高的性能，便于多个分析物的分析和分离。这对于不同化合物混合物的分析可能很重要，例如药物配方的分析或一系列不同分子的固相萃取。此外，新型手性OMNiMIP似乎能够印迹外消旋混合物，提供了一条更容易获得手性固定相的途径。这将消除对映体模板的需要，这通常是传统的MIP所需的。最后，OMNiMIP将与共轭聚合物杂交，提供一种在结合目标分子时能够产生荧光信号的材料，这对传感器和其他检测策略是有用的。本提案中描述的研究的一个重要主题是利用对单体起始材料的分子控制来优化OMNiMIP的宏观性能(例如负载能力和选择性)。该提案的核心是为OMNiMIP工艺设计、合成和评估新的交联剂，以最大限度地提高这些材料在上述应用中的性能。使用成功的交联剂的分子结构作为先导化合物，具有合理变化的类似物将被评估结构-性质关系的改善。该提案描述了新的MIP材料的基本发展，这些材料既提高了性能，又能够实现过去这项技术所不能提供的独特应用。尽快确定最佳的交联剂结构是很重要的，以便为全世界的研究人员提供最适合其应用的材料。对于社会来说，分子印迹的前景是检测医疗和环境毒素，检测和中和国家安全目标化合物、定制的催化剂和分离介质，这些将以多种方式服务于人类的健康和进步。分子印迹的这些更广泛的影响将通过开发用于上述新应用的OMNiMIP以几种方式得到加强。虽然这些材料的开发应该被视为这项研究的主要实践成果，但这些研究也将有助于从根本上理解OMNiMIP效应的基本原理，以及这些原理与传统的分子印迹方法有何不同。此外，OMNiMIPs的发展促进了与国内外研究人员的大量合作，导致了许多有趣的研究，以提高这些材料在当前和新的应用中的性能。OMNiMIP研究还为本科生和高中生提供了参与尖端研究并在会议上展示他们的成果的机会。OMNiMIP研究的成功和乐趣的真正功劳应归功于不同的研究生和博士后研究员群体，他们致力于日常问题的解决，使这项研究蓬勃发展。我们的团队很有才华，从路易斯安那州立大学这里得到很好指导的代表不足的群体中平均抽签。他们在分子印迹和OMNiMIP方面的培训继续提供与重要化学学科自然对接的机会，提供跨学科教育，提高他们在当前和未来市场的竞争力。这个整体计划中的人和研究将通过公开讲座和演讲接触到路易斯安那州更广泛的社区，特别是年轻一代，目的是提高他们对基础科学和技术的认识和兴趣。

0854105SpivakOne monomer molecularly imprinted polymers (referred to as 'OMNiMIPs'), synthesized from novel crosslinking monomers developed in the PI's group, exhibit fundamental differences that give rise to new and enhanced properties versus traditionally formed molecularly imprinted polymers (MIPs). First, the use of one monomer ultimately affords a higher loading capacity per gram of polymer, which can improve applications such as solid phase extraction and analytical separations. The increased rebinding capacity of OMNiMIPs could lead to applications beyond current limits of MIPs, such as high capacity removal of target compounds in solid phase extraction, environmental clean-up, or protein-purification strategies. We are currently investigating the underlying principles that are responsible for the high capacity and selectivity of OMNiMIPs. The higher capacity also affords higher performance for imprinting several different target compounds simultaneously, facilitating assays and separations of multiple analytes. This could be important for assays on mixtures of different compounds, such as the analysis of pharmaceutical formulations or solid phase extraction of an array of different molecules. In addition, novel chiral OMNiMIPs appear capable of imprinting racemic mixtures, providing an easier route to chiral stationary phases. This would eliminate the need for enantiopure templates, normally required for traditional MIPs. Last, OMNiMIPs will be hybridized with conjugated polymers to provide a material that can generate a fluorescence signal upon binding the target molecule, which is useful for sensors and other detection strategies. An important theme for the research described in this proposal is to utilize molecular control of the monomer starting materials toward optimizing macroscopic properties (e.g. loading capacity and selectivity) of OMNiMIPs. The heart of this proposal is the design, synthesis and evaluation of new crosslinkers for the OMNiMIP process that will maximize the performance of these materials for the applications described above. Using the molecular structure of successful crosslinkers as lead compounds, analogs with rational changes will be evaluated for improvements in structure-property relationships. This proposal describes the fundamental development of new MIP materials that both improve performance and are capable of unique applications that have not been available from this technology in the past. It is important to determine the optimal crosslinker structures as quickly as possible in order to provide researchers worldwide with the best materials for their applications. For society, the promise of molecular imprinting is the detection of medical and environmental toxins, detection and neutralization of national security target compounds, tailored catalysts, and separation media that will serve the health and advancement of mankind in numerous ways. These broader impacts of molecular imprinting will be enhanced in several ways by the development of OMNiMIPs for novel applications such as those described above. While the development of these materials should be seen as a major practical outcome of this research, these studies will also contribute to the fundamental understanding of the underlying principles of the OMNiMIP effect and how these differ from traditional molecular imprinting approaches. Furthermore, the development of OMNiMIPs has stimulated numerous collaborations with researchers, both nationally and internationally, resulting in many interesting studies toward the increased performance of these materials for current and new applications. OMNiMIP research has also provided opportunities for undergraduates and a high school student to participate in cutting edge research and present their results at conferences. The real credit for the success and fun of OMNiMIP research belongs to the diverse group of graduate students and post-doctoral fellows who have engaged themselves in the day-to-day problem solving that has made this research flourish. Our group is talented and draws evenly from underrepresented groups that are mentored well here at LSU. Their training in molecular imprinting and OMNiMIPs continues to present opportunities that interface important chemical disciplines naturally, providing an interdisciplinary education that will enhance their competitiveness in the current and future marketplace. The people and the research in this overall program will reach the broader community in Louisiana, especially younger generations, through public lectures and presentations with the goal to improve their awareness and interest of basic science and technology.