CAREER: Water-Soluble Metallofullerene Derivatives with Defined Structures and Tailorable Functions

在化学系大分子、超分子和纳米化学(MSN)计划的支持下，罗格斯大学的张建元和他的团队将合成和表征水溶性面体内金属富勒烯(EMF)，并探索其潜在的用途。电磁场是纳米大小的足球形状的碳分子，将金属离子封装在笼子里。电子、能源、量子材料、催化、电子学和生物技术是电磁场显示出前景的潜在应用。然而，要实现它们的全部潜力，需要更好地了解它们在水溶液中的行为。制造水溶性电动势衍生物的典型方法不会产生结构定义的分子；它们总是破坏电动势笼子的结构，并降低其电子性质。该项目将使用模块化合成方法来创建具有精确定义的结构的水溶电动势家族，并研究它们的结构参数与电光特性之间的相关性。在进行这个项目的过程中，学生将在一个多学科的研究环境中接受培训。将开发与研究结果相结合的真实世界实验的主动学习技术。将在当地社区大学开展针对不同人群的外展活动，向经济困难和代表性不足的学生介绍在科学领域的未来职业道路。该项目将利用首席研究员实验室最近开发的模块化“Metallobuckytrio”(MBT)平台。MBT平台由两个金属富勒烯共价键合到一个C60富勒烯上，通过合理选择配体，可以合成一系列具有理想性能的结构定义的水溶性电动势衍生物。将追求三个研究目标。在目标1中，糖功能化配体将被引入以增强用于下一代MRI造影剂的Gd(Gd)MBT的T1弛豫度。在目标2中，将引入卟啉功能化的配体，并将研究所得到的卟啉-富勒烯十三碳化合物的光致电荷分离和复合过程。在目标3中，将引入染料功能化的配体，以形成在光动力疗法(PDT)中具有潜在长期科学影响的协同光敏剂。该奖项反映了NSF的法定使命，并通过使用基金会的智力优势和更广泛的影响审查标准进行评估，被认为值得支持。

WIth support from the Macromolecular, Supramolecular, and Nanochemistry (MSN) Program of the Division of Chemistry, Jianyuan Zhang of Rutgers, The State University of New Jersey and his team will synthesize and structurally characterize water soluble endohedral metallofullerenes (EMFs) and explore their potential utility. EMFs are nanometer-sized soccer ball-shaped carbon molecules that encapsulate metal ions within their cages. Electronic, energy, quantum materials, catalysis, electronics, and biotechnologies are potential applications where EMFs show promise. However, realizing their full potential will require a better understanding of their behavior in aqueous solution. Typical approaches to making water-soluble EMF derivatives do not yield structurally defined molecules; they invariably disrupt the structure of the EMF cage and downgrade its electronic properties. This project will use a modular synthetic approach to create a family of water-soluble EMFs with precisely defined structures and study the correlation between their structural parameters and electro-optic properties. In the course of conducting this project, students will be trained in a multidisciplinary research environment. Active learning techniques with real world experiments that are integrated with the research results will be developed. Outreach activities targeting a diverse population in local community colleges will be carried out to introduce economically disadvantaged and underrepresented students future career paths in science.This project will utilize a modular “metallobuckytrio” (MBT) platform that was recently developed in the laboratory of the principal investigator. The MBT platform, which consists of two metallofullerenes covalently bonded to one C60 fullerene, allows the synthesis of a family of structurally defined water-soluble EMF derivatives with desirable properties via judicious selection of ligands. Three research aims will be pursued. In Aim 1, saccharide-functionalized ligands will be introduced to enhance the T1 relaxivity of gadolinium (Gd) MBTs for the next-generation MRI contrast agents. In Aim 2, porphyrin-functionalized ligands will be introduced and photo-induced charge separation and recombination processes of the resulting porphyrin-fullerene tridecads will be investigated. In Aim 3, dye-functionalized ligands will be introduced to form synergistic photosensitizers with potential long term scientific impact in photodynamic therapy (PDT).This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.