Collaborative Research: CAS: Exploration and Development of High Performance Thiazolothiazole Photocatalysts for Innovating Light-Driven Organic Transformations

合作研究：CAS：探索和开发高性能噻唑并噻唑光催化剂以创新光驱动有机转化

• 批准号: 2400166
• 负责人: James Hanna
• 金额: $ 19.22万
• 依托单位: Winthrop University
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2024
• 资助国家: 美国
• 起止时间: 2024-08-01 至 2027-07-31
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2400166&HistoricalAwards=false
• 关键词: Collaborative; Research; CAS; Exploration; Development; Collaborative; Research; CAS; Exploration; Development

With the support of the Chemical Catalysis program in the Division of Chemistry, Professor Michael G. Walter at the University of North Carolina at Charlotte and Professor James M. Hanna at Winthrop University are designing new, low-cost, scalable, and high efficiency photocatalysts, scaffolds that harness light energy for performing chemical transformations. The overall goal is to advance more sustainable, carbon-based photocatalyst scaffolds that will reduce cost and overall environmental impact compared to traditional precious metal-based systems. The study includes the synthesis and study of new catalyst scaffolds, with the goal of advancing fundamental knowledge about how modifications affect reactivity. The new catalysts will then be studied in a variety of chemical transformations that currently rely on expensive-metal photocatalysts. The work will be built upon a new regional collaboration between UNC Charlotte and Winthrop University and will involve both undergraduate and graduate students from both research groups who will gain exposure to diverse and interdisciplinary activities across the practice of chemical research. In addition, the research components will be connected with the classroom teaching of the investigators, introducing photochemical science topics to a diverse group of graduate and undergraduate students. The investigators will continue their collaborations with local science museums, educators, and schools to develop and provide chemistry outreach programs to the Charlotte region.The goal of this research is to study and develop new thiazolo(5,4-d)thiazole (TTz) organic photoredox catalyst derivatives. TTzs are attractive photocatalyst materials due to their low-cost, single reaction step syntheses, non-halogenated, and high photochemically stable heterobicyclic core. TTz photocatalysts will address the need to develop scalable, high efficiency organic photocatalyst tools to drive a wide array of organic transformations. The team hypothesizes that the unique TTz photochemical properties enable new and improve upon existing transformations currently driven with expensive and toxic molecular transition-metal catalysts. Secondly, it is proposed that extended TTz photocatalyst materials will enable lower energy (e.g. red light) driven transformations while helping to tune redox characteristics for specific transformations. Preliminary studies have demonstrated the ability of a series of TTzs to drive reactions with much higher efficiencies than previously used transition metal photocatalysts. The collaborative team will further explore photocatalyst stability, reaction rates, and ability to drive a range of organic transformations. A library of new TTz photocatalyst derivatives will be developed with tunable light absorption properties and redox characteristics. Photochemical studies will be carried out to establish reaction quantum yields, and rates will be monitored using fluorescence and chromogenic TTz coloration changes. This collaborative research program will focus on photochemical efficiency metrics to help guide subsequent generations of TTz photocatalysts with a focus on optimizing performance and versatility. The materials produced by this project can benefit society by contributing to the development of a new series of photocatalyst materials that have the potential to improve synthetic efficiency and lower provide for more sustainable organic synthesis methodology.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.

在化学催化计划的支持下，北卡罗来纳大学夏洛特大学的Michael G. Walter教授和Winthrop University的James M. Hanna教授正在设计新的，低成本，可扩展和高效率的光催化剂，可用于执行化学转化的轻能量。总体目标是促进更可持续的，基于碳的光催化剂脚手架，与传统的贵金属系统相比，将降低成本和整体环境影响。该研究包括对新催化剂支架的合成和研究，目的是促进有关修饰如何影响反应性的基本知识。然后，将研究新的催化剂，这些化学转化目前依赖于昂贵的金属光催化剂。这项工作将建立在UNC夏洛特大学和温思罗普大学之间的新区域合作的基础上，并将涉及来自两个研究小组的本科生和研究生，他们将在化学研究实践中获得各种各样和跨学科的活动。此外，研究组件将与研究人员的课堂教学有关，并将光化学科学主题介绍给多样化的研究生和本科生。调查人员将继续与当地科学博物馆，教育工作者和学校合作，开发并向夏洛特地区提供化学外展计划。这项研究的目的是研究和开发新的噻唑（5,4-D）噻唑（TTZ）有机光载体催化剂。 TTZ由于其低成本，单一反应步骤合成，非卤代化和高光化学上稳定的杂质核心而具有吸引力的光催化剂材料。 TTZ光催化剂将满足开发可扩展的高效有机光催化剂工具的需求，以驱动各种有机转化。该团队假设独特的TTZ光化学性能可以使新的转换具有昂贵和有毒的分子过渡金属催化剂的现有转换。其次，有人提出扩展的TTZ光催化剂材料将使能量较低的能量（例如红光）驱动的转换，同时帮助调整氧化还原特性以实现特定转换。初步研究表明，一系列TTZ驱动反应的能力比以前使用的过渡金属光催化剂更高。协作团队将进一步探索光催化剂稳定性，反应率以及推动一系列有机转化的能力。新的TTZ光催化剂衍生物的库将具有可调的光吸收特性和氧化还原特性。将进行光化学研究以建立反应量子产率，并将使用荧光和成色的TTZ着色变化来监测速率。该协作研究计划将重点介绍光化学效率指标，以帮助指导随后的TTZ光催化剂，重点是优化性能和多功能性。该项目生产的材料可以通过为开发一系列新的光催化剂材料做出贡献而受益匪浅，这些材料有可能提高合成效率并降低提供更可持续的有机综合方法。该奖项反映了NSF的法定任务，并被认为是通过基金会的智力功能和广泛影响的评估来评估CRETERIA的评估。