Redox catalysis strategies for synthesis

氧化还原催化合成策略

• 批准号: 1900266
• 负责人: Corey Stephenson
• 金额: $ 48万
• 依托单位: Regents of the University of Michigan - Ann Arbor
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2019
• 资助国家: 美国
• 起止时间: 2019-05-01 至 2023-04-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1900266&HistoricalAwards=false
• 关键词: Redox; catalysis; strategies; synthesis

This project is addressing issues - such as the environmentally-friendly manufacturing of economically-important chemicals - that are at the forefront of modern chemical synthesis, catalysis, and sustainability. Photochemistry is the conversion of solar energy into chemical energy and is an important component of this goal. The application of photochemistry to organic synthesis has traditionally required hazardous reagents and/or high energy, ultraviolet light. In this project, Dr. Stephenson is studying the use of complexes that harvest sunlight to power chemical reactions. Importantly, this research project is being carried out in collaboration with pharmaceutical companies. This collaboration enables the rapid incorporation of the new methods into practical applications. Dr. Stephenson's research group participates in several outreach programs to engage grade school (3rd-12th grade) students, with the intention of inspiring the next generation of scientists and leaders. For example, the research team is contributing to the Females Excelling More in Mathematics, Engineering, and the Science (FEMMES) and the Michigan Math and Science Scholars (MMSS) programs at the University of Michigan. This outreach is directly engaging grade school students in a fun and supportive atmosphere, while also encouraging them to pursue a career in STEM.With funding from the Chemical Catalysis program of the Chemistry Division, Dr. Stephenson at the University of Michigan - Ann Arbor is studying how transiently generated electron donor-acceptor (EDA) complexes can be leveraged for the development of new methods in chemical synthesis. The rational design of visible light-active EDA complexes is possible by applying basic principles of Mulliken theory. Such complexes are characterized by UV-Vis spectroscopy. EDA photocatalysis represents an exciting new frontier for the development of methods in organic synthesis. In this regard, methods for arene trifluoromethylation and radical aryl transpositions, for the rapid generation of molecular complexity, are being developed. Through a detailed understanding of each reaction mechanism, the developed methods are rapidly translated to industrial scale in collaboration with the AbbVie Process Research and Development team. Dr. Stephenson's research group is involved in several outreach programs that apply their expertise in synthetic chemistry to engage grade school (3rd-12th grade) students, with the intention of inspiring the next generation of scientific leaders. Dr. Stephenson's involvement in the Females Excelling More in Mathematics, Engineering, and the Science (FEMMES) and the Michigan Math and Science Scholars (MMSS) programs at the University of Michigan have allowed for the direct engagement of grade school students to teach synthetic chemistry in a fun and supportive atmosphere while also encouraging them to pursue a career in STEM.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.

该项目致力于解决现代化学合成、催化和可持续发展前沿的问题，例如具有重要经济意义的化学品的环保制造。 光化学是将太阳能转化为化学能，是这一目标的重要组成部分。光化学在有机合成中的应用传统上需要危险的试剂和/或高能紫外光。在这个项目中，斯蒂芬森博士正在研究利用复合物收集阳光来为化学反应提供动力。重要的是，该研究项目正在与制药公司合作开展。这种合作使新方法能够快速融入实际应用。斯蒂芬森博士的研究小组参加了几个外展计划，以吸引小学（3 - 12年级）的学生，目的是激励下一代的科学家和领导人。例如，该研究小组正在为密歇根大学的女性在数学，工程和科学（FEMMES）和密歇根数学和科学学者（MMSS）计划做出贡献。这项推广活动直接让小学生在一个有趣和支持的氛围中参与进来，同时也鼓励他们在STEM领域从事职业。在化学部化学催化项目的资助下，密歇根大学安阿伯分校的斯蒂芬森博士正在研究如何利用瞬时产生的电子供体-受体（EDA）复合物来开发化学合成的新方法。应用Mulliken理论的基本原理，可以合理设计可见光活性EDA配合物。 这种复合物的特征在于紫外-可见光谱。EDA技术代表了有机合成方法发展的一个令人兴奋的新领域。在这方面，芳烃三氟甲基化和自由基芳基转位的方法，快速生成分子的复杂性，正在开发中。通过对每种反应机理的详细了解，与艾伯维工艺研发团队合作，开发的方法迅速转化为工业规模。斯蒂芬森博士的研究小组参与了几个推广项目，这些项目运用他们在合成化学方面的专业知识吸引小学（3 - 12年级）学生，目的是激励下一代科学领袖。斯蒂芬森博士参与了“女性在数学、工程、科学（FEMMES）和密歇根数学和科学学者（MMSS）密歇根大学的项目允许小学生在有趣和支持的氛围中直接参与合成化学教学，同时鼓励他们从事STEM职业。该奖项反映了NSF的法定使命，并已通过使用基金会的知识价值和更广泛的影响审查标准进行评估，认为值得支持。

项目成果

Converting a Two-Week Chemistry Course for High School Students to a Virtual Format During COVID

• DOI: 10.1021/acs.jchemed.1c00069
• 发表时间: 2021-06-07
• 期刊: JOURNAL OF CHEMICAL EDUCATION
• 影响因子: 3
• 作者: Albright, Haley;Stephenson, Corey R. J.;Schindler, Corinna S.
• 通讯作者: Schindler, Corinna S.

High‐Throughput Optimization of Photochemical Reactions using Segmented‐Flow Nanoelectrospray ‐ Ionization Mass Spectrometry**

使用分段流纳电喷雾-电离质谱法对光化学反应进行高通量优化**

• DOI: 10.1002/anie.202301664
• 发表时间: 2023
• 期刊: Angewandte Chemie International Edition
• 作者: Sun, Alexandra C.;Steyer, Daniel J.;Robinson, Richard I.;Ginsburg‐Moraff, Carol;Plummer, Scott;Gao, Jinhai;Tucker, Joseph W.;Alpers, Dirk;Stephenson, Corey R. J.;Kennedy, Robert T.
• 通讯作者: Kennedy, Robert T.