New Catalysts to Expand the Scope of Donor/Acceptor Carbenes

扩大供体/受体卡宾范围的新催化剂

• 批准号: 1956154
• 负责人: Huw Davies
• 金额: $ 48万
• 依托单位: Emory University
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2020
• 资助国家: 美国
• 起止时间: 2020-08-15 至 2024-07-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1956154&HistoricalAwards=false
• 关键词: New; Catalysts; Expand; Scope; Donor

With this award, the Chemical Catalysis Program of the Division of Chemistry is supporting the research of Professor Huw M. L. Davies of Emory University. Professor Davies and his research team are developing new highly active catalysts for the synthesis of value-added compounds of importance to the pharmaceutical, agrochemical and materials science industries. These catalysts are improved versions of catalysts based upon rhodium metal that have been widely successful and that have new features to improve their function. A streamlined approach for making these elaborate catalysts is being implemented and their reactivity is being systematically evaluated. These studies are also serving as an excellent training environment for undergraduate and graduate students, as well as postdoctoral researchers. Professor Davies is further supporting the career development of chemists through the ACS Young Investigator Symposium and promoting diversity through the establishment of the Network for Diversity in Chemical Research. Professor Davies and his research group are also actively engaged in outreach activities to broaden engagement in STEM disciplines.Dirhodium tetracarboxylate paddlewheel complexes are highly-active catalysts for carbene transfer and insertion. Due to the fact that rhodium is a precious metal, the continued optimization of the reactivity and selectivity of these catalysts represents a critical need to be able to apply their reactivity to large scale chemical processes. Professor Davies and his research group are preparing new C4-symmetric dirhodium tetracarboxylate catalysts with periphery directing groups and/or critical additives to achieve high activity and unusual site selectivity. These studies are being directed toward cyclopropanation reactions with donor/acceptor carbenes in situations with competitive reactivity patterns or where opportunities for tandem reactivity are available. Professor Davies is following a robust student-mentoring plan to insure student/advisor focus. Dr. Davies is also leading several initiatives to enhance the academic research environment such as building a new model for collaborative research between academia and industry, organizing world-wide virtual symposia, and organizing special symposia for Assistant Professors to showcase their research at the national meetings of the American Chemical Society.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.

通过这个奖项，化学系的化学催化项目支持了埃默里大学Huw M. L. Davies教授的研究。Davies教授和他的研究团队正在开发新的高活性催化剂，用于合成对制药、农化和材料科学行业具有重要意义的增值化合物。这些催化剂是基于金属铑的催化剂的改进版本，这种催化剂已经广泛成功，并且具有改进其功能的新特性。目前正在采用一种简化的方法来制造这些复杂的催化剂，并且正在系统地评估它们的反应性。这些研究也为本科生、研究生和博士后研究人员提供了良好的培养环境。戴维斯教授通过美国化学学会青年研究员研讨会进一步支持化学家的职业发展，并通过建立化学研究多样性网络促进多样性。Davies教授和他的研究小组也积极参与外展活动，以扩大STEM学科的参与。四羧酸二钠桨轮配合物是一种高活性的碳转移和插入催化剂。由于铑是一种贵金属，这些催化剂的反应性和选择性的持续优化代表了能够将其反应性应用于大规模化学过程的关键需求。Davies教授和他的研究小组正在制备新的具有外围导向基团和/或关键添加剂的c4对称四羧酸二钠催化剂，以实现高活性和不同寻常的位点选择性。这些研究的目的是在具有竞争性反应模式或有机会进行串联反应的情况下，与供体/受体羰基进行环丙化反应。戴维斯教授正在遵循一个强有力的学生指导计划，以确保学生/顾问的关注。戴维斯博士还领导了几项提高学术研究环境的举措，如建立学术界和工业界合作研究的新模式，组织全球虚拟研讨会，以及为助理教授组织特别研讨会，在美国化学会的国家会议上展示他们的研究。该奖项反映了美国国家科学基金会的法定使命，并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，被认为值得支持。

项目成果

Copper-Catalyzed, Aerobic Oxidation of Hydrazone in a Three-Phase Packed Bed Reactor

• DOI: 10.1021/acs.oprd.1c00165
• 发表时间: 2021-07-22
• 期刊: ORGANIC PROCESS RESEARCH & DEVELOPMENT
• 影响因子: 3.4
• 作者: Hatridge, Taylor A.;Wei, Bo;Jones, Christopher W.
• 通讯作者: Jones, Christopher W.

Hexafluoroisopropanol for the Selective Deactivation of Poisonous Nucleophiles Enabling Catalytic Asymmetric Cyclopropanation of Complex Molecules

• DOI: 10.1021/acscatal.2c03909
• 发表时间: 2022-09-30
• 期刊: ACS CATALYSIS
• 影响因子: 12.9
• 作者: Sharland, Jack C.;Dunstan, David;Davies, Huw M. L.
• 通讯作者: Davies, Huw M. L.

Continuous Process to Safely Manufacture an Aryldiazoacetate and Its Direct Use in a Dirhodium-Catalyzed Enantioselective Cyclopropanation

• DOI: 10.1021/acs.oprd.2c00288
• 发表时间: 2022-12-14
• 期刊: ORGANIC PROCESS RESEARCH & DEVELOPMENT
• 影响因子: 3.4
• 作者: Lathrop, Stephen P.;Mlinar, Laurie B.;Davies, Huw M. L.
• 通讯作者: Davies, Huw M. L.

Copper(II) Acetate-Induced Oxidation of Hydrazones to Diazo Compounds under Flow Conditions Followed by Dirhodium-Catalyzed Enantioselective Cyclopropanation Reactions

乙酸铜 (II) 在流动条件下诱导腙氧化为重氮化合物，然后进行铑催化的对映选择性环丙烷化反应

• DOI: 10.1021/acs.orglett.1c01580
• 发表时间: 2021
• 期刊: Organic Letters
• 影响因子: 5.2
• 作者: Wei, Bo;Hatridge, Taylor A.;Jones, Christopher W.;Davies, Huw M.
• 通讯作者: Davies, Huw M.