New Approaches to Catalyst Screening and Development

催化剂筛选和开发的新方法

• 批准号: 1214019
• 负责人: Stephen DiMagno
• 金额: $ 46.5万
• 依托单位: University of Nebraska-Lincoln
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2012
• 资助国家: 美国
• 起止时间: 2012-08-01 至 2015-07-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1214019&HistoricalAwards=false
• 关键词: New; Approaches; Catalyst; Screening; Development

TECHNICAL SUMMARY:With this award the National Science Foundation is funding studies at the University of Nebraska, under the direction of Professor Stephen G. DiMagno (substitute PI for Professor David Berkowitz), to develop new enzyme-based methods for catalyst screening. This approach involves the use of enzymatic reporting enzymes operating in tandem with the organic/organometallic catalysts being screened, with the former in an aqueous reporting layer, and the latter in an organic solvent layer within the same vessel. This arrangement permits for the assessment of key variables including relative reaction rate and enantioselectivity, in real time, and is thus termed "In Situ Enzymatic Screening" (ISES). Particular focus here is on the identification of new screening enzymes/conditions that will permit the experimentalist to examine new leaving groups and new transformations and to move from ambient to elevated temperatures. Transformations being targeted include those of particular interest to bioorganic and medicinal chemists, such as catalytic routes to enantio-enriched, quaternary, alpha-vinyl amino acids as potential mechanism-based enzyme inhibitors.NON-TECHNICAL SUMMARY:This research project is inherently interdisciplinary, at the interface between organic chemistry and biology, as Nature's catalysts are exploited to assist with the development of useful human-made catalysts for chemical synthesis. Scientists working on the project will gain hands-on experience with both frontline asymmetric catalyst development and with modern preparative enzymology. The research is expected to have broader scientific impact on the areas of organic synthesis, green chemistry, biocatalysis, and process chemistry. The PI will continue to provide cross-disciplinary training to postdocs, graduate, and undergraduate students, and the group will continue to reach out to high school students through Chemistry Day.

技术概要：美国国家科学基金会通过该奖项资助内布拉斯加大学的研究，该研究由斯蒂芬·G·DiMagno（大卫Berkowitz教授的替代PI），开发新的基于酶的催化剂筛选方法。 该方法涉及使用酶报告酶与被筛选的有机/有机金属催化剂串联操作，前者在水性报告层中，后者在同一容器内的有机溶剂层中。 这种安排允许在真实的时间内评估关键变量，包括相对反应速率和对映选择性，因此被称为“原位酶筛选”（ISES）。 这里特别关注的是识别新的筛选酶/条件，这将允许实验者检查新的离去基团和新的转化，并从环境温度移动到高温。 目标转化包括那些特别感兴趣的生物有机和药物化学家，如催化路线对映体富集，季，α-乙烯基氨基酸作为潜在的机制为基础的酶inhibitors.NON-TECHNICAL概要：本研究项目本质上是跨学科的，在有机化学和生物学之间的接口，作为自然的催化剂被利用，以协助开发有用的人造催化剂用于化学合成。 从事该项目的科学家将获得一线不对称催化剂开发和现代制备酶学的实践经验。 该研究有望对有机合成、绿色化学、生物催化和过程化学等领域产生更广泛的科学影响。 PI将继续为博士后，研究生和本科生提供跨学科培训，该小组将继续通过化学日接触高中生。