Heterogeneous Alkene Epoxidation Catalysts Derived via Immobilization of Tripodal Titanium Silsesquioxane Complexes

三足钛硅倍半氧烷配合物固定化衍生的多相烯烃环氧化催化剂

• 批准号: 1058097
• 负责人: Folami Ladipo
• 金额: $ 37.5万
• 依托单位: University of Kentucky Research Foundation
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2011
• 资助国家: 美国
• 起止时间: 2011-09-01 至 2015-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1058097&HistoricalAwards=false
• 关键词: Heterogeneous; Alkene; Epoxidation; Catalysts; Derived

The Chemical Catalysis Program supports Professors Folami T. Ladipo and Mark Crocker, both at the University of Kentucky whose proposed research describes strategies for the design of heterogeneous catalysts incorporating tripodal Ti silsesquioxane moieties, and for fully assessing the synthetic potential of the resulting catalysts in the epoxidation of demanding substrates. The ultimate goal of the proposed research is the design and preparation of heterogeneous alkene epoxidation catalysts possessing improved activity, selectivity, and durability relative to current catalysts. These catalysts should be useful in alkene epoxidation using H2O2 and H2/O2 as the oxidant. Their research will focus on the immobilization of tripodal Ti silsequioxane complexes via physical encapsulation in polydimethylsiloxane (PDMS) membranes. This also includes anchoring the Ti silsesquioxane moieties to supported Gold (Au) nanoparticles with in situ generation of H2O2 via the Au-catalyzed reaction of H2 with O2. The properties of the resulting catalysts will be explored with regard to epoxidation of demanding substrates. These will include alkenes that are electronically and/or sterically "deactivated" with respect to epoxidation, such as allylic alcohols. Professors Folami T. Ladipo and Mark Crocker will design improved catalysts for olefin epoxidation. These catalysts are anticipated to be applicable to both fine chemicals synthesis and bulk production of simple aliphatic epoxides. The project will be an active collaboration between Professor Ladipo at the Department of Chemistry and Professor Crocker at the University of Kentucky's Center for Applied Energy Research. The research will be conducted at both locations, with joint responsibility for the direction of graduate and undergraduate students. Thus, this research will provide multidisciplinary training opportunities to students that would not be typically available in a traditional chemistry based project. Another vital objective of the proposed research is using research training to mentor students from groups traditionally under-represented in science. Through collaborations with colleagues at historically black colleges and universities (HBCUs) as well as regional universities, talented African American and Appalachian undergraduate students will be recruited to participate in the proposed research.

化学催化计划支持肯塔基大学的 Folami T. Ladipo 和 Mark Crocker 教授，他们提出的研究描述了包含三足钛硅倍半氧烷部分的多相催化剂的设计策略，以及全面评估所得催化剂在化学中的合成潜力。高要求底物的环氧化。本研究的最终目标是设计和制备相对于现有催化剂具有改进的活性、选择性和耐久性的多相烯烃环氧化催化剂。这些催化剂可用于使用 H2O2 和 H2/O2 作为氧化剂的烯烃环氧化。他们的研究重点是通过物理封装在聚二甲基硅氧烷（PDMS）膜中固定三足钛倍半硅氧烷复合物。这还包括将 Ti 倍半硅氧烷部分锚定到负载的金 (Au) 纳米颗粒上，并通过 Au 催化的 H2 与 O2 反应原位生成 H2O2。所得催化剂的性能将在要求较高的底物的环氧化方面进行探索。这些将包括在环氧化方面电子和/或空间“失活”的烯烃，例如烯丙醇。 Folami T. Ladipo 和 Mark Crocker 教授将设计改进的烯烃环氧化催化剂。这些催化剂预计适用于精细化学品合成和简单脂肪族环氧化物的批量生产。该项目将是化学系拉迪波教授和肯塔基大学应用能源研究中心克罗克教授之间的积极合作。该研究将在两个地点进行，共同负责研究生和本科生的指导。因此，这项研究将为学生提供多学科培训机会，而传统化学项目通常无法提供这些机会。拟议研究的另一个重要目标是利用研究培训来指导传统上在科学领域代表性不足的群体的学生。通过与传统黑人学院和大学（HBCU）以及地区大学的同事合作，将招募有才华的非裔美国人和阿巴拉契亚本科生来参与拟议的研究。