CAREER: Rational Design of Green Catalysts for Chemical Oxidations

职业：化学氧化绿色催化剂的合理设计

• 批准号: 0955636
• 负责人: Elon Ison
• 金额: $ 53万
• 依托单位: North Carolina State University
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2010
• 资助国家: 美国
• 起止时间: 2010-04-01 至 2015-03-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=0955636&HistoricalAwards=false
• 关键词: CAREER; Rational; Design; Green; Catalysts

The Chemical Catalysis Program supports Professor Elon A. Ison at North Carolina State University who will develop new methodologies using transition metal catalysis to accomplish the clean and efficient oxidation of hydrocarbons. The proposed work will rationally design new catalytic systems for use in the conversion of hydrocarbon feed stocks into valuable materials via chemical oxidation. Traditionally, oxidations are performed with strong stoichiometric oxidants, including salts of Mn(VII), Cr(VI), Os(VIII), and chlorine-based oxoanions. These reagents, in addition to their significant costs, lead to environmental contaminants. The solution to the critical problem of selective oxidation is the development of transition metal catalysts that can mediate reactions that result in desired oxidized products and minimize undesirable by-products. In nature, enzymes are employed as catalysts for aerobic oxidations and are characterized as oxidases and oxygenases depending on their catalytic mechanisms. Oxidases catalyze the oxidation of substrates by employing dioxygen as a hydrogen acceptor, while oxygenases oxidize substrates by oxygen atom transfer. Oxygen atom-transfer oxidation reactions, that is, oxygenase mimics, are well-known and are among the most successful methods in asymmetric catalysis. These processes highlight the two main strategies that will be employed in this research program that will design systems for the catalytic oxidation of organic substrates. Processes that do not involve oxygen atom transfer in substrate oxidation (?oxidase? systems), will utilize oxygen as a terminal oxidant, and processes that involve the transfer of an oxygen atom to a substrate (?oxygenase? systems), will utilize nitrous oxide as an oxidant.Broader impacts will involve the development of new courses and labs on the undergraduate and graduate levels in the area of catalysis and green chemistry. Additionally, a new graduate seminar series called ?Inorganic Research Seminar Series?, and an annual symposium entitled ?Inorganic Catalysis and Energy (ICE)? aimed at establishing collaborations among the inorganic groups at North Carolina State University and the research institutions within the Research Triangle area will be developed. Broadening participation will include the mentorship, development, and recruitment of a new generation of scientists (high-school, undergraduate, graduate students, and postdoctoral associates) from diverse backgrounds to explore careers in STEM fields that utilize catalysis as a technology.

化学催化计划支持教授埃隆A。他将开发利用过渡金属催化实现碳氢化合物清洁高效氧化的新方法。该工作将合理设计新的催化体系，用于通过化学氧化将烃原料转化为有价值的材料。传统上，氧化用强化学计量氧化剂进行，包括Mn（VII）、Cr（VI）、Os（VIII）和氯基含氧阴离子的盐。这些试剂，除了其显著的成本之外，还导致环境污染物。选择性氧化的关键问题的解决方案是开发过渡金属催化剂，其可以介导导致所需氧化产物的反应并使不需要的副产物最小化。在自然界中，酶被用作有氧氧化的催化剂，并且根据其催化机制被表征为氧化酶和加氧酶。氧化酶通过使用分子氧作为氢受体催化底物的氧化，而加氧酶通过氧原子转移氧化底物。氧原子转移氧化反应，即加氧酶模拟物，是众所周知的，并且是不对称催化中最成功的方法之一。这些过程突出了两个主要的策略，将在这个研究计划，将设计系统的有机底物的催化氧化。在衬底氧化过程中不涉及氧原子转移的过程（？氧化酶？系统），将利用氧作为终端氧化剂，和涉及氧原子转移到衬底（？加氧酶？系统），将利用一氧化二氮作为氧化剂。更广泛的影响将涉及在催化和绿色化学领域的本科生和研究生水平上开发新的课程和实验室。此外，一个新的研究生研讨会系列称为？无机研究研讨会系列？，以及一个年度专题讨论会，题目是？无机催化与能源（ICE）旨在建立在北卡罗来纳州州立大学和研究三角区内的研究机构之间的合作。扩大参与将包括指导，发展和招聘来自不同背景的新一代科学家（高中，本科，研究生和博士后），以探索利用催化作为技术的STEM领域的职业生涯。