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.

化学催化项目支持北卡罗来纳州立大学的 Elon A. Ison 教授，他将开发利用过渡金属催化的新方法，以实现碳氢化合物的清洁高效氧化。拟议的工作将合理设计新的催化系统，用于通过化学氧化将碳氢化合物原料转化为有价值的材料。传统上，氧化是使用强化学计量氧化剂进行的，包括 Mn(VII)、Cr(VI)、Os(VIII) 和氯基含氧阴离子的盐。这些试剂除了成本高昂之外，还会导致环境污染。选择性氧化关键问题的解决方案是开发过渡金属催化剂，该催化剂可以介导反应，产生所需的氧化产物并最大限度地减少不需要的副产物。在自然界中，酶被用作有氧氧化的催化剂，并根据其催化机制被分为氧化酶和加氧酶。氧化酶通过使用双氧作为氢受体来催化底物的氧化，而加氧酶通过氧原子转移来氧化底物。氧原子转移氧化反应，即加氧酶模拟反应，是众所周知的，并且是不对称催化中最成功的方法之一。这些过程突出了本研究项目将采用的两个主要策略，即设计有机底物催化氧化系统。底物氧化中不涉及氧原子转移的过程（“氧化酶”系统）将利用氧作为末端氧化剂，而涉及氧原子转移到底物的过程（“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催化和绿色化学领域本科生和研究生新课程和实验室的开发。此外，还有一个名为“无机研究研讨会系列”的新研究生研讨会系列，以及一个名为“无机催化和能源（ICE）”的年度研讨会。将开发旨在建立北卡罗来纳州立大学无机组与研究三角地区内研究机构之间合作的项目。扩大参与范围将包括指导、培养和招募来自不同背景的新一代科学家（高中生、本科生、研究生和博士后），探索利用催化技术的 STEM 领域的职业生涯。