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CAS: Metallopeptide Artificial Enzymes

CAS：金属肽人工酶

基本信息

批准号：
2108219
负责人：
Kara Bren
金额：
$ 49.44万
依托单位：
University of Rochester
依托单位国家：
美国
项目类别：
Standard Grant
财政年份：
2021
资助国家：
美国
起止时间：
2021-09-01 至 2024-08-31
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=2108219&HistoricalAwards=false
关键词：
CAS Metallopeptide Artificial Enzymes

项目摘要

With the support of the Chemistry of Life Processes (CLP) Program in the Division of Chemistry, Professor Kara Bren of the University of Rochester will develop and study small biomolecule catalysts for reactions relevant to developing alternative energy resources and to removing toxic species from water. One of the targeted reactions is the production of the clean-burning fuel hydrogen from water. The other reaction is the transformation of nitrite, a common groundwater pollutant, into ammonia and hydroxylamine, which are useful products. The planned studies will elucidate mechanistic details of these reactions. Furthermore, light-driven hydrogen production will be studied as a means for storing solar energy. These studies will yield information broadly applicable to the development of alternative energy resources and environmental remediation. This project will also contribute to growing a diverse scientific workforce by enhancing the Rochester Early Connection Opportunity program for undergraduates by addition of an independent study and research component. The research supported by this award will focus on the development and study of the mechanism of multi-electron, multi-proton reactions catalyzed by cobalt peptides from the amino terminal, copper- and nickel-binding family. Targeted reactions include proton reduction to dihydrogen and nitrite reduction to ammonia and hydroxylamine. Emphasis is on the understanding of the impact of diffusing proton shuttles and protonatable catalyst moieties on reaction activity, efficiency, and mechanism. The role of proton-coupled electron transfer (PCET) in these reactions will also be investigated. The results of the electrochemical studies will be applied to the development of photochemical systems with enhanced hydrogen evolution activity. Success in this project is expected to yield improved catalysts for nitrogen oxyanion reduction and proton reduction and enhance the understanding of the role of PCET in the catalysis of proton-requiring reactions in water.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.

在化学系生命过程化学（CLP）项目的支持下，罗切斯特大学的卡拉·布伦教授将开发和研究与开发替代能源和从水中去除有毒物质有关的反应的小生物分子催化剂。其中一个目标反应是从水中生产清洁燃烧的燃料氢。另一个反应是将地下水中常见的污染物亚硝酸盐转化为有用的产物氨和羟胺。计划中的研究将阐明这些反应的机理细节。此外，将研究光驱动制氢作为储存太阳能的手段。这些研究将产生广泛适用于开发替代能源和环境补救的资料。该项目还将通过增加独立学习和研究的组成部分，加强罗切斯特大学本科生早期联系机会计划，为培养多样化的科学队伍做出贡献。该奖项支持的研究将侧重于开发和研究氨基末端、铜和镍结合家族的钴肽催化的多电子、多质子反应机理。目标反应包括质子还原为二氢和亚硝酸盐还原为氨和羟胺。重点是了解扩散质子穿梭和可质子化催化剂部分对反应活性、效率和机理的影响。质子耦合电子转移（PCET）在这些反应中的作用也将被研究。电化学研究的结果将应用于开发具有增强析氢活性的光化学系统。该项目的成功有望产生改进的氮氧阴离子还原和质子还原催化剂，并加深对PCET在催化水中质子需要反应中的作用的理解。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。