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SusChEM: Artificial Hydrogenases

SusChEM：人工氢化酶

基本信息

批准号：
1708256
负责人：
Kara Bren
金额：
$ 44.85万
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：
2017
资助国家：
美国
起止时间：
2017-09-01 至 2021-08-31
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1708256&HistoricalAwards=false
关键词：
SusChEM Artificial Hydrogenases

项目摘要

The Chemistry of Life Processes Program in the Chemistry Division is making this award to Professor Kara L. Bren of the University of Rochester to develop and investigate complexes of cobalt with peptides for catalyzing the production of hydrogen gas from water using solar energy. Hydrogen is an attractive fuel because of its high-energy density and clean combustion. The catalytic activity of the cobalt complex is characterized using electrochemistry. These catalysts are integrated into photochemical systems for converting light energy to chemical energy. Investigations of reaction pathways and the effects of reaction conditions on the efficiency and rate of hydrogen production are emphasized in this research. Graduate students are trained in state-of-the-art biochemical, electrochemical, and photochemical techniques in this project. This award also supports the participation of hearing-impaired students from the National Technical Institute for the Deaf in Rochester in research, enhancing scientific workforce diversity. This project develops new metallopeptide catalysts and investigates catalytic mechanisms for the hydrogen evolution reaction in water, using electro-catalysis as well as photocatalytic systems and assemblies. Catalysis of hydrogen evolution by the metallopeptides studied in this work involves a proton-coupled electron transfer (PCET) step in which the peptide amine acts as a proton shuttle. In the research, Professor Bren determines the effects of altering peptide sequence and amine pKa on PCET and on the rate and overpotential for hydrogen production. In addition, the role of buffers in delivering protons to the catalyst is investigated in work with broad implications for understanding catalysis in an aqueous environment. Finally, integrated systems optimized to prevent back electron transfer and other unproductive pathways in the photochemical reaction are engineered and investigated. Success in this project provides environmentally friendly, water-soluble systems for the storage of solar energy in the form of hydrogen fuel and further develops our understanding of PCET in catalysis. This proposal is considered under the SusChEM program as it uses earth abundant, non-precious metal catalysts (cobalt).

化学系的生命过程化学项目将这个奖项授予卡拉·L·卡勒教授。罗切斯特大学的Bren开发和研究钴与肽的络合物，用于催化利用太阳能从水中产生氢气。氢气是一种有吸引力的燃料，因为它的高能量密度和清洁燃烧。采用电化学方法表征了钴配合物的催化活性。这些催化剂被整合到光化学系统中，用于将光能转化为化学能。本研究着重探讨反应途径及反应条件对产氢效率及产氢速率的影响。在这个项目中，研究生接受了最先进的生物化学，电化学和光化学技术的培训。该奖项还支持罗切斯特国家聋人技术研究所的听障学生参与研究，增强科学劳动力的多样性。该项目开发新的金属肽催化剂，并利用电催化以及光催化系统和组件研究水中析氢反应的催化机理。在这项工作中研究的金属肽催化析氢涉及质子耦合电子转移（PCET）的步骤，其中肽胺作为质子穿梭。在这项研究中，Bren教授确定了改变肽序列和胺pKa对PCET的影响以及对制氢速率和超电势的影响。此外，缓冲剂在传递质子到催化剂的作用进行了研究，在工作中理解催化在水环境中的广泛影响。最后，集成系统优化，以防止背电子转移和其他非生产性的途径在光化学反应的工程和调查。该项目的成功为以氢燃料的形式储存太阳能提供了环境友好的水溶性系统，并进一步发展了我们对PCET催化作用的理解。该提议被认为是在SusChEM计划下，因为它使用地球丰富的非贵金属催化剂（钴）。