权益分类	功能权益	普通用户	{{item.name}}会员
{{category.name}}	{{benefitItem.name}}

CAS: Principles of Cooperativity for the Electrocatalytic Reduction of Carbon Dioxide

CAS：二氧化碳电催化还原的协同原理

基本信息

批准号：
1955268
负责人：
Craig Grapperhaus
金额：
$ 32.35万
依托单位：
University of Louisville Research Foundation Inc
依托单位国家：
美国
项目类别：
Standard Grant
财政年份：
2020
资助国家：
美国
起止时间：
2020-08-01 至 2024-07-31
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1955268&HistoricalAwards=false
关键词：
CAS Principles Cooperativity Electrocatalytic Reduction

项目摘要

The Chemical Catalysis Program of the Division of Chemistry supports the research program of Professor Craig Grapperhaus and Dr. Joshua Spurgeon of the University of Louisville. This project focuses on the capture and reactivity of carbon dioxide. Generating fuels and chemicals using electricity is one of the most favorable approaches for using intermittent renewables such as wind and solar. Also, making commercial chemicals from electricity may also be more energetically efficient than using current methods which involve heating. This project develops more sustainable systems to capture carbon dioxide and convert it to fuels or other chemical products. The new reactions employ an abundant metal, such as zinc, within a supporting molecular framework synthesized from inexpensive starting materials. The fundamental research could provide a pathway by which renewable electricity and high concentrations carbon dioxide from fossil fuel combustion could be used to form commercially useful materials. The research provides undergraduate and graduate students hands-on interdisciplinary experience in renewable energy research preparing them for careers in science, technology, engineering, and mathematics. High-school student participants in the annual renewable energy workshop at the University of Louisville have the opportunity to participate in the research and develop independent science fair projects.With funding from the Chemical Catalysis Program of the Division of Chemistry, Professor Craig Grapperhaus and Dr. Joshua Spurgeon of the University of Louisville are developing hybrid thiosemicarbazone-pyridylhydrazone metal complexes as co-catalysts for carbon dioxide capture and reduction. The co-catalysts utilize metal-ligand cooperativity through the incorporation of neighboring Lewis acid and Lewis base sites. Reductions will be performed at a variety of electrodes including Cu-Ni alloys. The project will investigate the factors influencing product distribution, reaction mechanism, and reactivity between the co-catalyst and electrode. Projected outcomes include the quantification of the effect of Lewis acidity and Lewis basicity on the binding and catalytic reactivity of carbon dioxide with the metal co-catalyst. The research team will identify of unique C-C coupled products from carbon dioxide reduction at the Cu-Ni alloy and draw mechanistic insights into the C-C coupling process. The group will increase fundamental knowledge of the reactivity of Cu-Ni alloys with varying compositions. High-school student participants in the annual renewable energy workshop at the University of Louisville have the opportunity to participate in the research and develop independent science fair projects.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.

化学系的化学催化计划支持路易斯维尔大学克雷格·格拉珀豪斯教授和约书亚·斯普金博士的研究计划。该项目的重点是二氧化碳的捕获和反应性。使用电力生产燃料和化学品是使用风能和太阳能等间歇性可再生能源的最有利方法之一。此外，用电力制造商业化学品也可能比使用目前涉及加热的方法更节能。该项目开发了更可持续的系统来捕获二氧化碳，并将其转化为燃料或其他化学产品。新的反应使用了大量的金属，如锌，在由廉价的起始材料合成的支持分子框架内。基础研究可以提供一种途径，通过这种途径，可再生电力和化石燃料燃烧产生的高浓度二氧化碳可以用来形成商业有用的材料。这项研究为本科生和研究生提供了可再生能源研究的跨学科实践经验，为他们在科学、技术、工程和数学领域的职业生涯做好准备。路易斯维尔大学一年一度的可再生能源研讨会的高中生参与者有机会参与研究和开发独立的科学博览会项目。在化学系化学催化计划的资助下，路易斯维尔大学的克雷格·格拉珀豪斯教授和约书亚·斯普金博士正在开发混合硫代氨基脲-吡啶肼金属络合物，作为二氧化碳捕获和减少的联合催化剂。该助催化剂通过引入邻近的Lewis酸和Lewis碱位来利用金属-配体的协作性。还原将在包括铜镍合金在内的各种电极上进行。该项目将研究影响产物分布的因素、反应机理以及助催化剂与电极之间的反应性。预计的结果包括量化路易斯酸度和刘易斯碱度对二氧化碳与金属助催化剂的结合和催化反应性的影响。研究小组将确定铜镍合金二氧化碳还原产生的独特的碳-碳耦合产物，并从机理上深入了解碳-碳耦合过程。该小组将增加关于不同成分的铜镍合金反应性的基础知识。参加路易斯维尔大学一年一度的可再生能源研讨会的高中生有机会参与研究和开发独立的科学博览会项目。该奖项反映了NSF的法定使命，并通过使用基金会的智力优势和更广泛的影响审查标准进行评估，被认为值得支持。

项目成果

期刊论文数量（7）

专著数量（0）

科研奖励数量（0）

会议论文数量（0）

专利数量（0）

The pH and Potential Dependence of Pb‐Catalyzed Electrochemical CO 2 Reduction to Methyl Formate in a Dual Methanol/Water Electrolyte

双甲醇/水电解质中 Pb 催化 CO 2 电化学还原成甲酸甲酯的 pH 和电位依赖性

DOI：
10.1002/cssc.202102289
发表时间：
2022
期刊：
ChemSusChem
影响因子：
8.4
作者：
Hofsommer, Dillon T.;Liang, Ying;Uttarwar, Sandesh S.;Gautam, Manu;Pishgar, Sahar;Gulati, Saumya;Grapperhaus, Craig A.;Spurgeon, Joshua M.
通讯作者：
Spurgeon, Joshua M.

Physical structure of constitutional isomers influences antiproliferation activity of thiosemicarbazone-alkylthiocarbamate copper complexes

异构体的物理结构影响缩氨基硫脲-烷基硫代氨基甲酸盐铜配合物的抗增殖活性

DOI：
10.1016/j.jinorgbio.2023.112288
发表时间：
2023
期刊：
Journal of Inorganic Biochemistry
影响因子：
3.9
作者：
Bajaj, Kritika;Andres, Sarah A.;Hofsommer, Dillon T.;Greene, Aidan F.;Hietsoi, Oleksandr;Mashuta, Mark S.;Weis, Theresa;Beverly, Levi J.;Bates, Paula J.;Buchanan, Robert M.
通讯作者：
Buchanan, Robert M.

Unravelling the potential of disposable and modifiable pencils as catalyst supports for hydrogen evolution reaction

揭示一次性和可修改铅笔作为析氢反应催化剂载体的潜力

DOI：
10.1039/d2nj03359c
发表时间：
2022
期刊：
New Journal of Chemistry
影响因子：
3.3
作者：
Paudel, Mohan;Daniels, Braydan;Arts, Amanda M.;Gupta, Alexander;Kalbfleisch, Theodore;Hofsommer, Dillon T.;Grapperhaus, Craig A.;Buchanan, Robert M.;Gupta, Gautam
通讯作者：
Gupta, Gautam

Investigations of Bis(alkylthiocarbamato)copper Linkage Isomers

双(烷硫基氨基甲酸酯)铜连接异构体的研究

DOI：
10.1021/acs.inorgchem.2c00371
发表时间：
2022
期刊：
Inorganic Chemistry
影响因子：
4.6
作者：
Bajaj, Kritika;Andres, Sarah A.;Hofsommer, Dillon T.;Galib, Mirza;Mashuta, Mark S.;Bennett, Brian;Narayanan, Badri;Buchanan, Robert M.;Bates, Paula J.;Grapperhaus, Craig A.
通讯作者：
Grapperhaus, Craig A.