Electrocatalytic Oxidation of Alcohols, Amines, and Carbon-Carbon Bonds

醇、胺和碳-碳键的电催化氧化

基本信息

批准号：
1762350
负责人：
William Jones
金额：
$ 45.4万
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：
2018
资助国家：
美国
起止时间：
2018-09-01 至 2022-08-31
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1762350&HistoricalAwards=false
关键词：
Electrocatalytic Oxidation Alcohols Amines Carbon

项目摘要

With funding from the Chemical Catalysis Program of the Division of Chemistry, Dr. William D. Jones of the University of Rochester is developing new catalytic materials capable of removing hydrogen from organic molecules to make more valuable products. In this new method, hydrogen is transferred from the organic molecule to a carrier molecule using a metal catalyst. The carrier molecules are then recycled many times. Dr. Jones is studying the individual steps of the reaction cycle. These catalytic reactions have applications in the synthesis of pharmaceuticals and may also provide a better understanding of how electrical energy from hydropower or wind turbines could be captured and stored for later use on demand. Dr. Jones is engaged in outreach activities to inform the public about novel new concepts for energy storage and organic compound synthesis. He and his group participate in public radio shows such as WXXI Connections, and speak on television news programs. The researchers include both undergraduate and graduate students who are being trained to solve difficult technical problems of broad societal interest. This research advances the national health and prosperity by contributing to technical innovations in the pharmaceuticals and renewable energy industries. Dr. Jones is developing homogeneous transition metal catalysts that can be used to dehydrogenate alcohols, amines, and heterocycles electrochemically. The group is studying the use of new and known catalysts in combination with quinones as electron transfer mediators, as the latter have the ability to undergo reversible electrochemical reduction and oxidation, and show promise as mediators with transition metal catalysts. The group is examining stoichiometric reactions for alcohol and amine dehydrogenation with various quinones as hydrogen acceptors. The group is also developing electrochemical recycling of the hydroquinone hydrogen acceptors. By proper choice of solvent and electrolyte, an electrochemical route for dehydrogenations is being extended to substrates that can produce heterocycles such as indoles and quinolones. Finally, this electrochemical method is being used in applications for dehydrogenation of activated C-C bonds to generate oxidized organic products that serve as building blocks in the chemical and pharmaceutical industry. This work has the potential to occur with dihydrogen as the only byproduct, using electrochemistry to provide the driving force for the thermodynamically uphill reaction. This work is focusing on the use of these catalysts in organic synthesis, but also can find applications in hydrogen storage, and fuel cells. The students engaged in this research are learning advanced techniques for handling sensitive compounds and therefore are being trained as Highly Qualified Personnel (HQP) for work in advanced industrial research labs.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.

在化学系化学催化计划的资助下，罗切斯特大学的William D. Jones博士正在开发能够从有机分子中去除氢以制造更有价值的产品的新催化材料。在这种新方法中，使用金属催化剂将氢从有机分子转移到载体分子。然后将载体分子回收多次。琼斯博士正在研究反应周期的各个步骤。这些催化反应在合成药品中具有应用，还可以更好地了解如何捕获水力发电或风力涡轮机的电能，以供以后使用。琼斯博士从事外展活动，以告知公众有关储能和有机复合合成的新型新概念。他和他的小组参加了公共广播节目，例如WXXI Connections，并在电视新闻节目中发表讲话。研究人员包括正在接受培训的本科和研究生，以解决广泛的社会兴趣的困难技术问题。这项研究通过为制药和可再生能源行业的技术创新做出贡献，推动了民族健康和繁荣。琼斯博士正在发展均匀的过渡金属催化剂，可用于电化学上脱氢醇，胺和杂环。该小组正在研究新的和已知的催化剂与奎因酮作为电子传递介体的使用，因为后者具有经历可逆的电化学还原和氧化的能力，并显示出具有过渡金属催化剂的介体的希望。该小组正在研究与各种喹酮作为氢受体的酒精和胺脱氢作用的化学计量反应。该组还正在开发氢醌氢受体的电化学回收。通过正确选择溶剂和电解质，将脱氢的电化学途径扩展到可以产生诸如吲哚和喹诺酮等杂环的底物。最后，这种电化学方法用于应用于激活的C-C键脱氢，以生成氧化有机产品，这些有机产品是化学和制药行业中的基础。这项工作有可能以二氢为唯一的副产品发生，使用电化学为热力学上坡反应提供驱动力。这项工作的重点是在有机合成中使用这些催化剂，但也可以在氢气中找到应用和燃料电池。从事这项研究的学生是学习用于处理敏感化合物的高级技术，因此正在接受高级工业研究实验室工作的高素质人员（HQP）培训。基金会的智力优点和更广泛的影响审查标准。

项目成果

期刊论文数量（6）

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 functionalization of benzene by boranes using trispyrazolylborate complexes

使用三吡唑基硼酸酯配合物通过硼烷对苯进行官能化

DOI：
10.1016/j.poly.2021.115042
发表时间：
2021
期刊：
Polyhedron
影响因子：
2.6
作者：
Vetter, Andrew J.;DiBenedetto, Tarah A.;Ritz, Mikhaila D.;Jones, William D.
通讯作者：
Jones, William D.

Bisoxazoline-pincer ligated cobalt-catalyzed hydrogenation of alkenes

DOI：
10.1016/j.poly.2020.114416
发表时间：
2020-04
期刊：
Polyhedron
影响因子：
2.6
作者：
Mikhaila D. Ritz;A. M. Parsons;Philip N Palermo;W. Jones
通讯作者：
Mikhaila D. Ritz;A. M. Parsons;Philip N Palermo;W. Jones

Synthesis, characterization, and structure determination of Cp*Ir(dpms)Cl

Cp*Ir(dpms)Cl 的合成、表征和结构测定

DOI：
10.1016/j.ica.2022.121210
发表时间：
2022
期刊：
Inorganica Chimica Acta
影响因子：
2.8
作者：
Pohorenec, Ryan;Drelles, William G.;Cuneo, Daniel;Brennessel, William W.;Jones, William D.
通讯作者：
Jones, William D.

Reversible Concerted Metalation–Deprotonation C–H Bond Activation by [Cp*RhCl 2 ] 2

[Cp*RhCl 2 ] 2 可逆协同金属化 - 去质子化 C - H 键激活