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Developing Continuous Electroorganic Catalysis - It's Got Potential

开发连续有机电催化——它有潜力

基本信息

批准号：
EP/R006504/1
负责人：
Louis Morrill
金额：
$ 50.45万
依托单位：
CARDIFF UNIVERSITY
依托单位国家：
英国
项目类别：
Research Grant
财政年份：
2017
资助国家：
英国
起止时间：
2017 至无数据
项目状态：
已结题

来源：
https://gtr.ukri.org/projects?ref=EP%2FR006504%2F1
关键词：
Developing Continuous Electroorganic Catalysis Got

项目摘要

The combination of electricity with chemical reactions has a long history. The ability to use a single electron from an electric current in order to trigger a chemical reaction is an exciting concept, especially from the perspective of sustainability. Electrons are one of the cleanest possible chemical reagents (i.e. there is no waste generated from their use) with photons of light representing a complementary alternative. It is surprising therefore that organic chemistry, the branch of chemistry involved with creating molecules for society, such as pharmaceuticals, crop-protection agents, dyes, pigments, flavours, fragrances and polymers does not often use such electro-chemical methods at both the discovery and manufacture stages. One of the key reasons for this lack of adoption is that often the applied current, or the energy of the electron, is not properly tuned to the reaction system. This can lead to undesired reactions and impure reaction profiles. However, there have been some recent pioneering developments in the field that may permit broadening of the application of this electro-organic chemistry. The developments are two-fold and concern the chemistry and the reactor design.1) With regards to the chemistry, several examples now exist where complex reaction processes can be triggered by appropriate choice of electrolyte and careful planning of the chemical reactants. Furthermore, it has recently been proven that catalytic systems can be sustained by the input of electrons, with such processes giving rise to complex and interesting molecules of the kind that could feature in 'molecules for society'.2) With regards to the reactor design, the development and advancement of continuous flow chemistry (chemistry in pipes and tubing circuits rather than beakers and flasks) has permitted the lowering of the electric current and thus allows more sensitive 'surgical incisions' to be made in the reaction process, thus reducing the undesired reactions and propensity to yield impure reaction profiles. This proposal looks to work in an area of catalysis known as organo-catalysis, where a small amount of an organic molecule is used to accelerate the rate of reactions (this is in contrast to a precious metal-based system). Here the electro-chemistry approach will help to sustain and maintain the catalytic cycle. Notably, in all other organo-catalytic processes of this type an equal amount of an addition chemical is needed to maintain the catalytic activity. This chemical is purely sacrificial in nature and is thus extremely wasteful. A preliminary hit from the UK has already demonstrated that organo-catalytic reactions can be sustained using electro-chemical methods. This proposal aims to greatly diversify the application of this observation. The combination of an organo-catalytic, electro-chemical and continuous flow approach will serve to amplify the sustainability of the processes that we use to deliver these industrially useful reactions.

电与化学反应的结合有着悠久的历史。利用电流中的单个电子来触发化学反应的能力是一个令人兴奋的概念，尤其是从可持续性的角度来看。电子是最干净的化学试剂之一（即使用它们不会产生废物），光子则是互补的替代品。因此，令人惊讶的是，有机化学是化学的一个分支，涉及为社会创造分子，如药物、作物保护剂、染料、色素、香精、香料和聚合物，在发现和制造阶段并不经常使用这种电化学方法。不被采用的一个关键原因是，通常施加的电流或电子的能量没有适当地调整到反应系统。这可能导致不期望的反应和不纯的反应概况。然而，最近在该领域有一些开创性的发展，可能允许扩大这种电有机化学的应用。这些发展是两方面的，涉及化学和反应堆设计。1)在化学方面，现在有几个例子可以通过适当选择电解质和仔细规划化学反应物来触发复杂的反应过程。此外，最近已经证明，催化系统可以通过电子的输入来维持，这样的过程会产生复杂而有趣的分子，这种分子可能会成为“社会分子”的特征。2)在反应器设计方面，连续流动化学的发展和进步（管道和管道回路中的化学，而不是烧杯和烧瓶）允许降低电流，从而允许在反应过程中进行更敏感的“手术切口”，从而减少不希望发生的反应和产生不纯反应曲线的倾向。这一提议似乎适用于被称为有机催化的催化领域，在该领域中，少量的有机分子被用来加速反应的速度（这与基于贵金属的系统形成对比）。这里电化学方法将有助于维持和维持催化循环。值得注意的是，在所有其他这种类型的有机催化过程中，需要等量的添加化学物质来维持催化活性。这种化学物质本质上是纯粹的牺牲，因此是极其浪费的。来自英国的一项初步研究已经证明，使用电化学方法可以维持有机催化反应。这一建议旨在使这一观察结果的应用大为多样化。有机催化，电化学和连续流方法的结合将有助于扩大我们用于提供这些工业上有用的反应的过程的可持续性。

项目成果

期刊论文数量（10）

专著数量（0）

科研奖励数量（0）

会议论文数量（0）

专利数量（0）

Ball-Milling-Enabled Reactivity of Manganese Metal**

锰金属的球磨反应活性**

DOI：
10.1002/ange.202108752
发表时间：
2021
期刊：
Angewandte Chemie
影响因子：
0
作者：
Nicholson W
通讯作者：
Nicholson W

Manganese-Catalyzed Electrochemical Deconstructive Chlorination of Cycloalkanols via Alkoxy Radicals

DOI：
10.26434/chemrxiv.9275441.v1
发表时间：
2019-08
期刊：
Organic Letters
影响因子：
5.2
作者：
Benjamin D W Allen;Mishra Deepak Hareram;Alex C Seastram;T. McBride;T. Wirth;D. Browne;Louis C. Morrill-Loui
通讯作者：
Benjamin D W Allen;Mishra Deepak Hareram;Alex C Seastram;T. McBride;T. Wirth;D. Browne;Louis C. Morrill-Loui

Ball Milling Enabled Reactivity of Manganese Metal

球磨使锰金属具有反应性

DOI：
10.33774/chemrxiv-2021-s7r6b
发表时间：
2021
期刊：
影响因子：
0
作者：
Browne D
通讯作者：
Browne D

Ball-Milling-Enabled Reactivity of Manganese Metal*.

DOI：
10.1002/anie.202108752
发表时间：
2021-10-18
期刊：
Angewandte Chemie (International ed. in English)
影响因子：
0
作者：
Nicholson WI;Howard JL;Magri G;Seastram AC;Khan A;Bolt RRA;Morrill LC;Richards E;Browne DL
通讯作者：
Browne DL

Iron-Catalyzed Methylation Using the Borrowing Hydrogen Approach