New Insights, New Catalysts and New Processes using Enantioselective Carbonylations.
New Insights, New Catalysts and New Processes using Enantioselective Carbonylations.
批准号:
EP/M003868/1
负责人:
Matthew Clarke
金额:
$66.33万
依托单位:
依托单位国家:
英国
项目类别:
Research Grant
财政年份:
2014
资助国家:
英国
项目状态:
已结题
起止时间:
2014 至 --
中文摘要
这个项目属于化学催化领域。催化在大多数日常用品(塑料、药品、食品补充剂、香精/香料、饰面和涂料)的生产中都有应用。在最重要的反应中,通常用于制造各种产品,如清漆,塑料,香蕉调味剂和消炎药!,是那些使用一氧化碳作为构件的。一氧化碳是最便宜的化学物质之一,可以来自煤炭、石油、天然气和可再生能源。由于一氧化碳价格低廉,而且在催化剂的作用下,它可以与其他分子以一种非常干净的方式反应,这些催化羰基化反应产生的废物很少,即使在非常大的规模(数百万吨)下也是经济的。这些特点也有可能使这种反应成为一种清洁和经济的方式来制造更高价值、更复杂的分子,如药物。然而,为了制造这些分子,需要对几种类型的选择性进行精确的控制。例如,许多药物以两种镜像形式存在(光学异构体),必须优先制造一种异构体。另一种光学异构体通常是无活性的,或者实际上可以引起另一种生物效应(沙利度胺的副作用是一种光学异构体引起不必要的生物效应的悲惨例子)。这导致化学家们进行了大量的研究工作,以开发能够选择性地产生单一光学异构体的化学反应(“不对称合成”)。这一领域取得了重大进展,一些不对称合成的先驱获得了几项诺贝尔化学奖。研究小组最近获得了令人兴奋的初步结果,他们开发的催化剂可以控制几种羰基化模型研究中几个方面的选择性,包括对一种光学异构体的优异选择性。这个新项目致力于在这些结果的基础上开发通往不同目标化学品的路线。高价值精细化学品/医药中间体部门需要开发新型羰基化或在迄今为止未反应的底物上工作的能力。一些潜在的令人兴奋的新反应,如将几个反应组合成一个合成阶段,一个反应器,一套溶剂,净化等被提出。该项目还将获得新催化剂的机理见解,并利用这些信息进行精细的催化剂设计和催化剂的合理设计,以完成新的任务。总的来说,该项目有可能对基础知识产生影响,为新的工业目标提供概念证明,并为一系列重要化学品提供更好、更良性的途径。
英文摘要
This project is in the field of chemo-catalysis. Catalysis is used somewhere in the manufacture of most everyday items (plastics, drugs, food supplements, flavours/fragrances, finishes and coatings). Amongst the most important reactions, generally used in the manufacture of diverse products such as varnishes, plastics, banana flavouring and anti-inflammatories!, are those that use carbon monoxide as a building block. Carbon monoxide is one of the cheapest chemicals and can come from coal, oil, gas and renewables. Due to the low price of carbon monoxide and the fact that it can, in the presence of a catalyst, react in a very clean fashion with other molecules, these catalytic carbonylation reactions generate very little waste and are economical even at very large scale (Millions of tonnes). These features also potentially make this type of reaction a clean and economical way to make much higher value, more sophisticated molecules such as drugs. However, to make these molecules, exquisite control of several types of selectivity is needed. For example, many drugs exist as two mirror image forms (optical isomers) and one isomer must be made prefentially. The other optical isomer is often inactive, or in fact can cause an alternative biological effect (The side effects of Thalidomide are a tragic example of one optical isomer causing unwanted biological effects). This has led to a massive research effort by chemists to develop chemical reactions that are capable of selectively producing a single optical isomer ('Asymmetric Synthesis'). Significant developments have been made in this area, with several Nobel prizes in chemistry being awarded to some of the pioneers in asymmetric synthesis. The investigators group has recently obtained exciting preliminary results developing catalysts that can control several aspects of selectivity in model studies on a few types of carbonylation, including excellent selectivity to one optical isomer. This new project addresses building on these results to develop routes to different target chemicals.Development of new types of carbonylation or the ability to work on hitherto unreactive substrates is needed for the higher value fine chemicals/pharma intermediates sector. A number of potentially exciting new reactions such as combining several reaction into one stage of a synthesis, and one reactor, one set of solvents, purification etc. are proposed. This project will also gain mechanistic insights on the new catalyst and use this information to generate refined catalyst design and rational design of catalysts to accomplish new tasks. Overall the project has the potential to impact on fundamental knowledge, generate proof of concept for new industrial targets, and provide better, more benign routes to a range of important chemicals.
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DOI:
10.1002/ejoc.202000336
发表时间:
2020-05
期刊:
European Journal of Organic Chemistry
影响因子:
2.8
作者:
[Sophie H. Gilbert;J. Fuentes;D. Cordes;A. Slawin;M. Clarke]
通讯作者:
Sophie H. Gilbert;J. Fuentes;D. Cordes;A. Slawin;M. Clarke
DOI:
10.1021/acs.orglett.7b01049
发表时间:
2017-05
期刊:
Organic letters
影响因子:
5.2
作者:
[Rachael Pittaway;J. Fuentes;M. Clarke]
通讯作者:
Rachael Pittaway;J. Fuentes;M. Clarke
A Highly Enantioselective Alkene Methoxycarbonylation Enables a Concise Synthesis of ( S )-Flurbiprofen
高度对映选择性烯烃甲氧基羰基化可实现 (S)-氟比洛芬的简洁合成
DOI:
10.1002/ejoc.201700791
发表时间:
2017
期刊:
European Journal of Organic Chemistry
影响因子:
2.8
作者:
[Harkness G]
通讯作者:
Harkness G
DOI:
10.1002/chem.201502049
发表时间:
2015-07-20
期刊:
Chemistry (Weinheim an der Bergstrasse, Germany)
影响因子:
--
作者:
[Fuentes JA, Pittaway R, Clarke ML]
通讯作者:
Clarke ML
DOI:
10.1021/jacs.7b09164
发表时间:
2017-11-08
期刊:
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
影响因子:
15
作者:
[Dingwall, Paul, Fuentes, Jose A., Clarke, Matthew L.]
通讯作者:
Clarke, Matthew L.
共 8 条
Highly reactive catalysts for the hydrogenation of poorly reactive substrates
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批准号:EP/G063591/1
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项目类别:Research Grant
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资助金额:$2.29万
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财政年份:2009
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负责人:Matthew Clarke
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依托单位:
Self-assembly of asymmetric catalysts
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批准号:EP/G036314/1
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项目类别:Research Grant
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资助金额:$44.11万
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财政年份:2009
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负责人:Matthew Clarke
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依托单位:
Ruthenium complexes of chiral tridentate ligands: a new class of catalyst for asymmetric ketone and imine hydrogenation.
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批准号:EP/F030576/1
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项目类别:Research Grant
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资助金额:$31.29万
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财政年份:2007
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负责人:Matthew Clarke
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依托单位:
国内基金
海外基金
Behavioral Insights on Cooperation in Social Dilemmas
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批准号:--
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项目类别:外国优秀青年学者研究基金项目
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资助金额:--
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批准年份:2024
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负责人:LIEN,Jaimie Wei-Hung
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依托单位: