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A New Class of Hybrid Polyoxometalate Catalysts for C-H Functionalisation

用于 C-H 官能化的新型杂化多金属氧酸盐催化剂

基本信息

批准号：
EP/V047124/1
负责人：
Hon Lam
金额：
$ 25.73万
依托单位：
University of Nottingham
依托单位国家：
英国
项目类别：
Research Grant
财政年份：
2021
资助国家：
英国
起止时间：
2021 至无数据
项目状态：
已结题

来源：
https://gtr.ukri.org/projects?ref=EP%2FV047124%2F1
关键词：
New Class Hybrid Polyoxometalate Catalysts

项目摘要

Many decades of research in chemical synthesis have provided numerous new reactions to prepare molecules required by society, such as pharmaceuticals, agrochemicals, and materials. At the forefront of modern synthesis is late-stage catalytic C-H functionalisation (LSF), which can be faster and more efficient for producing libraries of diverse compounds compared with conventional synthetic approaches, where diversification occurs at an early stage and more highly functionalised substrates are required. However, despite numerous advances, significant challenges remain. The majority of LSF reactions occur at positions dictated by the intrinsic reactivity of the substrates, defined on the basis of steric and/or electronic factors. The ability to override intrinsic substrate reactivity to functionalise at "unexpected" sites in a controllable and switchable manner, is an ongoing challenge.Key to making advances in this area is the development of fundamentally new types of catalysts operating on unique design principles to override intrinsic substrate reactivity and control site-selectivity. In particular, harnessing a wide range of non-covalent and dynamic covalent interactions to bind and orient substrates to expose one particular site towards the reactive part of the catalyst will be required. In this project, we propose to develop a new class of catalysts for highly site-selective C-H functionalisation, using photochemical activation. Polyoxometalate clusters will be modified with organic groups to give organic-inorganic hybrids containing substrate binding units to coordinate and orient substrates to override intrinsic reactivity. These new hybrid catalysts will be used for diverse C-H functionalisation reactions of a wide range of compounds, such as steroids and peptides. The preparation of chiral catalysts to enable the synthesis of chiral products enriched in one particular enantiomer (non-superimposable mirror image) will also be investigated.We hope this research will enable the development of increasingly more versatile and efficient catalysts for chemical synthesis.

几十年的化学合成研究提供了许多新的反应来制备社会所需的分子，如药物、农用化学品和材料。现代合成的前沿是后期催化C-H功能化（LSF），与传统的合成方法相比，它可以更快、更有效地产生多种化合物的文库，在传统的合成方法中，多样化发生在早期阶段，需要更高功能化的底物。然而，尽管取得了许多进展，但仍存在重大挑战。大多数LSF反应发生在由底物的固有反应性决定的位置，根据空间和/或电子因素确定。能够以可控和可切换的方式覆盖内在的底物反应性，在“意想不到的”位置发挥功能，是一个持续的挑战。在这一领域取得进展的关键是开发基于独特设计原理的新型催化剂，以超越固有的底物反应性并控制位点选择性。特别是，需要利用广泛的非共价和动态共价相互作用来结合和定向底物，以使一个特定的位点暴露于催化剂的活性部分。在这个项目中，我们建议开发一种新的催化剂，用于高度选择性的C-H功能化，利用光化学活化。多金属氧酸盐簇将被有机基团修饰，从而得到含有底物结合单元的有机-无机杂化物，以协调和定向底物，从而超越内在反应性。这些新的杂化催化剂将用于各种化合物的C-H功能化反应，如类固醇和肽。还将研究手性催化剂的制备，以合成富含一种特定对映体（非重叠镜像）的手性产物。我们希望这项研究将推动越来越多的多功能和高效的化学合成催化剂的发展。