Microporous metal oxides for the oxidation of alkanes to primary alcohols

新型选择性氧化反应催化剂的开发对工业界和学术界都具有决定性的重要意义。事实上，主要需要：（i）能够提供具有对所需产物的增强的选择性的节能工艺的催化剂和（ii）利用空气（分子氧）的氧化路线，用于更绿色的制造工艺。为了实现这些结果，该提案将开发新型结构的微孔金属氧化物用作催化剂。这些新材料将用于以分子氧为氧化剂由烷烃合成伯醇。伯醇在化学中起着至关重要的作用，因为它们是制药，食品添加剂和化妆品行业的基本组成部分。然而，全范围的伯醇难以合成获得，或从天然来源提取。除了少数能够催化单羟基化的细菌之外，所有用于烷烃氧化的现有催化剂都缺乏对所需醇产物的选择性的控制。这些可以选择性地官能化烃链末端的C-H键，而不攻击碳链内更具反应性的C-H键。因此，一个新的模式选择性氧化烷烃伯醇是必要的，将是极其重要的。事实上，这也将把烷烃从不可再生的化石燃料来源转化为有用的化学合成原料。因此，这些新的微孔金属氧化物将提供形状选择性控制的反应性结合氧化还原化学，如在酶系统中。本项目还将研究基本的催化机制，使用一系列光谱工具，包括X射线光电子能谱和电子顺磁共振，以及X射线衍射方法。这些见解将提供一种新的酒精制造技术，这将有利于英国工业，以及将影响催化以外领域的材料设计，例如材料科学，光谱学，仿生合成和化学工程。

The development of novel catalysts for selective oxidation reactions is an area of decisive importance for both industry and academia. In fact, there is a major need for: (i) catalysts capable of delivering energy-efficient processes with enhanced selectivity to a desired product and (ii) oxidation routes that make use of air (molecular oxygen) for greener manufacturing processes. To achieve these results, this proposal will develop novel structured microporous metal oxides to use as catalysts. These novel materials will be targeted to the synthesis of primary alcohols from alkanes using molecular oxygen as oxidant. Primary alcohols play a crucial role in chemistry, as they are essential building blocks for the pharmaceutical, food additives and cosmetics industries. However, a full range of primary alcohols is difficult to obtain synthetically, or to extract from natural sources.All of the current catalysts for alkane oxidation lack control of selectivity to a desired alcohol product, with the exception of a few bacteria capable of catalytic monohydroxylation. These can selectively functionalise C-H bonds at the end of a hydrocarbon chain without attacking more reactive C-H bonds within the carbon chain. Therefore, a new paradigm for selective oxidation of alkanes to primary alcohols is necessary and would be of immense importance. In fact, this would also convert alkanes from a non-renewable fossil fuel source into a useful chemical synthesis feedstock. Thus these new microporous metal oxides will deliver shape-selective control of reactivity combined with redox chemistry, as in enzymatic systems.This project will also investigate the fundamental catalytic mechanisms using an array of spectroscopic tools including X-ray photoelectron spectroscopy and electron paramagnetic resonance, as well as X-ray diffraction methods. These insights will deliver a new alcohol manufacturing technology that will be of benefit for the UK industry, as well as the design of materials that will impact areas beyond catalysis, e.g. materials science, spectroscopy, biomimetic synthesis and chemical engineering.