Transition Metal/Aluminium Bimetallics for Cooperative Catalysis

催化-通过在反应结束时再生的化合物的干预来提高化学转化的速率和选择性（因此可以重复循环），代表了以资源有效的方式组装复杂分子的非常强大的工具。因此，催化是化学制造的核心，超过75%的化学产品在制造过程中的某些阶段需要使用催化剂。来自催化过程的产品的年度全球市场超过9万亿美元，并且催化剂广泛用于与商品和精细化学品、食品、药品、燃料、聚合物等的制造相关的关键工业过程中。此外，实现新的催化剂和催化过程对于在可持续框架内发展未来的生产能力至关重要，这减少了浪费并使化学原料得到最佳利用。碳和氢之间的键在天然化合物中无处不在。C-H键的直接官能化（即将它们转化为更有用的化学结构单元）代表了构建有价值的化学靶标的有吸引力的原子效率方法。然而，这种方法带来了许多化学挑战-与C-H键相对惰性（难以断裂）和化学均匀（难以选择性断裂）的事实有关。因此，难以实现反应性的控制。从酶（生物催化剂）中汲取灵感，这些问题中的一些可以通过开发双金属化合物（即含有两种金属的化合物）来解决-其中两种不同的金属被定制以完成不同的化学任务。该提案的关键是提供一种用于合成和优化催化剂的路线，其中一种金属是铝-一种在催化中具有悠久历史的元素。迄今为止，由于缺乏制造这种催化剂的可行路线，这种方法的发展受到阻碍。然而，利用我们最近的工作，我们有独特的机会来产生一系列的含铝双金属，可以系统地调整，以优化反应特性。在这样做的过程中，我们将不仅建立这些系统的基本化学反应特性，而且还建立它们在新型催化C-H官能化过程中的能力。

Catalysis - the enhancement of the rate and selectivity of a chemical transformation through the intervention of a compound that is regenerated at the end of reaction (and can therefore be repeatedly recycled), represents an immensely powerful tool for assembling complex molecules in a resource-efficient manner. As such, catalysis is central to chemical manufacturing, with over 75% of chemical products requiring the use of a catalyst at some stage in their manufacture. The annual world-wide market for products derived from catalytic processes is in excess of $9 trillion, and catalysts are widely employed in key industrial processes allied to the manufacture of commodity and fine chemicals, food products, pharmaceuticals, fuels, polymers, etc. Moreover, the realization of new catalysts and catalytic processes is critical to developing future production capabilities within a sustainable framework, which reduces waste and makes optimal use of chemical feedstocks. Bonds between carbon and hydrogen are ubiquitous in naturally occurring chemical compounds. Direct functionalization of C-H bonds (i.e. converting them into more useful chemical building blocks) represents an attractive, atom-efficient approach to construct valuable chemical targets. However, this approach brings a number of chemical challenges - relating to the facts that C-H bonds are relatively inert (difficult to break), and chemically uniform (so difficult to break selectively). Control of reactivity is therefore difficult to achieve. Drawing inspiration from enzymes (biological catalysts), a number of these issues can be addressed by exploiting bimetallic compounds (i.e. compounds containing two metals) - in which two different metals are tailored to accomplish different chemical tasks. The crux of this proposal is to offer a route for the synthesis and optimization of bimetallic catalysts in which one of the metals is aluminium - an element with a long history of exploitation in catalysis. The development of this approach has been hampered to date by the lack of viable routes to make such catalysts. However, exploiting our recent work, we have the unique opportunity to generate a range of aluminium-containing bimetallics that can be systematically tuned to optimize reactivity characteristics. In doing so, we will establish not only the fundamental chemical reactivity profiles of such systems, but also their capabilities in novel catalytic C-H functionalization processes.