Growing Carbon Chains on Organometallic Networks

一氧化碳（CO）和二氧化碳（CO2）的化学性质深深植根于我们未来的能源生产、化学制造和可持续生活计划中。近十年来，二氧化碳的修复已成为一个重要的研究课题，将二氧化碳转化为碳氢化合物已在工业上得到大规模应用。催化是这个行业发展的基础。COx-to-fuels、COx-to-molecules和COx-to-materials （x = 1或2）的研究对于经济的增长、生活质量的改善和对导致气候变化的气体排放的调控是不可或缺的。可以说，在这一领域最成熟的技术是费托催化（F-T）。F-T过程将CO和H2的混合物转化为短链到中链碳氢化合物。最近的研究集中在利用富含二氧化碳的气流。该反应可视为CO / CO2的可控聚合和加氢反应，以生成液体燃料。尽管F-T催化有很多优点，但它产生的是简单的烷烃和烯烃，而不是复杂的分子。碳链的形成伴随着氧原子以水的形式被去除，从而降低了复杂性和价值。F-T没有利用在结合COx单元形成链时可能引入的潜在化学复杂性。在这个项目中，我们将开发一种全新的方法，在化学制造中使用CO和CO2。我们计划利用我们实验室最近的一项显著发现（JACS, 2018, 13614）：有机金属网络上可以从CO和CO2中生长出3到4个单位长度的碳链。我们将发展基础科学，发现连锁增长的规律。我们将提供新的方法，从CO和CO2中产生具有大小和形状控制的小碳链。新的碳链将作为复杂有机分子结构的主要分子成分在合成中得到开发。该项目的长期愿景是开发一种现代催化方法，与F-T工艺和二氧化碳-材料研究相辅相成。一种利用CO和CO2构建分子复杂性的物质。该提案描述了一个为期三年的项目，代表了从发现到实现这一目标的第一步。

The chemistry of carbon monoxide (CO) and carbon dioxide (CO2) is deeply embedded in our future plans for energy production, chemical manufacturing and sustainable living. Remediation of CO2 has become a major topic of research in the last ten years and conversion of CO to hydrocarbons is already being applied on vast scales in industry. Catalysis underpins the development of this industry. COx-to-fuels, COx-to-molecules and COx-to-materials (x = 1 or 2) research is indispensable for the growth of the economy, improvement of quality of life, and regulation of gas emissions that contribute to climate change. Arguably the most established technology operating in this landscape if Fischer-Tropsch (F-T) catalysis. The F-T process converts mixtures of CO and H2 into short to medium chain hydrocarbons. Recent research has focused on the use of CO2 rich gas streams. This reaction can be considered as a controlled polymerisation and hydrogenation of CO / CO2 to generate liquid fuels. Despite its advantages, F-T catalysis produces simple alkanes and alkenes, not complicated molecules. Carbon chain formation occurs alongside removal of the oxygen atoms, in the form of H2O, reducing complexity and value. F-T does not capitalise on the potential chemical intricacy that could be introduced when combining COx units to form chains.In this project we will develop an entirely new approach to use CO and CO2 in chemical manufacture. We plan to exploit a remarkable recent finding from our labs (JACS, 2018, 13614): that carbon chains of 3 to 4 units of length can be grown from CO and CO2 on organometallic networks. We will develop underpinning science to discover the rules for chain growth. We will deliver new approaches to generate small carbon chains from CO and CO2 with control of size and shape. The new carbon chains will be exploited in synthesis as the major molecular component in the construction of complex organic molecules.The long-term vision behind this project is the development of a modern approach in catalysis that is complementary to both F-T processes and CO2-to-materials research. One that builds molecular complexity from CO and CO2. This proposal describes a three-year project that represents the first steps from discovery toward this goal.