Katalytische Fixierung von Kohlenstoffdioxid mittels früher Übergangsmetallkomplexe

二氧化碳是一种天然丰富，但很少使用的碳源。从长远来看，CO2的利用将作为用于生产有价值的化学产品或燃料（例如羧酸及其衍生物或甲烷）的可持续且无毒的C1原料而受到关注。过渡金属催化领域的实质性进展为努力奋进节能催化CO2固定方案的挑战提供了基础。本研究项目旨在研究在路易斯酸硼烷助催化剂存在下，用一系列阳离子第3族和第4族无碱金属-烷基络合物活化和官能化CO2。关键步骤包括通过与高度亲氧金属中心配位并插入金属-碳或-氢化物片段以产生金属-羧酸盐的CO2活化。在短期内，金属羧酸盐物质的预期官能化方案将利用刘易斯酸活化的第13和14族基还原剂，例如硅烷/硼烷组合。在这种情况下，活性催化剂的再生是特别感兴趣的。这些努力预计将提供基础，调查利用工业上适用的共反应物，如H2，CO2还原和功能化。

Carbon dioxide is a naturally abundant, yet little used source of carbon. Over the long term, the utilization of CO2 will be of interest as a sustainable, and nontoxic C1 feedstock for the production of valuable chemical products or fuels, such as carboxylic acids and derivatives thereof, or methane. Substantial progress in the field of transition metal catalysis has provided a basis to endeavor the challenge of energy-efficient catalytic CO2 fixation schemes. This research project is directed at studying the activation and functionalization of CO2 with a series of cationic group 3 and 4 base-free metal-alkyl complexes in the presence of Lewis-acid borane cocatalysts. Key steps involve CO2 activation through coordination to a highly oxophilic metal center and insertion into a metal-carbon or -hydride fragment to produce a metal-carboxylate. Over the short term, the anticipated functionalization schemes of metal-carboxylate species will utilize Lewis acid activated group 13 and 14 based reducing agents, e.g. silane/ borane combinations. The regeneration of an active catalyst is of particular interest in this context. These efforts are anticipated to provide basis to survey the utilization of industrially applicable coreactants, such as H2, for CO2 reduction and functionalization.