Katalytische Fixierung von Kohlenstoffdioxid mittels früher Übergangsmetallkomplexe

二氧化碳是一种天然丰富的碳源，但很少被利用。从长期来看，利用二氧化碳作为一种可持续的、无毒的C1原料，用于生产有价值的化学产品或燃料，如羧酸及其衍生物或甲烷，将引起人们的兴趣。过渡金属催化领域的重大进展为解决节能催化CO2固定方案的挑战提供了基础。本研究项目旨在研究在lewis -酸硼烷共催化剂存在下，一系列阳离子3和4基无碱金属-烷基配合物对CO2的活化和功能化。关键步骤包括通过配位到高度亲氧的金属中心并插入金属-碳或-氢化物片段以产生金属-羧酸盐来激活二氧化碳。在短期内，预期的金属-羧酸类的功能化方案将使用路易斯酸活化的13和14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。预计这些工作将为调查工业上适用的共反应物（如H2）用于CO2还原和功能化的利用提供基础。

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.