Burning fossil fuels worldwide has led to an increasing CO2 concentration in the atmosphere to such a large extent that global climate change caused by greenhouse gases has become a major ecological challenge. At present, its amount can be reduced by either capture and storage or by chemical conversion and utilization. There is no doubt that carbon dioxide storage is a cheaper solution and that it is useful for reducing CO2 emissions quickly. Unfortunately, it does not solve the accumulation problem in the long term, whereas converting CO2 into carbon-containing value-added products and feedstock does. The catalytic conversion of CO2/H2/CO to methanol is already being performed on an industrial scale. Other products, such as formic acid and its derivatives, can be synthesized by carbon dioxide hydrogenation. However, despite this progress, we are still far from the point where carbon dioxide becomes a concrete player in the sustainable chemistry/energy market. Significant steps should be taken toward developing more efficient catalysts for CO2 conversion processes, as well as developing new reaction schemes that allow for more efficient utilization of carbon dioxide in fine and bulk synthesis. The talk is devoted to designing ligand-metal cooperative catalytic systems for the dehydrogenation of formic acid and hydrogenation of CO2. Our studies revolve around a family of 3-dimensional PC(sp3)P pincer complexes developed by our group. The synthetic approach leading to all these examples is straightforward and represents a modular and divergent approach to a variety of 3-dimensional platforms equipped with custom-tailored primary and secondary coordination spheres. In particular, we address the cooperative activation and functionalization of carbon dioxide by bifunctional catalysts possessing transition metals in the primary coordination sphere and a pendant Lewis acidic functionality in the secondary sphere.

Multifunctional pincer complexes possessing a secondary coordination sphere as catalysts for CO2 hydrogenation

ACS Fall 2021

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