The efficient reduction of carbon dioxide (CO2) into value-added products is a cornerstone of future sustainable energy systems and chemical industries based on renewable energy and raw materials. Transition metal catalysis can selectively convert carbon dioxide to a single product platform that, however, rarely goes beyond the formate level. An important task consists of developing molecular systems that are adaptive and therefore, can selectively lead to different product platforms. This motivated a research team at the MPI CEC lead by Prof. Walter Leitner and Dr. Christophe Werlé to develop a cobalt-based catalytic system for the adaptive and highly selective transformation of carbon dioxide individually to either the formic acid, the formaldehyde, or the methanol level, demonstrating the possibility of molecular control over the desired product platform. These results were recently presented as a research article in the journal <link https: onlinelibrary.wiley.com doi abs anie.202004463>Angewandte Chemie International Edition.<link https: doi.org anie.202004463>
“The selectivity towards the different reduction levels is very sensitive towards changes in reaction conditions like the choice of reducing hydrosilane, solvent, temperature, and CO2 pressure,” explains Hanna H. Cramer, the Ph.D. student responsible for the experimental work at the department of <link>Molecular Catalysis. “Based on these insights, we combined the best conditions for each reduction level. This way, we could selectively obtain formates, acetals, and methoxides with one catalytic system.”
Future efforts will aim at transferring the concept of adaptive catalysis to other systems and reducing agents (i.e., hydrogen). Furthermore, the underlying mechanistic aspects responsible for the changes in selectivity are currently being investigated in cooperation with the group of Prof. Frank Neese as part of the the Joint Work Space with the Max-Planck-Institut für Kohlenforschung.
Original publication: Leitner, W., Werlé, C., Weyhermüller, T., Chatterjee, B., Cramer, Hanna H. Controlling the Product Platform of Carbon Dioxide Reduction: Adaptive Catalytic Hydrosilylation of CO2 Using a Molecular Cobalt (II) Triazine Complex. Angewandte Chemie International Edition. <link https: doi.org anie.202004463>DOI: 10.1002/anie.202004463