The burning of fossil fuels is causing a global climatic emergency. In order to solve this crisis, is very important to improve the efficiency of the production of renewable energies by transforming CO2 into carbon-based fuels. In this report, the member of the DIMOCAT Josep M. Luis in collaboration with the Julio Lloret group, determined the mechanism and bottlenecks of the CO2 reduction reaction with a model cobalt catalyst. The theoretical calculations, in combination with in situ measurements, pinpointed an elusive cobalt(I) carbonyl intermediate, which is formed very early in the reaction and is responsible for one of the most problematic bottlenecks in the CO2 reduction process. The mechanistic studies allowed the identification the bottlenecks of the reaction and the design of a photocatalytic strategy to break the carbonylic compounds and then strongly improve the efficient of the catalytic reduction of the CO2.
Sergio Fernández, Federico Franco, Carla Casadevall, Vlad Martin-Diaconescu, Josep M. Luis, Julio Lloret-Fillol.
“A Unified Electro- and Photocatalytic CO2 to CO Reduction Mechanism with Aminopyridine Cobalt Complexes”
J. Am. Chem. Soc. 2019, ASAP