Proceedings of MATSUS23 & Sustainable Technology Forum València (STECH23) (MATSUS23)
DOI: https://doi.org/10.29363/nanoge.matsus.2023.032
Publication date: 22nd December 2022
Hydrogenation reactions are fundamental functional group transformations in chemical synthesis. Initially, research on hydrogenation reactions focused on the use of noble metal complexes based on Ru, Rh, Ir, Pd, Pt and remarkable achievements have been made using such complexes. However, recently the focus shifted towards the use of base metal catalysts, as these metals exhibit a higher availability in earth’s crust.[1] In the first instance, the direct reduction of C=O bonds with H2 seems to be a very atom and redox economic approach. However, the reaction protocols for base-metal catalyzed hydrogenation reactions require often harsh reaction conditions and high H2 pressure to activate H2 and each ton of H2 that is formed via steam reforming produces about 12 tons of CO2.[2]
I will present an electrochemical approach utilizing electrons and protons for the catalytic hydrogenation of polar double bonds, such as C=O in CO2, ketones, and aldehydes.[3] In a proof of principle study we demonstrated that in-situ generated Mn hydride species hydrogenate CO2 forming formic acid. This protocol was later expanded to aromatic, and aliphatic ketones as well as aldehydes. The method is selective for C=O bonds over the thermodynamically favored hydrogenation of C=C bonds. The competing hydrogen evolution reaction was suppressed successfully, and the reactions proceed with high Faraday efficiencies. A large variety of substrates was accessible by this method and in-depth mechanistic studies gave valuable insights for catalyst improvement.
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