Abstract
Catalytic hydrogenation of amides could be an excellent option for the green atom efficient formation of alcohols and amines. However, the low reactivity of amides has been a big drawback for this reaction. In the last decade, the emergence of bifunctional catalysts for hydrogenation reactions improved the conditions for amide hydrogenation and made them feasible on larger scales. Still, the reaction mechanisms remained underinvestigated. In the course of his PhD studies, the candidate has elucidated the reaction mechanisms and bottlenecks by computational simulations at a quantum scale. With that information, the candidate proposed new catalysts that avoided such bottlenecks. Later, experimental studies proved the increased performance of the predicted catalysts.
List of papers
Paper 1: The key role of the Hemiaminal Intermediate in the Iron-Catalyzed Deaminative Hydrogenation of Amides. Artús Suàrez, L.; Culakova, Z.; Balcells, D.; Bernskoetter, W. H.; Eisenstein O.; Goldberg, K. I.; Hazari, N.; Tilset, M.; Nova, A. ACS Catalysis, 2018, 8, 8751-8762. DOI: 10.1021/acscatal.8b02184. The article is not available in DUO due to publisher restrictions. The published version is available at: https://doi.org/10.1021/acscatal.8b02184 |
Paper II: Rational Selection of co-Catalysts for the Deaminative Hydrogenation of Amides. Artús Suàrez, L.; Jayarathne, U.; Balcells, D.; Bernskoetter, W. H.; Hazari, N.; Jaraiz M.; Nova A. Chemical Science, 2020, 11, 2225-2230. DOI: 10.1039/c9sc03812d. The article is included in the thesis. Also available at: https://doi.org/10.1039/c9sc03812d |
Paper III: Highly Selective Hydrogenation of Amides Catalyzed by a Molybdenum Pincer Complex: Scope and Mechanism. Leischner, T.; Artús Suàrez, L.; Spannenberg, A.; Junge, K.; Nova A.; Beller M. Chemical Science, 2019, 10, 10566-10576. DOI: 10.1039/c9sc03453f. The article is included in the thesis. Also available at: https://doi.org/10.1039/c9sc03453f |