Computational Study on Heterogeneous Borrowing Hydrogen Amination Catalysts

• Applicant: Dr. Julien Engel
• Subject Area: Theoretical Chemistry: Molecules, Materials, Surfaces ; Solid State and Surface Chemistry, Material Synthesis
• Term: from 2018 to 2021
• Project identifier: Deutsche Forschungsgemeinschaft (DFG) - Project number 404962435

Amines are not only among the building blocks of all living organisms, but also have a wide range of applications in the chemical industry. Therefore, the development of efficient and sustainable methods for the synthesis of amines is of great importance. One such method is the heterogeneously catalysed amination of alcohols using the so-called “borrowing hydrogen” concept. These reactions are one-pot cascade reactions in which the alcohol is first oxidised to a carbonyl compound (aldehyde, ketone). Next, the carbonyl compound reacts in a condensation reaction with an amine or ammonia to form an imine which is subsequently reduced to the desired amine. In this research project, computational methods are used to find supported metal catalysts, which efficiently catalyse all steps of the amination process. To do so, the reactivity of supported metal nanoparticles of group X and XI as well as ruthenium on different support materials are investigated systematically. Using different computational models for the description of the catalytic system, trends for the activity depending on the specific metal, support material, as well as the size and shape of the metal particles are obtained. These results are then used to propose new and more efficient catalysts. Finally, their activity is validated experimentally.

• DFG Programme: Research Fellowships
• International Connection: United Kingdom
• Host: Dr. Alberto Roldan Martinez