Computation modeling as a tool for the exploration of complex multistep reaction cycles in homogeneous catalysis. Some selected examples in the framework of the use of hydrogen as a fuel of the future

摘要

Computational modeling methods play a prominent role in the field of homogeneous catalysis given that reaction cycles tend to be multistep complicated processes, where the active catalytic species or intermediates are challenging or impractical to study via experimental approaches. At the same time, as such processes are purely molecular, modeling is viable even if very often computationally costly. The possibility to equally well access stable experimentally observable catalytic intermediates and short-life inaccessible species, such as high energy intermediates and, especially, transition states allows exploring and unraveling complete reaction mechanisms. The quantum mechanical description of intricate catalytic cycles is discussed here for three homogeneous catalytic systems all focused on the use of hydrogen as a potential zero-emission energy carrier for the future.