The Computational Road to Better Catalysts

Computational studies, especially those using Density Functional Theory (DFT), have become pervasive in the characterisation, mechanistic study and optimisation of homogeneous organometallic catalysts and the “rational” design of such catalysts seems within reach once more. But how advanced, user-friendly and reliable are the computational tools currently available?
Here we summarise the current state of the art for predictive computational organometallic chemistry in reference to the different stages of catalyst development, considering characterisation, mechanistic studies, fine-tuning/optimisation and evaluation of novel designs. We also assess critically where the strengths and weaknesses of computational studies lie and hence map the road ahead for the design and discovery of novel catalysts in silico and in combination with targeted experimental studies.