Advanced computation of enthalpies for a range of hydroformylation reactions with a predictive power to match experiments

Papp, Tamara and Nagy, Péter R. and Kégl, Tamás (2024) Advanced computation of enthalpies for a range of hydroformylation reactions with a predictive power to match experiments. CHEMICAL PHYSICS LETTERS, 861. No. 141833. ISSN 0009-2614

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Abstract

While hydroformylation is a central homogeneous catalytic industrial processes, we find a relatively large (17 kcal/mol) scatter of DFT reaction enthalpies with a range of widely-employed DFT methods, unexpected in organic chemistry. Thus, we obtained gold standard hydroformylation enthalpies for a large variety of substrates exploiting the local natural orbital method. The corresponding hydroformylation enthalpies of ethylene and propylene agree with the experiments within a few tenth of a kcal/mol. This predictive power enabled the study of nuanced trends in the hydroformylation for a wide range of aliphatic and aromatic substrates as a function of chain elongation, branching, and substituent effects.

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