A joint experimental/computational effort to elucidate the mechanism of dihydrogen activation by a gold(I)/platinum(0) metal-only frustrated Lewis pairs is described herein. We have also investigated the drastic effects on H2 activation derived from subtle ligand modifications. The importance of the balance between bimetallic adduct formation and complete frustration has been interrogated, providing for the first time evidence for genuine metal-only FLP reactivity in solution. The origin of a strong inverse kinetic isotopic effect has also been clarified, offering further support for the proposed bimetallic FLP-type cleavage of dihydrogen.

https://doi.org/10.1002/chem.201905793

Nereida Hidalgo