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The Lewis acidities of a series of [ n ]magnesocenophanes ( 1 a – d ) have been investigated computationally and found to be a function of the tilt of the cyclopentadienyl moieties. Their catalytic abilities in amine borane dehydrogenation/dehydrocoupling reactions have been probed, and C[1]magnesocenophane ( 1 a ) has been shown to effectively catalyze the dehydrogenation/dehydrocoupling of dimethylamine borane ( 2 a ) and diisopropylamine borane ( 2 b ) under ambient conditions. Furthermore, the mechanism of the reaction with  2 a  has been investigated experimentally and computationally, and the results imply a ligand‐assisted mechanism involving stepwise proton and hydride transfer, with dimethylaminoborane as the key intermediate.

Magnesocenophane‐Catalyzed Amine Borane Dehydrocoupling