Abstract
The reaction of the intramolecular frustrated Lewis pair (FLP) tBu2PCH2BPh2 with the amine‐boranes NH3·BH3 and Me2NH·BH3 leads to the formation of the corresponding FLP‐H2 adducts as well as novel five‐membered heterocycles that result from capturing the in situ formed amino‐borane by a second equivalent of FLP. The sterically more demanding tBu2PCH2BMes2 does not form such a five‐membered heterocycle when reacted with Me2NH·BH3 and its H2 adduct liberates dihydrogen at elevated temperatures, promoting the metal‐free catalytic dehydrogenation of amine‐boranes.
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