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Activation and cleavage of molecular hydrogen (H2) to proton and hydride is an important task for several reasons, especially as a reagent in hydrogenation. In this scenario, with the support of density‐functional theory methods, a novel strategy has been devised for the conversion of coordinated nitride into ammonia using molecular hydrogen in the presence of tri‐tert‐butylphosphine (PtBu3). The...