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The Ni‐B complex 1BCF with a facilely accessible monophosphine (PtBu3) unit was theoretically designed, which was found to be more active than that with an ambiphilic ligand for hydrogenation of styrene. Substituting PtBu3 with a stronger electron donating ligand N‐heterocyclic carbene largely improves the activity of the Ni‐B complex.
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