The first examples of reactivity at the backbone of a bidentate PN-ligand L1H relevant to N–H activation are described, leading to novel PdII and CuI amido complexes. Activation of the PN-ligand backbone led to selective dearomatization of the pyridyl ring structure. In the case of PdII, the intermediate could be efficiently stabilized using PMe3. Selective N–H bond cleavage of e.g. trifluorosulfonylamide resulted in facile formation of mononuclear metal–amido species 2 and 4, which have been crystallographically characterized. Hydrogen-bonding dimerization is observed in these solid state structures. The results obtained with these structurally versatile and reactive scaffolds likely open up new avenues in cooperative catalysis.
Dalton Transactions
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