Mild conversion of the nitrile substituent into an amide functional group is observed upon coordination of CNTPA [CNTPA = (6-cyano 2-pyridylmethyl)bis(2-pyridylmethyle)amine] to FeCl2 followed by reaction with water. The crystal structure of CNTPAFeCl(2) is reported and reveals that the nitrile group does not coordinate but is activated in the vicinity of the ferrous center. Upon treatment with water under anaerobic conditions, CNTPAFeCl(2) converts into H(2)NCOTPAFeCl(2), [H(2)NCOTPA = (6-carboxamido 2-pyridylmethyl)bis(2-pyridylmethyle)amine], the X-ray crystal structure of which is reported. The new ligand H(2)NCOTPA can easily be obtained upon decomplexation.