Our attempts to generate a palladium hydride with the formula [HPd(triphos)(PPh3)] + in H2 heterolysis equilibria using guanidine and phosphazene bases are described in equation We observed a similar reaction for the palladium complex with the tridentate PN H P ligand, (PN H P = HN[CH2CH2PPh2]2), shown in Scheme 2; when we attempted to deprotonate the ligand to prepare the neutral complex with an anionic PNP ligand, N(CH2CH2PPh2) -, as shown in equation (3), we instead observed the formation of the cyanomethyl complex [Pd(PN H P)(CH2CN)]Cl, 2, as shown in equation ( ), after washing the product with acetonitrile. 2 was crystallized from an acetonitrile solution upon vapor diffusion with diethyl ether. X-ray crystal structures of both 1 and 2 were determined, although the data quality obtained from the crystals of 2 was poor, and the crystal structure is sufficient primarily for the purposes of establishing the identity of the product and identifying a hydrogen-bonding interaction between the outer-sphere chloride and the N-H group of the ligand.