Abstract Ditopic bis (acylhydrazone) ligands, derived from the reactions of carbohydrazides with 2-phenylpyrimidine-4, 6-dicarbaldehyde and designed for grid formation with octahedrally coordinating transition-metal ions, exhibit a varied coordination chemistry depending upon the degree of their deprotonation. The neutral acylhydrazones are relatively poor ligands and are seemingly involved in multiple, labile complexation ...