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The crystal structures of six (pyrazinecarbonyl)hydrazone di-substituted benzaldehyde derivatives [N 2 C 4 H 3 CONHN = CHC 6 H 3 XY: X,Y = 2,3-Cl 2 ; 2,3-(MeO) 2 ; 2,4-F 2 ; 2,4-Me 2 ; 3-HO—4-MeO; 3-MeO—4-HO] and one tri-substituted benzaldehyde derivative, [N 2 C 4 H 3 CONHN = CHC 6 H 2 X 3 : X 3  = 3,4,5-(MeO) 3 ] are reported. In all cases extensive intermolecular C—H···X (X = O, N or π-ring) hydrogen-bonding is present in which the the oxygen atoms of OH and OMe substituents act as hydrogen-bond acceptors and C—H bonds of methyl groups act as hydrogen-bond donors. The connectivity attained is one-dimensional in chains or ribbons in the 2,3-(OMe) 2  and 2,4-Me 2  derivatives, three dimensional only in the case of the 3-MeO—4-HO derivative and two dimensional in layers of molecules otherwise. It is concluded, therefore, that the bulky nature of the substituents limits the connectivity attainable in this series of compounds.

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Structures of (pyrazinecarbonyl)hydrazones of substituted benzaldehydes: different supramolecular arrangements from C—H···X (X = O, N, π) hydrogen bonds