The bis(diaminotriazinyl)-substituted derivatives of benzene,
pyridine, and pyrazine 1−6 were made to test the ability of the 4,6-diamino1,3,5-triazinyl group (DAT) to direct molecular organization by hydrogen bonding. Analysis of the structures of compounds 1−6 by X-ray crystallography revealed that the DAT groups control association by forming hydrogen bonds according to the well-established motifs I−III. The resulting association normally produces complex networks consisting of tapes, rings, and sheets. 1,2- Disubstituted compounds 1−3 have structures in which the DAT groups do not lie close to the plane of the aryl or heteroaryl core, whereas 1,3-disubstituted compounds 4−6 adopt flattened conformations. The observed structures of compounds 1−6, which include novel embraces and rings held together by hydrogen bonds, highlight the special ability of motifs based on DAT groups to
direct molecular association.