Abstract

Two ionic hydrogen-bonded organic frameworks (iHOFs) assembled from 4-cyano- N -(4-cyanobenzyl)pyridinium, have been crystallized with Br − and antimony(III) pentabromide, [SbBr 5 ] 2− , as counter-ions and characterized. These are 4-cyano- N -(4-cyanobenzyl)pyridinium bromide, C 14 H 10 N 3 + ·Br − , and bis[4-cyano- N -(4-cyanobenzyl)pyridinium] antimony(III) pentabromide, (C 14 H 10 N 3 ) 2 [SbBr 5 ]. The CH...NC interactions induced by templating anions construct disparate frameworks. Hirshfeld surface analysis indicated that these crystals exhibit two types of hydrogen-bonding interactions, specifically CH...NC and CH...Br. Consecutive reverse-parallel CH...NC hydrogen-bonding interactions in these crystals induced the formation of a large number of CH...NC bonds which exhibit both cis and trans configurations.