Crystal structure and Hirshfeld surface analysis of two iHOFs based on CH...NC hydrogen bonding.

Two ionic hydrogen‐bonded organic frameworks (iHOFs) assembled from 4‐cyano‐N‐(4‐cyanobenzyl)pyridinium, have been crystallized with Br− and antimony(III) pentabromide, [SbBr5]2−, as counter‐ions and characterized. These are 4‐cyano‐N‐(4‐cyanobenzyl)pyridinium bromide, C14H10N3+·Br−, and bis[4‐cyano‐N‐(4‐cyanobenzyl)pyridinium] antimony(III) pentabromide, (C14H10N3)2[SbBr5]. 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. [ABSTRACT FROM AUTHOR]