Imidazolium units represent the main structural moths for the formation of
unconventional C-H ... Cl- hydrogen bonds which become the noncovalent forc
es driving the anion interactions exibited by dicationic [1(4)]imidazolioph
anes in the solid state, while C-H ... O hydrogen bonds with water play a c
rucial role in governing the conformation of the solid-state aggregates, as
well as in solution, wherein NMR studies also reveal the importance of hyd
rogen bonds in controlling the tendency to anion binding.