“…Some hydrogen-bonded water molecules, such as water clusters (Ghosh et al, 2005;Dai et al, 2008), one-dimensional water chains (Sreenivasulu et al, 2004) and two-dimensional water layers (Janiak et al, 2002), have been found. However, infinite chains of hydrogen-bonded water molecules in biological molecules, especially in supramolecular compounds, are still rare (Wang et al, 2007;Mukherjee et al, 2004;Neogi et al, 2005). We report here the synthesis and characterization of a novel three-dimensional hydrogen-bonded framework of 2-[(1H-imidazol-1-yl)methyl]-1H-benzimidazole dihydrate (LÁ2H 2 O), (I), which contains infinite chains of hydrogenbonded water molecules.…”