It is a challenge to generate predictable, reproducible supramolecular architectures, especially in the relatively unexplored area of hydrogen-bonded coordination complexes.  We have recently become interested in clay mimics because of their rich diversity of chemical applications.  They are known to intercalate or absorb gases, small molecules and ions, and thus serve as materials capable of storage, chemical separations, and catalysis.  Further, clays, unlike zeolites, are anisotropic solids, so that 2-D (in addition to 3-D) functionality can be accessed.  Our approach to materials synthesis and design is based on Crystal Engineering, in which e.g. hydrogen bonds are used as directional forces for assembly.  Using flat organic acids (such as 3,5-pyrazoledicarboxylic acid, 3,5-pyridinedicarboxylic acid, oxamic acid) and amines, we can synthesize crystalline solids with bilayer, single layer, or pillared architectures (below) with a surprising amount of predictability and reproducibility.

        

Especially the pillared solids have potential for practical applications (vide supra).  Therefore, in order to create more thermally stable and potentially useful materials, we have extended organic Crystal Engineering design principles to inorganic/organic hybrid materials.  The synthesis and solid state structure of hydrogen-bonded coordination complexes, and methods of obtaining pillared layered structures, versus single-layer or bilayer architectures, will be discussed.  In addition, thermal and physico-mechanical properties of organic and inorganic clay mimic structures will be compared