Rational Design of Molecular Sheets Composed of Interconnecting Eight- and Twenty-Four-Membered Rings: Use of Lithiated Aggregates To Control Network Assembly

The lithiated (organo)sulfonylacetonitrile complex [MeSO2CHCNLi THF] (3) has been prepared and structurally characterized in order to demonstrate that well-known molecular aggregates of s-block metals may be used as building blocks in the controlled assembly of complex supramolecular architectures. The solid state structure of 3 can be described as a novel basket-weaved, 2-D network, composed of (SO2Li)2 "dimeric" rings joined via "interdimer" donation of nitrile units.