A series of oligothiophene dinitriles, containing one, two, or three oligothiophene rings between nitrile donors NC-(C 4 H 2 S) n -CN are reacted with silver(I) salts to form coordination compounds. In most cases, the resulting metal−organic frameworks are one-dimensional coordination polymers containing roughly linear divalent Ag(I) centers. However, in the case of bithiophene (n = 2) and terthiophene (n = 3) bridges, a three-dimensional structure is also possible if the silver(I) counterion is just the right size to fit into the diamondoid pores that form with four-coordinate tetrahedrally oriented Ag(I) centers. Thus, only ClO 4 − and BF 4 − form three-dimensional structures with the bithiophenebridged ligands, while the larger CF 3 SO 3 − and SbF 6 − anions will support a threedimensional structure for the terthiophene-bridged ligand. Any counterion larger or smaller than the "just right" size will result in the one-dimensional structure instead.
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