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Mononuclear iridium(III) complexes, NBu 4 [IrBr 4 (bpym)] ( 1 ) and [IrBr 3 (bpym)(MeCN)] ( 2a  and  2b ) [NBu 4+  = tetra( n -butyl)ammonium cation; bpym = 2,2'-bipyrimidine], have been prepared and characterized. Their crystal structures were determined by single-crystal X-ray diffraction.  1  and  2a  crystallize in the monoclinic crystal system with space groups  P 2 1 /c and  P 2 1 /n, respectively. The  2b  phase crystallizes in the orthorhombic crystal system with space group  P 2 1 2 1 2 1 . In these complexes, each iridium(III) is six-coordinate and bonded to two ( 1 ) or three ( 2a  and  2b ) nitrogen atoms from bpym and MeCN ( 2a  and  2b ) molecules and three ( 2a  and  2b ) or four ( 1 ) bromides. In all the cases, they exhibit a distorted octahedral environment.  2a  and  2b  display a packing polymorphism containing π···Br, C–H···Br and Br···Br intermolecular interactions. Further analyses of their crystal structures were performed through the SHAPE and CrystalExplorer programs. The electrochemical properties of  1  and  2  were investigated through cyclic voltammetry (CV) technique, with  1  showing a reversible iridium(III)–iridium(IV) redox process.

Crystal polymorphism in 2,2'-bipyrimidine-based iridium(III) complexes