In this work, by using two kinds of viologen ligands three POM-based compounds were obtained under hydrothermal and solvothermal conditions, namely {Cu2(Cbybpy)6(Cl)2[H4(β-Mo8O26)3]}·12H2O (1), (HCbybpy)2·(β-Mo8O26) (2) (Cbybpy·Br = 1-(2'-Cyano-biphenyl-4-ylmethyl)-[4,4']bipyridinyl-1-ium bromide) and...