Abstract: | Two new compounds, (H2en)3(H2enMe)4(H3O){CuI[MoV 6O12(OH)3(HPO4)(PO4)3]2}?·?6H2O (1) and (H2enMe)4{CuICuII[MoV 6O12(OH)3(PO4)(HPO4)2(H2PO4)]2}?·?3H2O (2), were hydrothermally synthesized and characterized by elemental analysis, IR, TGA, and single-crystal X-ray diffraction analysis. Crystallographic analysis reveals that 1 is constructed from cluster anions {CuI[MoV 6O12(OH)3(HPO4)(PO4)3]2}15?, protonated organic amines, and water molecules. Each cluster is bridged through hydrogen bonds to form a 3-D supermolecular structure. For 2, {CuI[MoV 6O12(OH)3(PO4)(HPO4)2(H2PO4)]2}11? are connected by CuII cations to form an infinite chain. The formation of 1 and 2 reveals that organoamines influence the structures of the crystals. |