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Functionalization of polyoxotungstates with organoarsonate co-ligandsenabling surface decoration was explored for the triangular clusterarchitectures of the composition[CoII9(H2O)6(OH)3(p-RC6H4AsVO3)2({\alpha}-PV2WVI15O56)3]25-({Co9(P2W15)3}, R =H or NH2), isolated as Na25[Co9(OH)3(H2O)6(C6H5AsO3)2(P2W15O56)3]86H2O (Na-1)and Na25[Co9(OH)3(H2O)6(H2NC6H4AsO3)2(P2W15O56)3]86H2O (Na-2). The axiallyoriented para-aminophenyl groups in 2 facilitate the formation ofself-assembled monolayers on gold surfaces, and thus provide a viable molecularplatform for charge transport studies of magnetically functionalizedpolyoxometalates. The title systems were isolated and characterized in thesolid state and in aqueous solutions, and on metal surfaces. Using conductingtip atomic force microscopy (C-AFM), the energies of {Co9(P2W15)3} frontiermolecular orbitals in the surface-bound state were found to directly correlatewith cyclic voltammetry data in aqueous solution.

Probing frontier orbital energies of (Co9(P2W15)3) polyoxometalate clusters at molecule-metal and molecule-water interfaces