Abstract
Solutions to two general limitations in the immobilization of molecular water oxidation catalysts (WOCs) on nanoparticle or photoelectrode surfaces have been investigated: (a) a straightforward electrostatic method to bind charged WOCs more effectively to these surfaces and (b) a method to increase the concentration of the semiconductor- and/or electrode-immobilized WOCs so they can be spectroscopically characterized in this form. Polyoxometalate (POM) WOCs, known to be fast, selective, and oxidatively stable under homogeneous conditions, and their high negative charges are a good test case to assess the viability of electrostatic surface immobilization. The POM WOCs, [RuIV4O5(OH)(H2O)4(γ-PW10O36)2]9– (Ru4P2) and [{RuIV4(OH)2(H2O)4}(γ-SiW10O34)2]10- (Ru4Si2), have been immobilized by silanization on TiO2 nanoparticles and nanoporous electrodes and have been found to retain catalytic water oxidation activity. In photoelectrochemical systems, increased current density of WOC-TiO2/FTO electrodes is consisten...
Published Version
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