Electrochemical Oxidation of Water by an Adsorbed μ-Oxo-Bridged Ru Complex
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Abstract
The μ-oxo-bridged complex, [((OH)2OP-tpy)(H2O)2RuORu(OH2)2(tpy-PO(OH)2)]4+ (tpy-PO(OH)2 is 4‘-phosphonato-2,2‘:6‘,2‘ ‘-terpyridine), was prepared and attached to ITO (Sn(IV)-doped In2O3) and nanocrystalline 10−20 nm diameter TiO2, ZrO2, and SnO2 thin film (∼10 μm thickness) electrodes. The complex retains its proton-coupled electron transfer (PCET) and water oxidation properties on oxide surfaces. The electrochemically generated RuVI−O−RuV and RuV−O−RuV forms of the complex oxidize water with turnover numbers of 3.0 and 2.6 for RuVI−O−RuV and 1.8 and 1.0 for RuV−O−RuV at pH = 1 (triflic acid) and pH = 6 (terephthalic acid buffer), respectively. Cyclic voltammetric and spectroelectrochemical measurements have given significant insight into the water oxidation mechanism and origins of catalyst deactivation.
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