期刊
ACS APPLIED MATERIALS & INTERFACES
卷 6, 期 11, 页码 8022-8031出版社
AMER CHEMICAL SOC
DOI: 10.1021/am405295c
关键词
polyoxometalates; immobilization; conducting polymer; water oxidation; multilayer assembly; electrocatalysis
资金
- Irish Government's Programme for Research in Third Level Institutions, Cycle 4, National Development Plan
- EU-COST Action [CM1203]
A tetra Ru-substituted polyoxometalate Na-10[{Ru4O4(OH)(2)(H2O)(4)}(gamma-SiW10O36)(2)] (Ru4POM) has been successfully immobilised onto glassy carbon electrodes and indium tin oxide (ITO) coated glass slides through the employment of a conducting polypyrrole matrix and the layer-by-layer (LBL) technique. The resulting Ru4POM doped polypyrrole films showed stable redox behavior associated with the Ru centres within the Ru4POM, whereas, the POM's tungsten-oxo redox centres were not accessible. The films showed pH dependent redox behavior within the pH range 2-5 whilst exhibiting excellent stability towards redox cycling. The layer-by-layer assembly was constructed onto poly(diallyldimethylammonium chloride) (PDDA) modified carbon electrodes by alternate depositions of Ru4POM and a Ru(II) metallodendrimer. The resulting Ru4POM assemblies showed stable redox behavior for the redox processes associated with Ru4POM in the pH range 2-5. The charge transfer resistance of the LBL films was calculated through AC-Impedance. Surface characterization of both the polymer and LBL Ru4POM films was carried out using atomic force microscopy (AFM), X-ray photoelectron spectroscopy (XPS), and scanning electron microscopy (SEM). Initial investigations into the ability of the Ru4POM LBL films to electrocatalytically oxidise water at pH 7 have also been conducted.
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