Light-Driven Water Splitting with a Molecular Electroassembly-Based Core/Shell Photoanode

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• 作者：Benjamin D. Sherman ; Dennis L. Ashford ; Alexander M. Lapides ; Matthew V. Sheridan ; Kyung-Ryang Wee ; Thomas J. Meyer
• 刊名：The Journal of Physical Chemistry Letters
• 出版年：2015
• 出版时间：August 20, 2015
• 年：2015
• 卷：6
• 期：16
• 页码：3213-3217
• 全文大小：310K
• ISSN：1948-7185

文摘

An electrochemical procedure for preparing chromophore-catalyst assemblies on oxide electrode surfaces by reductive vinyl coupling is described. On core/shell SnO₂/TiO₂ nanoparticle oxide films, excitation of the assembly with 1 sun (100 mW cm^鈥?) illumination in 0.1 M H₂PO₄^{鈥?/sup>/HPO₄2鈥?/sup> at pH 7 with an applied bias of 0.4 V versus SCE leads to water splitting in a DSPEC with a Pt cathode. Over a 5 min photolysis period, the core/shell photoanode produced O₂ with a faradaic efficiency of 22%. Instability of the surface bound chromophore in its oxidized state in the phosphate buffer leads to a gradual decrease in photocurrent and to the relatively modest faradaic efficiencies.}