Stabilization of a molecular water oxidation catalyst on a dye−sensitized photoanode by a pyridyl anchor

Yong Zhu, Degao Wang, Qing Huang, Jian Du, Licheng Sun, Fei Li () and Thomas J. Meyer ()
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Yong Zhu: Dalian University of Technology
Degao Wang: Chinese Academy of Sciences
Qing Huang: Chinese Academy of Sciences
Jian Du: Dalian University of Technology
Licheng Sun: Dalian University of Technology
Fei Li: Dalian University of Technology
Thomas J. Meyer: University of North Carolina at Chapel Hill

Nature Communications, 2020, vol. 11, issue 1, 1-8

Abstract: Abstract Understanding and controlling the properties of water-splitting assemblies in dye-sensitized photoelectrosynthesis cells is a key to the exploitation of their properties. We demonstrate here that, following surface loading of a [Ru(bpy)3]2+ (bpy = 2,2′-bipyridine) chromophore on nanoparticle electrodes, addition of the molecular catalysts, Ru(bda)(L)2 (bda = 2,2′-bipyridine-6,6′-dicarboxylate) with phosphonate or pyridyl sites for water oxidation, gives surfaces with a 5:1 chromophore to catalyst ratio. Addition of the surface-bound phosphonate derivatives with L = 4-pyridyl phosphonic acid or diethyl 3-(pyridin-4-yloxy)decyl-phosphonic acid, leads to well-defined surfaces but, following oxidation to Ru(III), they undergo facile, on-surface dimerization to give surface-bound, oxo-bridged dimers. The dimers have a diminished reactivity toward water oxidation compared to related monomers in solution. By contrast, immobilization of the Ru-bda catalyst on TiO2 with the 4,4′-dipyridyl anchoring ligand can maintain the monomeric structure of catalyst and gives relatively stable photoanodes with photocurrents that reach to 1.7 mA cm−2 with an optimized, applied bias photon-to-current efficiency of 1.5%.

Date: 2020
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DOI: 10.1038/s41467-020-18417-5

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