Journal of the American Chemical Society p. 5543 - 5549 (1980)
Update date:2022-08-25
Topics:
Ghosh, Pushpito K.
Spiro, Thomas G.
Ru(bpy)32+ (bpy = 2,2'-bipyridyl) has been covalently attached to n-type SnO2 via condensation of surface hydroxyl groups with ruthenium (4-(trichlorosilylethyl)-4'-methyl-2,2'-bipyridine)bis(2,2'-bipyridine) bis(hexafluorophosphate)).A thick coating (ca. 1000 layers, based on the surface hydroxyl group concentration) was produced, presumably via oligomerization of hydrolyzed -SiCl3 groups.The coating, which was stable to organic solvents as well as to aqueous acids and bases, gave reversible cyclic voltammograms, with peak potentials shifted slightly from those of aqueous Ru(bpy)32+, but the number of electroactive molecules corresponding only to a few layers.The coated electrode gave a photocurrent about twice that observed for SnO2 in contact with aqueous 4mM Ru(bpy)32+, with a slightly red-shifted excitation spectrum.Only a small fraction of the electroactive molecules appeared to participate in excited-state electron transfer, although a steady-state current was supported, presumably by slow electron transfer from the outer layers.Prolonged illumination produces extensive hydrolysis of the outer layers of the coating, but a modest reduction of electroactivity, and only a slight decrease in photocurrent.The photocurrent increases with applied potential, then reaches a plateau, and falls off again near the reduction potential of Ru(bpy)32+*; the falloff is attributed to back-electron transfer via tunnelling through the thin space charge layer.
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