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Transparent Fe1-xNixOOH overlayers (~2 nm thick) were depositedphotoelectrochemically on (001) oriented heteroepitaxial Sn- and Zn-dopedhematite (Fe2O3) thin film photoanodes. In both cases, the waterphoto-oxidation performance was improved by the co-catalyst overlayers.Intensity modulated photocurrent spectroscopy (IMPS) was applied to study thechanges in the hole current and recombination current induced by theoverlayers. For the Sn-doped hematite photoanode, the improvement inperformance after deposition of the Fe1-xNixOOH overlayer was entirely due toreduction in the recombination current, leading to a cathodic shift in theonset potential. For the Zn-doped hematite photoanode, in addition to areduction in recombination current, an increase in the hole current to thesurface was also observed after the overlayer deposition, leading to a cathodicshift in the onset potential as well as an enhancement in the plateauphotocurrent. These results demonstrate that Fe1-xNixOOH co-catalysts can playdifferent roles depending on the underlying hematite photoanode. The effect ofthe co-catalyst is not always limited to changes in the surface properties, butalso to an increase in hole current from the bulk to the surface that indicatesa possible crosslink between surface and bulk processes.

Different roles of Fe1-xNixOOH co-catalyst on hematite ({\alpha}-Fe2O3) photoanodes with different dopants