Water Oxidation at Hematite Photoelectrodes （水在赤铁矿光电极氧化）.pdfVIP

Article /JPCC Water Oxidation at Hematite Photoelectrodes with an Iridium-Based Catalyst Laura Badia-Bou,† Elena Mas-Marza,‡ Pau Rodenas,† Eva M. Barea,† Francisco Fabregat-Santiago,† Sixto Gimenez,*,† Eduardo Peris,*,‡ and Juan Bisquert*,† †Photovoltaics and Optoelectronic Devices Group, Departament de Física, and ‡Departament de Química Inorganica Organica,̀ ̀ Universitat Jaume I, 12071 Castello, Spaiń S *Supporting Information ABSTRACT: The iridium complex [Cp*Ir(H O) ](SO ) was used as an organometallic source for the electrodeposition of 2 3 4 iridium oxide onto Fe O . The new iridium-containing electrode allowed us to study the coupling between the photocatalytic 2 3 properties of hematite and the electrocatalytic properties of the iridium-based material. A cathodic shift of the photocurrent for water oxidation upon electrodeposition of the iridium complex was observed, which increased with increasing surface concentration of IrO on Fe O . The shift for the highest surface concentration of iridium tested amounts to 300 mV at 200 x 2 3 μA ·cm−2 current density. The catalytic mechanism of the IrOx layer was unveiled by impedance spectroscopy measurements fitted to a physical model and can be explained on the basis of a highly capacitive layer, which enhances charge separation and stores photogenerated holes at Fe O , subsequently oxidizing water. These findings