Abstract
A new approach is described that overcomes the problems of photocorrosion and slow heterogeneous electron-transfer kinetics associated with light-assisted water oxidation at semiconductor electrodes. The photoanode, n-MoS{sub 2}, was immersed in an immiscible organic phase, nitromethane, or 1,2-dichloroethane, which insulated it from the aqueous catholyte. Tetrabutylammonium chloride provided ion environment that stabilized n-MoS{sub 2} in the unavoidably water-saturated nitromethane (or dichloroethane) phase. Chemical water oxidation by photoelectrogenerated Cl{sub 2} proceeded through a hypochlorite intermediate that was broken down with the help of RuO{sub 2} colloid catalysts, releasing O{sub 2}, H{sup +}, and Cl{sup {minus}}. Significant reduction of oxygen overvoltage was attained, corresponding to a photoanodic efficiency of 3%. Combined with efficient photocathodes developed in recent years, this could provide prospective foundations for hydrogen fuel generation by photoelectrochemical solar energy conversion.
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