WO_(3),an abundant transition metal semiconductor,is one of the most discussed materials to be used as a photoanode in photoelectrochemical water-splitting devices.The photoelectrochemical properties,such as photoacti...WO_(3),an abundant transition metal semiconductor,is one of the most discussed materials to be used as a photoanode in photoelectrochemical water-splitting devices.The photoelectrochemical properties,such as photoactivity and selectivity of WO_(3) in different electrolytes,are already well understood.However,the understanding of stability,one of the most important properties for utilization in a commercial device,is still in the early stages.In this work,a photoelectrochemical scanning flow cell coupled to an inductively coupled plasma mass spectrometer is applied to determine the influence of co-catalyst overlayers on photoanode stability.Spray-coatedWO_(3) photoanodes are used as a model system.Iridium is applied to the electrodes by atomic layer deposition in controlled layer thickness,as determined by ellipsometry and x-ray photoelectron spectroscopy.Photoactivity of the iridium-modified WO_(3) photoanodes decreases with increasing iridium layer thickness.Partial blocking of the WO_(3) surface by iridium is proposed as the main cause of the decreased photoelectrochemical performance.On the other hand,the stability of WO_(3) is notably increased even in the presence of the thinnest investigated iridium overlayer.Based on our findings,we provide a set of strategies to synthesize nanocomposite photoelectrodes simultaneously possessing high photoelectrochemical activity and photostability.展开更多
基金German Ministry of Education and Reseach(BMBF),Grant/Award Number:03SF0564ADeutsche Forschungsgemeinschaft(DFG),Grant/Award Number:429730598。
文摘WO_(3),an abundant transition metal semiconductor,is one of the most discussed materials to be used as a photoanode in photoelectrochemical water-splitting devices.The photoelectrochemical properties,such as photoactivity and selectivity of WO_(3) in different electrolytes,are already well understood.However,the understanding of stability,one of the most important properties for utilization in a commercial device,is still in the early stages.In this work,a photoelectrochemical scanning flow cell coupled to an inductively coupled plasma mass spectrometer is applied to determine the influence of co-catalyst overlayers on photoanode stability.Spray-coatedWO_(3) photoanodes are used as a model system.Iridium is applied to the electrodes by atomic layer deposition in controlled layer thickness,as determined by ellipsometry and x-ray photoelectron spectroscopy.Photoactivity of the iridium-modified WO_(3) photoanodes decreases with increasing iridium layer thickness.Partial blocking of the WO_(3) surface by iridium is proposed as the main cause of the decreased photoelectrochemical performance.On the other hand,the stability of WO_(3) is notably increased even in the presence of the thinnest investigated iridium overlayer.Based on our findings,we provide a set of strategies to synthesize nanocomposite photoelectrodes simultaneously possessing high photoelectrochemical activity and photostability.