Abstract

One‐dimensional anodic titanium oxide (ATO) nanotube arrays hold great potential as electrode materials for both dye‐sensitized solar cells (DSSCs) and electrochemical supercapacitors (SCs). In this work, a novel stack‐integrated photo‐supercapacitor (PSC) thin‐film device is presented, composed of a DSSC and a SC built on bi‐polar ATO nanotube arrays, where an improved SC performance is achieved through selective plasma‐assisted hydrogenation treatment. At a high current density of 1 mA/cm2 in charge/discharge measurements, the areal capacitance of selective hydrogenated ATO two‐electrode sub‐device is substantially increased ∼5.1 times, with the value as high as 1.100 mF/cm2. The optimized PSC exhibits a remarkable overall photoelectric conversion and storage efficiency up to 1.64%, with fast response and superior cycling capability for more than 100 photocharge/galvanostatic discharge cycles without any decay. To meet applicable demands with a larger output voltage, a tandem PSC system is constructed, serving as the self‐driven power source for an LED.

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