A Cu(2)S-CuInS(2)-ZnSe quantum dot (QD)-sensitized solar cell with cascaded energy gap structures has been fabricated. Under simulated illumination (AM 1.5, 100 mW cm(-2)), the best device is obtained with a Cu(2)S-CuInS(2)-ZnSe QD-sensitized solar cell, yielding a power conversion efficiency of 2.52%.

A simple one-pot approach was developed to obtain nonstoichiometric CuInS2 nanocrystals. Using this approach, both In-rich and Cu-rich CuInS2 nanocrystals could be reliably synthesized by tuning stoichiometric combinations of [Cu]/[In] precursor constituents. By designing Cu-rich CuInS2 heteronanostructures to serve as counter electrodes, quantum-dot-sensitized solar cells (QDSSCs) equipped with In-rich CuInS2 and CdS cosensitizers delivered a power conversion efficiency of 2.37%, which is significantly more efficient than conventional Pt counter electrodes. To the best of our knowledge, this study represents the first report utilizing nonstoichiometric CuInS2 nanocrystals as a photon-harvesting sensitizer comprised of a photoanode and photocathode in QDSSCs; also unique to this report, these nonstoichiometric CuInS2 nanocrystals were formed by simply changing the cationic molar ratios without complicated precursor preparation. Impedance spectroscopy and Tafel polarization indicated that these Cu-rich CuInS2 heteronanostructures had electrocatalytic activities (used for reducing S(2-)/Sn(2-)) that were superior to a Pt catalyst. Moreover, we demonstrated that Cu-rich CuInS2 heteronanostructures were also useful counter electrodes in dye-sensitized solar cells, and this finding revealed a promising conversion efficiency of 6.11%, which was ∼96% of the efficiency in a cell with a Pt-based counter electrode (6.32%).

This paper reports a facile and environmentally friendly approach to the preparation of highly efficient quantum dot-sensitized solar cells (QDSSCs) based on a combination of aqueous CuInS2 quantum dots (QDs) and thiol coadsorbents. The photovoltaic properties of the QDSSCs were found to be dependent on the type and concentration of the thiol coadsorbent. The incorporation of thiol coadsorbents results in improved JSC and VOC because (1) they provide disulfide reductants during the QD sensitization process and (2) the coadsorbent molecules are anchored on the TiO2 surface, thus affecting the movement of the conduction band of TiO2. To the best of the our knowledge, this is the first demonstrated use of various thiol coadsorbents as reducing agents in the fabrication of high-efficiency QDSSCs. CuInS2 QDSSCs fabricated with the assistance of thioglycolic acid coadsorbents exhibited efficiencies as high as 5.90%, which is 20 times higher than that of the control device without thiol coadsorbents (0.29%). In addition, the photovoltaic properties of a device fabricated using the colloidal CuInS2 QDs coated with different bifunctional linkers were investigated for comparison. The versatility of this facile fabrication process was demonstrated in the preparation of solar cells sensitized with aqueous AgInS2 or CdSeTe QDs. The AgInS2 QDSSC showed a conversion efficiency of 2.72%, which is the highest reported for Ag-based metal sulfides QDSSCs thus far.