ZnSxSe1-x Alloy Passivation Layer for High-Efficiency Quantum-Dot-Sensitized Solar Cells.

Abstract

Interface modification is an important means for improving the performance of almost all optoelectronic devices. In quantum-dot-sensitized solar cells (QDSCs), effective surface modification of photoanode also has a critical impact on photovoltaic performance. At present, ZnS and ZnSe wide band gap semiconductors are the mainstream materials used for photoanode/electrolyte interface passivation in QDSCs. However, the problem with these two materials is that the passivation effect and the lattice match with TiO2/QD are difficult to be balanced. Although ZnS can form a larger energetic barrier due to the higher conduction band edge, its lattice mismatch with TiO2 and QD (such as CdSe and CuInSe2) is large, leading to the formation of additional defect states. On the contrary, ZnSe has a small lattice mismatch with TiO2 and QD but a relatively lower conduction band edge. Herein, we propose a strategy to employ ZnSxSe1-x alloy materials as a passivation layer for the first time to solve the drawbacks of single-component passivation layers. The ZnSxSe1-x alloy passivation layer was deposited on the Zn-Cu-In-Se (ZCISe) QD-sensitized TiO2 film electrode via successive ionic layer adsorption and reaction (SILAR) method. A stable polyselenosulfide/sulfide mixed anions were served as anion precursor for the formation of ZnSxSe1-x alloy passivation layer. Experimental results revealed that the alloy passivation layer is more favorable for the suppression of charge recombination at the photoanode/electrolyte interface. In addition, the ZnSxSe1-x alloy passivation layer can significantly improve the photogenerated electron extraction efficiency compared to the current classical ZnS passivation layer as confirmed by the transient absorption (TA) measurement. Consequently, the average efficiency of QDSCs was improved from 12.17 to 13.08% with the replacement of traditional ZnS passivation layer by ZnSSe-10 under AM 1.5G one full sun illumination.