Enhancing dye-sensitized solar cell performance: Optimizing Cu2ZnSnS4/ZnCo2O4 nanocomposites as efficient and cost-effective counter electrodes

Abstract

This study investigates the utilization of Cu2ZnSnS4/ZnCo2O4 (CZTS/ZCO) nanocomposites prepared through hydrothermal and combustion methods as counter electrodes in Dye-Sensitized Solar Cells (DSSCs). Different ratios of Cu2ZnSnS4 and ZnCo2O4 were explored, and comprehensive analyses were conducted using X-ray Diffraction (XRD), Transmission Electron Microscopy (TEM), High-Resolution TEM (HRTEM), Brunauer–Emmett–Teller (BET) surface area analysis, Raman Spectroscopy, Electrochemical Impedance Spectroscopy (EIS), cyclic voltammetry (CV), Tafel analysis, Field Emission Scanning Electron Microscopy (FESEM), and Incident Photon-to-Electron Conversion Efficiency (IPCE), alongside long-term stability assessments. The CZTS:ZCO ratio of 2:1 exhibited the highest efficiency, reaching 8.81 %, with an open-circuit voltage of 729 mV, short-circuit current of 17.80 mAcm−2, and a fill factor of 67.9 %. This surpasses the efficiency of the reference Pt cell (8.42 %), which had an open-circuit voltage of 735 mV, short-circuit current of 17.16 mAcm−2, and a fill factor of 66.8 %. The average crystallite sizes for the main peaks of CZTS and ZCO samples were estimated to be 19.8 and 16.7 nm, respectively. The crystallite size can significantly affect the charge transfer and conductivity in the counter electrode during electrochemical processes; the presence of nanocrystals with these sizes can notably enhance the electrochemical properties and conductivity of the synthesized samples. Raman analysis results indicate that no additional phases or secondary phases such as ZnS and CuSnS3 have formed in the kesterite CZTS structure, and the crystal has formed as a single phase. Additionally, the F2g modes in the Raman spectrum of ZCO indicate tetrahedral units in the spinel ZCO structure, and the A1g modes represent octahedral structures in this phase, indicating the formation of suitable ZCO phase. The superior performance of the CZTS/ZCO nanocomposite can be attributed to its enhanced crystalline structure, superior charge transport characteristics, and improved electrocatalytic behaviours.