Investigation of single phase C u2ZnS nx S b1-x S4 compounds processed by mechanochemical synthesis

The copper zinc tin sulfide (CZTS) compound is a promising candidate as an alternative absorber material for thin-film solar cells. In this study, we investigate the direct formation of Cu1.92ZnSnx(Sb1-x)S4 compounds [CZT(A)S], with x=1, 0.85, 0.70, and 0.50, via a mechanochemical synthesis (MCS) approach, starting from powders of the corresponding metals, zinc sulfide, and sulfur. The thermal stability of the CZT(A)S compounds was evaluated in detail by in situ synchrotron high-energy x-ray diffraction measurements up to 700 °C. The CZT(A)S compounds prepared via MCS revealed a sphalerite-type crystal structure with strong structural stability over the studied temperature range. The contribution of the MCS to the formation of such a structure at room temperature is analyzed in detail. Additionally, this study provides insights into the MCS of CZTS-based compounds: the possibility of a large-scale substitution of Sn by Sb and the production of single phase CZT(A)S with a Cu-poor/Zn-poor composition. A slight increase in the band gap from 1.45 to 1.49-1.51 eV was observed with the incorporation of Sb, indicating that these novel compounds can be further explored for thin-film solar cells.