Add time:08/24/2019         Source:sciencedirect.com

Presented is a study on the mechanochemically assisted synthesis of kesterite Cu2ZnSnS4 from the elements for photovoltaic applications. Initial application of high energy ball milling under selected conditions, including the highest achievable rotation speeds up to 1000 rpm, affords a pure cubic nanophase with the nominal kesterite composition. The phase is tentatively called a pre-kesterite and it is shown by EPR to be magnetic. Accordingly, it does not produce either 65Cu or 119Sn MAS NMR spectra. Also, the material shows no well-defined absorption in the UV–vis range and, based on this, does not exhibit definite semiconducting properties. The highly disordered and defected structure with random metal site occupation originated in the mechanochemical synthesis step is proposed to account for the observed properties of pre-kesterite. Upon subsequent pyrolysis under argon at temperatures above 300 °C, preferably at around 500 °C, the cubic phase is converted to the tetragonal phase of kesterite, apparently, by metal site reconfiguration. The annealed nanopowders show the expected 65Cu and 119Sn MAS NMR characteristics. The Raman spectra support similar bonding environment and lattice phonon characteristics for both related phases as well as the eventual formation of kesterite nanopowders whereas their UV–vis spectra provide the direct band gap in the range of 1.35–1.48 eV, typical for semiconducting kesterite.

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