In situ formation of reactive sulfide precursors in the one-pot, multigram synthesis of Cu2ZnSnS4 nanocrystals

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dc.contributor.authorChesman, ASRen_AU
dc.contributor.authorvan Embden, Jen_AU
dc.contributor.authorDuffy, NWen_AU
dc.contributor.authorWebster, NASen_AU
dc.contributor.authorJasieniak, JJen_AU
dc.date.accessioned2015-09-28T06:58:03Zen_AU
dc.date.available2015-09-28T06:58:03Zen_AU
dc.date.issued2013-03-05en_AU
dc.date.statistics2015-09-16en_AU
dc.description.abstractHerein we outline a general one-pot method to produce large quantities of compositionally tunable, kesterite Cu2ZnSnS4 (CZTS) nanocrystals (NCs) through the decomposition of in situ generated metal sulfide precursors. This method uses air stable precursors and should be applicable to the synthesis of a range of metal sulfides. We examine the formation of the ligands, precursors, and particles in turn. Direct reaction of CS2 with the aliphatic primary amines and thiols that already constitute the reaction mixture is used to produce ligands in situ. Through the use of 1H and 13C nuclear magnetic resonance, Fourier transform infrared spectroscopy, and optical absorption spectroscopy, we elucidate the formation of the resulting oleyldithiocarbamate and dodecyltrithiocarbonate ligands. The decomposition of their corresponding metal complexes at temperatures of ∼100 °C yields nuclei with a size of 1–2 nm, with further growth facilitated by the decomposition of dodecanethiol. In this way the nucleation and growth stages of the reaction are decoupled, allowing for the generation of NCs at high concentrations. Using in situ X-ray diffraction, we monitor the evolution of our reactions, thus enabling a real-time glimpse into the formation of Cu2ZnSnS4 NCs. For completeness, the surface chemistry and the electronic structure of the resulting CZTS NCs are studied. © 2013, American Chemical Society.en_AU
dc.identifier.citationChesman, A. S. R., van Embden, J., Duffy, N. W., Webster, N. A. S., & Jasieniak, J. J. (2013). In situ formation of reactive sulfide precursors in the one-pot, multigram synthesis of Cu2ZnSnS4 nanocrystals. Crystal Growth & Design, 13(4), 1712-1720. doi:10.1021/cg4000268en_AU
dc.identifier.govdoc6079en_AU
dc.identifier.issn1528-7483en_AU
dc.identifier.issue4en_AU
dc.identifier.journaltitleCrystal Growth & Designen_AU
dc.identifier.pagination1712-1720en_AU
dc.identifier.urihttp://dx.doi.org/10.1021/cg4000268en_AU
dc.identifier.urihttp://apo.ansto.gov.au/dspace/handle/10238/6234en_AU
dc.identifier.volume13en_AU
dc.language.isoenen_AU
dc.publisherAmerican Chemical Societyen_AU
dc.subjectLigandsen_AU
dc.subjectPrecursoren_AU
dc.subjectX-ray diffractionen_AU
dc.subjectNuclear magnetic resonanceen_AU
dc.subjectEmission spectroscopyen_AU
dc.subjectSulfidesen_AU
dc.subjectMetalsen_AU
dc.titleIn situ formation of reactive sulfide precursors in the one-pot, multigram synthesis of Cu2ZnSnS4 nanocrystalsen_AU
dc.typeJournal Articleen_AU
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