Understanding the role of zinc dithiocarbamate complexes as single source precursors to ZnS nanomaterials

被引:18
|
作者
Islam, Husn-Ubayda [1 ,2 ]
Roffey, Anna [1 ]
Hollingsworth, Nathan [1 ]
Bras, Wim [2 ,3 ]
Sankar, Gopinathan [1 ]
De Leeuw, Nora H. H. [4 ]
Hogarth, Graeme [3 ]
机构
[1] UCL, Dept Chem, 20 Gordon St, London WC1H OAJ, England
[2] Netherlands Org Sci Res DUBBLE ESRF, F-38043 Grenoble, France
[3] Oak Ridge Natl Lab, Chem Sci Div, Oak Ridge, TN 37831 USA
[4] Cardiff Univ, Sch Chem, Main Bldg,Pk Pl, Cardiff CF10 3AT, Wales
来源
NANOSCALE ADVANCES | 2020年 / 2卷 / 02期
基金
英国工程与自然科学研究理事会;
关键词
CHEMICAL-VAPOR-DEPOSITION; SULFIDE THIN-FILMS; SOURCE MOLECULAR PRECURSORS; NATURAL-ABUNDANCE C-13; RAY CRYSTAL-STRUCTURES; N-15 CP/MAS NMR; THERMAL-DECOMPOSITION; METAL SULFIDES; QUANTUM DOTS; CORE/SHELL NANOPARTICLES;
D O I
10.1039/c9na00665f
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Zinc sulfide is an important wide-band gap semi-conductor and dithiocarbamate complexes [Zn(S2CNR2)(2)] find widespread use as single-source precursors for the controlled synthesis of ZnS nanoparticulate modifications. Decomposition of [Zn((S2CNBu2)-Bu-i)(2)] in oleylamine gives high aspect ratio wurtzite nanowires, the average length of which was increased upon addition of thiuram disulfide to the decomposition mixture. To provide further insight into the decomposition process, X-ray absorption spectroscopy (XAS) of [Zn(S2CNMe2)(2)] was performed in the solid-state, in non-coordinating xylene and in oleylamine. In the solid-state, dimeric [Zn(S2CNMe2)(2)](2) was characterised in accord with the single crystal X-ray structure, while in xylene this breaks down into tetrahedral monomers. In situ XAS in oleylamine (RNH2) shows that the coordination sphere is further modified, amine binding to give five-coordinate [Zn(S2CNMe2)(2)(RNH2)]. This species is stable to ca. 70 degrees C, above which amine dissociates and at ca. 90 degrees C decomposition occurs to generate ZnS. The relatively low temperature onset of nanoparticle formation is associated with amine-exchange leading to the in situ formation of [Zn(S2CNMe2)(S2CNHR)] which has a low temperature decomposition pathway. Combining these observations with the previous work of others allows us to propose a detailed mechanistic scheme for the overall process.
引用
收藏
页码:798 / 807
页数:10
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