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SOLID-STATE SYNTHESIS OF LOW DIMENSIONAL LEAD FREE Mn BASED FLUORESCENT ORGANIC INORGANIC HYBRID COMPOUNDS

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Title
SOLID-STATE SYNTHESIS OF LOW DIMENSIONAL LEAD FREE Mn BASED FLUORESCENT ORGANIC INORGANIC HYBRID COMPOUNDS
Author
Zhumagali, Shynggys
Advisor
Kim, Kwang S.
Issue Date
2019-08
Publisher
Graduate School of UNIST
Abstract
We report the first solid-phase gram-scale syntheses of range of low-dimensional leadfree Mn-based fluorescent organic-inorganic hybrid compounds, with a general formula of [R4Y]MnX3 and [R4Y]2MnX4 (R = CH3, C2H5, C4H9, C6H5; Y = N, P; X = Cl, Br). This has been achieved by mechanochemical grinding of the organic tetraalkyl halide with manganese (II) halides in the absence of any liquid reaction media. Solid-phase synthetic route has several advantages, in particular, in the synthesis of hybrid compounds with different molecular dimensionalities. During the mechanochemical synthesis process, the organic R4Y+ and inorganic Mn2+ cations co-crystallized together with halide anions in solid state, forming low-dimensional molecular assembly, where each individual metal centers are suspended in the matrix of organic cations. Mainly, the mechanochemical synthesis was applied to prepare 0D-[Me4N]2MnCl4, 0D-[Bu4N]2MnBr4, 0D-[Ph4P]2MnCl4 with brilliant green fluorescence at 520 nm, and 1D- [Me4N]MnCl3 with bright orange fluorescence at 620 nm. Additionally, a range of similar compounds with varying organic substituents were prepared to show the scope of this methodology. The ground products exhibit emission phenomena upon exciting with both below and above band gap photons with high photoluminescence quantum yield (PL-QY), which is attributed to the individual tetrahedral manganese centers. These findings open a new path for development of highly fluorescent non-toxic hybrid compounds with remarkable photochemical properties.
Description
Department of Chemistry
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