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Molecules versus Nanoparticles: Identifying a Reactive Molecular Intermediate in the Synthesis of Ternary Coinage Metal Chalcogenides

Abstract : The identification of reactive intermediates during molecule-to-nanoparticle (NP) transformation has great significance in comprehending the mechanism of NP formation and, therefore, optimizing the synthetic conditions and properties of the formed products. We report here the room temperature (RT) synthesis of AgCuSe NPs from the reaction of di-tert-butyl selenide with trifluoroacetates (TFA) of silver(I) and copper(II). The isolation and characterization of a molecular species during the course of this reaction, [Ag2Cu(TFA)4(tBu2Se)4] (1), which shows extraordinary reactivity and interesting thermochromic behavior (blue at 0 °C and green at RT), confirmed that ternary metal selenide NPs are formed via this intermediate species. Similar reactions with related dialkyl chalcogenide R2E resulted in the isolation of molecular species of similar composition, [Ag2Cu(TFA)4(R2E)4] [R = tBu, E = S (2); R = Me, E = Se (3); R = Me, E = S (4)], which are stable at RT but can be converted to ternary metal chalcogenides at elevated temperature. Density functional theory calculations confirm the kinetic instability of 1 and throw light on its thermochromic properties.
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https://hal.archives-ouvertes.fr/hal-02869528
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Submitted on : Friday, November 6, 2020 - 7:53:51 AM
Last modification on : Thursday, January 6, 2022 - 6:38:02 PM
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Sweta Gahlot, Erwann Jeanneau, Deobrat Singh, Pritam Kumar Panda, Yogendra Kumar Mishra, et al.. Molecules versus Nanoparticles: Identifying a Reactive Molecular Intermediate in the Synthesis of Ternary Coinage Metal Chalcogenides. Inorganic Chemistry, American Chemical Society, 2020, 59 (11), pp.7727-7738. ⟨10.1021/acs.inorgchem.0c00758⟩. ⟨hal-02869528⟩

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