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Chemistry in the Molten State: Opportunities for Designing and Tuning the Emission Properties of Halide Perovskites

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Download Hi-Res ImageDownload to MS-PowerPointCite This:Inorg. Chem. 2023, 62, 35, 14252-14260
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    Chemistry in the Molten State: Opportunities for Designing and Tuning the Emission Properties of Halide Perovskites
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    • Feten Hleli
      Feten Hleli
      MOLTECH-Anjou, UMR-CNRS 6200, Université d’Angers, 2 Bd Lavoisier, 49045 Angers, France
      Laboratoire Physico-Chimie de l′Etat Solide, Département de Chimie, Faculté des Sciences de Sfax, Université de Sfax, B.P. 1171, 3000 Sfax, Tunisia
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    • Nicolas Mercier*
      Nicolas Mercier
      MOLTECH-Anjou, UMR-CNRS 6200, Université d’Angers, 2 Bd Lavoisier, 49045 Angers, France
      *Email: [email protected]
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      Orcidhttps://orcid.org/0000-0003-0458-0789
    • Maroua Ben Haj Salah
      Maroua Ben Haj Salah
      MOLTECH-Anjou, UMR-CNRS 6200, Université d’Angers, 2 Bd Lavoisier, 49045 Angers, France
      More by Maroua Ben Haj Salah
    • Magali Allain
      Magali Allain
      MOLTECH-Anjou, UMR-CNRS 6200, Université d’Angers, 2 Bd Lavoisier, 49045 Angers, France
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    • Nabil Zouari
      Nabil Zouari
      Laboratoire Physico-Chimie de l′Etat Solide, Département de Chimie, Faculté des Sciences de Sfax, Université de Sfax, B.P. 1171, 3000 Sfax, Tunisia
      More by Nabil Zouari
    • Florian Massuyeau
      Florian Massuyeau
      Nantes Université, CNRS, Institut des Matériaux de Nantes Jean Rouxel, IMN, F-44000 Nantes, France
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    • Romain Gautier
      Romain Gautier
      Nantes Université, CNRS, Institut des Matériaux de Nantes Jean Rouxel, IMN, F-44000 Nantes, France
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    Inorganic Chemistry

    Cite this: Inorg. Chem. 2023, 62, 35, 14252–14260
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    https://doi.org/10.1021/acs.inorgchem.3c01566
    Published August 22, 2023
    Copyright © 2023 American Chemical Society
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    Abstract

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    A series of monolayered lead halide hybrid perovskites (HO2C(CH2)n−1NH3)2PbX4, named (Cn)2PbX4 (n = 4–6, X = Cl, Br), exhibiting a low congruent melting temperature (Tm) (Tm = 130 °C for (C4)2PbBr4), high stability in the molten state, and whitish type emission, are reported. From the synthesis in the molten state, rare solid solutions of mixed organic cations (Cn1–xCn′x)2PbX4 (n, n′ = 4–6; X = Cl, Br; 0 ≤ x ≤1) as well as solid solutions of mixed halides (Cn)2Pb(X1–yX′y)4 (n = 4–6; X, X′ = Cl, Br; 0 ≤ y ≤1) have been prepared and characterized (thermal behavior, powder X–ray diffraction (PXRD), photoluminescence properties). The impact of substitutions is significant on the thermal properties, lowering the Tm down to 100 °C for (C4)2Pb(Br0.25Cl0.75)4. The emission properties are slightly tuned in the case of mixed organic cation systems, whereas modifications are more dramatic in the case of mixed halide systems, leading to emission properties through the entire visible region. These results illustrate the great opportunities offered by the congruent melting properties of halide perovskites allowing syntheses in the molten state.

    Copyright © 2023 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.inorgchem.3c01566.

    • Experimental details for synthesis; XRD characterizations; DSC curves; structural analysis; PL and PLE spectra, and X-ray crystallographic data of (Cn)2PbX4 (n = 6, X = Br; n = 6, X = Cl; n = 4, X = Cl) (PDF)

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    CCDC 2256357–2256359 contain the supplementary crystallographic data for this paper. These data can be obtained free of charge via www.ccdc.cam.ac.uk/data_request/cif, or by emailing [email protected], or by contacting The Cambridge Crystallographic Data Centre, 12 Union Road, Cambridge CB2 1EZ, UK; fax: +44 1223 336033.

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    Cited By

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    This article is cited by 2 publications.

    1. Irina A. Shentseva, Andrey N. Usoltsev, Nikita A. Korobeynikov, Maxim N. Sokolov, Sergey A. Adonin. Discrete Hexa- and Binuclear Heterometallic Iodobismuthate(III) Complexes with Cu(I) and Ag(I). Inorganic Chemistry 2024, 63 (40) , 18774-18780. https://doi.org/10.1021/acs.inorgchem.4c02792
    2. Wei Wang, Cheng-Dong Liu, Chang-Chun Fan, Xiao-Bin Fu, Chang-Qing Jing, Ming-Liang Jin, Yu-Meng You, Wen Zhang. Rational Design of 2D Metal Halide Perovskites with Low Congruent Melting Temperature and Large Melt-Processable Window. Journal of the American Chemical Society 2024, 146 (13) , 9272-9284. https://doi.org/10.1021/jacs.4c00768
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    Inorganic Chemistry

    Cite this: Inorg. Chem. 2023, 62, 35, 14252–14260
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.inorgchem.3c01566
    Published August 22, 2023
    Copyright © 2023 American Chemical Society
    Request reuse permissions

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