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Novel 3D Cubic Topology in Hybrid Lead Halides with a Symmetric Aromatic Triammonium Exhibiting Water Stability

Cite this: Chem. Mater. 2023, 35, 14, 5267–5280
Publication Date (Web):July 5, 2023
https://doi.org/10.1021/acs.chemmater.3c00164
Copyright © 2023 American Chemical Society

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    Abstract

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    The limitations of three-dimensional (3D) perovskites are related to their narrow structural tunability of the organic cations and their moisture sensitivity. Herein, we report a new family of 3D cubic hybrid metal halides (T-Et6)3Pb11X31 (X = I, Br), where T is 1,3,5-tris-(4-aminophenyl)benzene. The materials are synthesized through an in situ N-alkylation of T and an efficient one-step solvothermal reaction containing ethanol, initiating a tunable synthetic avenue for the acquisition of structurally complex hybrid halides with luminophores. (T-Et6)3Pb11X31 consist of an unprecedented Ia3̅ framework of [Pb11X31]9– one-dimensional (1D) chains embedded with (T-Et6)3+ cations, affording an overall 3D topology. The constituent [Pb11X31]9– chains include exclusively octahedral lead halide units with clusters of face- and edge-sharing connectivity, giving rise to weak broad emission centered at ∼660 nm observed at 78 K. (T-Et6)3Pb11I31 demonstrates water stability for at least 7 days. Synthesis through ambient pressure results in tunable structural variations of zero-dimensional (0D) structures rendering T7Pb3Br27·DMF and T2Sn3Br18·4H2O·0.5Br2, both of which feature blue PL emission at room temperature.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.chemmater.3c00164.

    • Methods; complementary syntheses; and additional structural and characterization data: data, single-crystal and powder X-ray diffraction, electronic structure, photoluminescence spectroscopy and optical properties, NMR spectroscopy, and microscope images (PDF)

    Accession Codes

    CCDC 2216512−2216515 contain the supplementary crystallographic data for this paper: X-ray crystallographic data for (T-Et6)3Pb11I31; X-ray crystallographic data for (T-Et6)3Pb11Br31; X-ray crystallographic data for T7Pb3Br27·DMF; X-ray crystallographic data for T2Sn3Br18·4H2O·0.5Br2.

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