TY - JOUR
T1 - Novel 3D Cubic Topology in Hybrid Lead Halides with a Symmetric Aromatic Triammonium Exhibiting Water Stability
AU - Vasileiadou, Eugenia S.
AU - Tajuddin, Imra S.
AU - De Siena, Michael C.
AU - Klepov, Vladislav V.
AU - Kepenekian, Mikaël
AU - Volonakis, George
AU - Even, Jacky
AU - Wojtas, Lukasz
AU - Spanopoulos, Ioannis
AU - Zhou, Xiuquan
AU - Iyer, Abishek K.
AU - Fenton, Julie L.
AU - Dichtel, William R.
AU - Kanatzidis, Mercouri G.
N1 - Publisher Copyright:
© 2023 American Chemical Society.
PY - 2023/7/25
Y1 - 2023/7/25
N2 - 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.
AB - 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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U2 - 10.1021/acs.chemmater.3c00164
DO - 10.1021/acs.chemmater.3c00164
M3 - Article
AN - SCOPUS:85164692485
SN - 0897-4756
VL - 35
SP - 5267
EP - 5280
JO - Chemistry of Materials
JF - Chemistry of Materials
IS - 14
ER -