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Highly Efficient Self-Trapped Bluish White-Light Emission from[Pb4Cl5]3+Nodes in a Moisture-Tolerant Metal–Organic Framework

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摘要 Highly luminescent zero-dimensional(0D)metal halide clusters attract widespread attention owing to strong exciton confinement and populated self-trapped states but often exhibit narrow emission and are susceptible to hydrolysis.Herein,we demonstrate a moisture-resistant metal–organic framework(MOF)consisting of cationic 0D[Pb_(4)Cl_(5)]^(3+)nodes bridged by adamantanetetracarboxylate.Upon near-UV excitation,the material emits intrinsic broadband bluish white-light emission with high external quantum efficiency of 35%and a color rendering index of 76.Unlike organoammonium cations in lead perovskites,the Pb-carboxylate coordination affords the MOF to be chemically stable and photostable in high humidity.The photoemitter exhibits undiminished photoemissions under ambient conditions[∼60%relative humidity(RH)]upon continuous UV irradiation(143 mW/cm^(2),365 nm)for 7 days.The insertion of[Na_(4)Cl]^(3+)moieties will connect 0D units into two-dimensional(2D)metal halide layers to limit structural strain and decrease the quantum efficiency from 35%to 15%,confirming the key importance of 0D units for efficient emission.
出处 《CCS Chemistry》 CAS 2022年第2期540-547,共8页 中国化学会会刊(英文)
基金 supported by grants from the National Natural Science Foundation of China(nos.21971197 and 51772217) the Shanghai Rising-Star Program(no.20QA1409500) the Recruitment of Global Youth Experts by China,the Fundamental Research Funds for the Central Universities,and the Science&Technology Commission of Shanghai Municipality(no.19DZ2271500).
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