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Family of Robust and Strongly Luminescent CuI-Based Hybrid Networks Made of Ionic and Dative Bonds
Chemistry of Materials ( IF 7.2 ) Pub Date : 2020-12-01 , DOI: 10.1021/acs.chemmater.0c03984 Alexander V. Artem’ev 1 , Maria P. Davydova 1 , Xiuze Hei 2 , Mariana I. Rakhmanova 1 , Denis G. Samsonenko 1 , Irina Yu. Bagryanskaya 3 , Konstantin A. Brylev 1 , Vladimir P. Fedin 1 , Jia-Shiang Chen 4 , Mircea Cotlet 4 , Jing Li 2
Chemistry of Materials ( IF 7.2 ) Pub Date : 2020-12-01 , DOI: 10.1021/acs.chemmater.0c03984 Alexander V. Artem’ev 1 , Maria P. Davydova 1 , Xiuze Hei 2 , Mariana I. Rakhmanova 1 , Denis G. Samsonenko 1 , Irina Yu. Bagryanskaya 3 , Konstantin A. Brylev 1 , Vladimir P. Fedin 1 , Jia-Shiang Chen 4 , Mircea Cotlet 4 , Jing Li 2
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The CuI-derived inorganic–organic hybrid compounds are considered as promising phosphors for the lighting industry. Herein, exploiting N-monoalkylated hexaminium salts, [R-HMTA]X (R = Me, Et, Pr, and propargyl; X = Cl and I), as multibridging ligands, we have designed and synthesized a unique class of one-dimensional and two-dimensional hybrid CuI-materials. The reactions of these salts with CuI give rise to All-in-One (AIO) type compounds combining ionic and dative bonds between inorganic and organic components. The latter is formed by structurally unique inorganic [CuxIy](y−x)– clusters, chains, or sheets interconnected through [R-HMTA]+ cations via multiple Cu–N bonds. The so-designed compounds at ambient temperature exhibit tunable luminescence spanning from deep blue to red color (λem = 430–625 nm) with microsecond lifetimes and the quantum efficiency of up to 78%. Remarkably, the AIO materials feature nontrivial excitation- (ED) and temperature-dependent (TD) luminescence, allowing their emission color to be finely adjusted from deep blue to red through changing the excitation wavelength and/or temperature. Based on the TD emission spectroscopy and theoretical calculations, a possible mechanism of the luminescence has been proposed. The very interesting luminescence characteristics coupled with good thermal and photostability render these AIO hybrid materials possible candidates for applications in energy-efficient lighting devices.
中文翻译：
由离子键和相键构成的基于CuI的强大且强发光的混合网络家族
CuI衍生的无机-有机杂化化合物被认为是照明行业有希望的磷光体。在本文中，我们以N-单烷基化六铵盐[R-HMTA] X（R = Me，Et，Pr和炔丙基； X = Cl和I）作为多桥联配体，设计并合成了一类独特的一维和二维混合CuI材料。这些盐与CuI的反应产生了在无机和有机组分之间结合离子键和键键的多合一（AIO）型化合物。后者是由结构独特的无机[Cu x I y ] （y - x）–通过[R-HMTA] +相互连接的簇，链或片形成的通过多个Cu–N键的阳离子。如此设计的化合物在室温下表现出从深蓝色到红色（λem = 430–625 nm）的可调发光，具有微秒的寿命，量子效率高达78％。值得注意的是，AIO材料具有非平凡的激发（ED）和温度相关（TD）发光特性，可通过改变激发波长和/或温度，将其发射颜色从深蓝色微调为红色。基于TD发射光谱和理论计算，提出了一种可能的发光机理。非常有趣的发光特性以及良好的热稳定性和光稳定性使这些AIO混合材料成为了在节能照明设备中应用的候选材料。
更新日期：2020-12-22
中文翻译：
由离子键和相键构成的基于CuI的强大且强发光的混合网络家族
CuI衍生的无机-有机杂化化合物被认为是照明行业有希望的磷光体。在本文中，我们以N-单烷基化六铵盐[R-HMTA] X（R = Me，Et，Pr和炔丙基； X = Cl和I）作为多桥联配体，设计并合成了一类独特的一维和二维混合CuI材料。这些盐与CuI的反应产生了在无机和有机组分之间结合离子键和键键的多合一（AIO）型化合物。后者是由结构独特的无机[Cu x I y ] （y - x）–通过[R-HMTA] +相互连接的簇，链或片形成的通过多个Cu–N键的阳离子。如此设计的化合物在室温下表现出从深蓝色到红色（λem = 430–625 nm）的可调发光，具有微秒的寿命，量子效率高达78％。值得注意的是，AIO材料具有非平凡的激发（ED）和温度相关（TD）发光特性，可通过改变激发波长和/或温度，将其发射颜色从深蓝色微调为红色。基于TD发射光谱和理论计算，提出了一种可能的发光机理。非常有趣的发光特性以及良好的热稳定性和光稳定性使这些AIO混合材料成为了在节能照明设备中应用的候选材料。
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