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A Highly Luminescent Metallo-Supramolecular Radical Cage
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-10-05 , DOI: 10.1021/jacs.3c07477 Junjuan Shi 1 , Wei Xu 2 , Hao Yu 1 , Xing Wang 3 , Feng Jin 4 , Qingming Zhang 4 , Houyu Zhang 1 , Qiming Peng 3 , Alim Abdurahman 5 , Ming Wang 1
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-10-05 , DOI: 10.1021/jacs.3c07477 Junjuan Shi 1 , Wei Xu 2 , Hao Yu 1 , Xing Wang 3 , Feng Jin 4 , Qingming Zhang 4 , Houyu Zhang 1 , Qiming Peng 3 , Alim Abdurahman 5 , Ming Wang 1
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Luminescent metal-radicals have recently received increasing attention due to their unique properties and promising applications in materials science. However, the luminescence of metal-radicals tends to be quenched after formation of metallo-complexes. It is challenging to construct metal-radicals with highly luminescent properties. Herein, we report a highly luminescent metallo-supramolecular radical cage (LMRC) constructed by the assembly of a tritopic terpyridinyl ligand RL with tris(2,4,6-trichlorophenyl)methyl (TTM) radical and Zn2+. Electrospray ionization-mass spectrometry (ESI-MS), traveling-wave ion mobility-mass spectrometry (TWIM-MS), X-ray crystallography, electron paramagnetic resonance (EPR) spectroscopy, and superconducting quantum interference device (SQUID) confirm the formation of a prism-like supramolecular radical cage. LMRC exhibits a remarkable photoluminescence quantum yield (PLQY) of 65%, which is 5 times that of RL; meanwhile, LMRC also shows high photostability. Notably, significant magnetoluminescence can be observed for the high-concentration LMRC (15 wt % doped in PMMA film); however, the magnetoluminescence of 0.1 wt % doped LMRC film vanishes, revealing negligible spin-spin interactions between two radical centers in LMRC.
中文翻译：
高发光金属超分子自由基笼
发光金属自由基由于其独特的性质和在材料科学中的广阔应用前景，最近受到越来越多的关注。然而，金属自由基的发光在形成金属络合物后往往会被猝灭。构建具有高发光特性的金属自由基具有挑战性。在此，我们报道了一种高发光金属超分子自由基笼（LMRC ），其由三位三联吡啶基配体RL与三（2,4,6-三氯苯基）甲基（TTM）自由基和Zn 2+组装而成。电喷雾电离质谱 (ESI-MS)、行波离子淌度质谱 (TWIM-MS)、X 射线晶体学、电子顺磁共振 (EPR) 光谱和超导量子干涉装置 (SQUID) 证实了棱柱状超分子自由基笼。LMRC的光致发光量子产率（PLQY）高达65%，是RL的5倍；同时，LMRC还表现出较高的光稳定性。值得注意的是，高浓度LMRC（PMMA 薄膜中掺杂 15 wt%）可以观察到显着的磁致发光；然而，0.1 wt% 掺杂的LMRC薄膜的磁致发光消失，表明LMRC中两个自由基中心之间的自旋-自旋相互作用可以忽略不计。
更新日期：2023-10-05
中文翻译：
高发光金属超分子自由基笼
发光金属自由基由于其独特的性质和在材料科学中的广阔应用前景，最近受到越来越多的关注。然而，金属自由基的发光在形成金属络合物后往往会被猝灭。构建具有高发光特性的金属自由基具有挑战性。在此，我们报道了一种高发光金属超分子自由基笼（LMRC ），其由三位三联吡啶基配体RL与三（2,4,6-三氯苯基）甲基（TTM）自由基和Zn 2+组装而成。电喷雾电离质谱 (ESI-MS)、行波离子淌度质谱 (TWIM-MS)、X 射线晶体学、电子顺磁共振 (EPR) 光谱和超导量子干涉装置 (SQUID) 证实了棱柱状超分子自由基笼。LMRC的光致发光量子产率（PLQY）高达65%，是RL的5倍；同时，LMRC还表现出较高的光稳定性。值得注意的是，高浓度LMRC（PMMA 薄膜中掺杂 15 wt%）可以观察到显着的磁致发光；然而，0.1 wt% 掺杂的LMRC薄膜的磁致发光消失，表明LMRC中两个自由基中心之间的自旋-自旋相互作用可以忽略不计。
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