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首页> 外文期刊>Chemistry: A European journal >High-Nuclear Organometallic Copper(I)-Alkynide Clusters: Thermochromic Near-Infrared Luminescence and Solution Stability
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High-Nuclear Organometallic Copper(I)-Alkynide Clusters: Thermochromic Near-Infrared Luminescence and Solution Stability

机译：高核有机金属铜（I）-炔烃簇：热致变色近红外发光和溶液稳定性

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摘要

Cu(CF3COO)(2) reacts with tert-butylacetylene (tBuC equivalent to CH) in methanol in the presence of metallic copper powder to give two air-stable clusters, [Cu-15(I)(tBuC equivalent to C)(10)(CF3COO)(5)]center dot tBuC equivalent to CH (1) and [Cu-16(I)(tBuC equivalent to C)(12)(CF3COO)(4)(CH3OH)(2)] (2). The assembly process involves in situ comproportionation reaction between Cu2+ and Cu-0 and the formation of two different clusters is controlled by reactants concentration. The clusters consist of Cu-15 and Cu-16 cores co-stabilized by strong by sigma- and pi-bonded tert-butylethynide and CF3COO- (together with methanol molecule in 2). Their stabilities in solution were confirmed using electrospray ionization mass spectrometry in which the cluster core remains intact for 1 in chloroform and acetone, and for 2 in acetonitrile. Strong thermochromic luminescence in the near infrared (NIR) region was observed in the solidstate. Of particular interest, the emission maximum of 1 is red-shifted from 710 nm at 298 K to 793 nm at 93 K, along with a 17-fold fluorescence enhancement. In contrast, 2 exhibits red shift from 298 to 123 K followed by blue shift from 123 to 93 K. The emission wavelength was correlated with the structural parameters using variable-temperature Xray single-crystal analyses. The rich cuprophilic interaction plays a significant role in the formation of (LMCT)-L-3 (tBuC equivalent to C -> Cu-x) excited state mixed with cluster-centered ((CC)-C-3) characters, which can be considerably influenced by temperature, leading to thermochromic luminescence. The present work provides 1) a new synthetic protocol for the high-nuclear Cu-I-alkynyl clusters; 2) a comprehensive insight into the mechanism of thermochromic luminescence; 3) unusual emissive materials with the characters of NIR and thermochromic luminescence simultaneously.
机译：Cu（CF3COO）（2）在金属铜粉存在下与叔丁基乙炔（tBuC相当于CH）在甲醇中反应生成两个空气稳定的簇[Cu-15（I）（tBuC相当于C）（10 ）（CF3COO）（5）]等于CH（1）和[Cu-16（I）（tBuC相当于C）（12）（CF3COO）（4）（CH3OH）（2）的中心点tBuC]（2） 。组装过程涉及Cu2 +和Cu-0之间的原位互补反应，两个不同簇的形成受反应物浓度控制。团簇由Cu-15和Cu-16核组成，这些核通过σ键和pi键键合的叔丁基乙炔和CF3COO-（与2中的甲醇分子共同）牢固地稳定在一起。使用电喷雾电离质谱法确认了它们在溶液中的稳定性，其中簇核对于氯仿和丙酮中的1个保持不变，而对于乙腈中的2个保持完整。在固态中，在近红外（NIR）区域观察到强热致变色发光。特别令人感兴趣的是，发射最大值1从298 K的710 nm到93 K的793 nm红移，同时荧光增强了17倍。相反，2表现出从298到123 K的红移，然后是从123到93 K的蓝移。使用可变温度X射线单晶分析，发射波长与结构参数相关。丰富的嗜铜相互作用在形成（LMCT）-L-3（tBuC等效于C-> Cu-x）激发态并混合以簇中心（（CC）-C-3）字符的过程中起着重要作用，受温度影响很大，导致热致变色发光。目前的工作提供了1）高核Cu-I-炔基簇的新合成方案; 2）全面了解热致变色发光的机理; 3）同时具有近红外和热致变色发光特性的异常发光材料。

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