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Targeted Synthesis of NIR Luminescent Rhenium Diimine cis,trans‐[Re( )(CO)2(L)2]n+ Complexes Containing N‐Donor Axial Ligands: Photophysical, Electrochemical, and Theoretical Studies
ChemPlusChem ( IF 3.4 ) Pub Date : 2020-11-09 , DOI: 10.1002/cplu.202000597
J. R. Shakirova 1 , S. Nayeri 2 , S. Jamali 2 , Vitaly V. Porsev 1 , Vladislav V. Gurzhiy 1 , Oleg V. Levin 1 , I. O. Koshevoy 3 , S. P. Tunik 1
Affiliation  

The combined action of ultraviolet irradiation and microwave heating onto acetonitrile solution of [Re(urn:x-wiley:21926506:media:cplu202000597:cplu202000597-math-0002 )(CO)3(NCMe)]OTf (urn:x-wiley:21926506:media:cplu202000597:cplu202000597-math-0003 =phenantroline and neocuproine) afforded cis,trans‐Re(urn:x-wiley:21926506:media:cplu202000597:cplu202000597-math-0004 )(CO)2(NCMe)2]+ acetonitrile derivatives. Substitution of relatively labile NCMe with a series of aromatic N‐donor ligands (pyridine, pyrazine, 4,4’‐bipyridine, N‐methyl‐4,4’‐bipyridine) gave a novel family of the diimine cis,trans‐[Re(urn:x-wiley:21926506:media:cplu202000597:cplu202000597-math-0005 )(CO)2(L)2]+ complexes. Photophysical studies of the obtained compounds in solution revealed unusually high absorption across the visible region and NIR phosphorescence with emission band maxima ranging from 711 to 805 nm. The nature of emissive excited states was studied using DFT calculations to show dominant contribution of 3MLCT (dπ(Re)→π*(urn:x-wiley:21926506:media:cplu202000597:cplu202000597-math-0006 )) character. Electrochemical (CV and DPV) studies of the monocationic diimine complexes revealed one reduction and one oxidation wave assigned to reduction of the diimine moiety and oxidation of the rhenium center, respectively.

中文翻译:

NIR发光R二亚胺的顺式,反式[Re()(CO)2(L)2] n +含N受体轴向配体的配合物的靶向合成:光物理,电化学和理论研究

紫外辐射和微波加热对[Re(缸:x-wiley:21926506:media:cplu202000597:cplu202000597-math-0002 )(CO)3(NCMe)] OTf(缸:x-wiley:21926506:media:cplu202000597:cplu202000597-math-0003 =菲咯啉和新铜环素)的乙腈溶液的联合作用提供了顺式,反式-Re(缸:x-wiley:21926506:media:cplu202000597:cplu202000597-math-0004 )(CO)2(NCMe)2 ] +乙腈衍生物。用一系列芳香族N-供体配体(吡啶,吡嗪,4,4'-联吡啶,N-甲基-4,4'-联吡啶)取代相对不稳定的NCMe,得到了一个新的二亚胺顺式,反式-[Re (缸:x-wiley:21926506:media:cplu202000597:cplu202000597-math-0005 )(CO)2(L)2 ] +复合体。对溶液中获得的化合物的光物理研究表明,可见光区域的吸收异常高,NIR磷光的最大发射带范围为711至805 nm。使用DFT计算研究了发射激发态的性质,以显示3 MLCT(dπ(Re)→π*(缸:x-wiley:21926506:media:cplu202000597:cplu202000597-math-0006 ))特征的主要贡献。对单阳离子二亚胺配合物的电化学(CV和DPV)研究表明,一种还原和一种氧化波分别对应于二亚胺部分的还原和the中心的氧化。
更新日期:2020-11-23
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