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首页> 外文期刊>Chemistry: A European journal >Luminescent alkynylplatinum(II) complexes of 2,6-bis(N-alkylbenzimidazol-2 '-yl)pyridine-type ligands with ready tunability of the nature of the emissive states by solvent and electronic property modulation
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Luminescent alkynylplatinum(II) complexes of 2,6-bis(N-alkylbenzimidazol-2 '-yl)pyridine-type ligands with ready tunability of the nature of the emissive states by solvent and electronic property modulation

机译：2,6-双（N-烷基苯并咪唑-2'-基）吡啶型配体的发光炔基铂（II）配合物，可通过溶剂和电子性质调节来调节发射态的性质

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A new class of luminescent alkynylplatinum(II) complexes of tridentate bis(N-alkylbenzimidazol-2'-yl)pyridines (bzimpy), [Pt(R,R'-bzimpy)(C C-R '')]X (X=PF6; OTf), and one of their chloro precursor complexes, [Pt(R,R'-bzimpy)Cl]PF6, have been synthesized and characterized; one of the alkynyl complexes has also been structurally characterized by X-ray crystallography. Electrochemical studies showed that the oxidation wave is alkynyl ligand-based in nature with some mixing of the metal center-based contribution, whereas the two quasi-reversible reduction couples are mainly bzimpy-based reductions. The electronic absorption and luminescence properties of the complexes have also been investigated. In solution, the high-energy and intense absorption bands are assigned as the pi-pi* intraligand (IL) transitions of the bzimpy and alkynyl ligands, whereas the low-energy and moderately intense absorptions are assigned to an admixture of metal-to-ligand charge-transfer (MLCT) (d pi(Pt)->pi*(R,R'-bzimpy)) and ligand-to-ligand charge-transfer (LLCT) (pi(C C-R '')->pi*(R,R'-bzimpy)) transitions. Upon variation of the electronic effects of the arylalkynyl ligands, vibronic-structured or structureless emission bands, originating from triplet metal-perturbed intraligand (IL) or an admixture of triplet metal-to-ligand charge-transfer (MLCT) and ligand-to-ligand charge-transfer (LLCT) excited states respectively, were observed in solution. Interestingly, two of the complexes showed a dual luminescence that was sensitive to the polarity of the solvents. Upon cooling from 298 K to 155 K, drastic color, UV/Vis, and luminescence changes were observed in a butyronitrile solution of 1, and were ascribed to the formation of aggregate species through (PtPt)-Pt-... and pi-pi stacking interactions. DFT and time-dependent DFT (TD-DFT) calculations have been performed to verify and elucidate the results of the electrochemical and photophysical properties.
机译：三齿双（N-烷基苯并咪唑-2'-基）吡啶（bzimpy），[Pt（R，R'-bzimpy）（C CR''）] X（X = PF6）的新型发光炔基铂（II）配合物; OTf），及其氯前体配合物之一[Pt（R，R'-bzimpy）Cl] PF6均已合成并表征;炔基配合物之一也已经通过X射线晶体学进行了结构表征。电化学研究表明，氧化波本质上是基于炔基配体的，并且混合了一些基于金属中心的贡献，而两个准可逆的还原对主要是基于bzimpy的还原。还研究了配合物的电子吸收和发光性质。在溶液中，高能和强吸收带被指定为bzimpy和炔基配体的pi-pi *配体（IL）跃迁，而低能和中等强度的吸收被指定为金属与金属的混合物配体电荷转移（MLCT）（d pi（Pt）-> pi *（R，R'-bzimpy））和配体至配体电荷转移（LLCT）（pi（C CR''）-> pi * （R，R'-bzimpy））过渡。改变芳基炔基配体的电子效应后，会产生振动结构或无结构的发射带，该发射带源自三重态金属扰动的配体（IL）或三重态金属至配体的电荷转移（MLCT）和配体至的混合物在溶液中分别观察到配体电荷转移（LLCT）激发态。有趣的是，两种配合物均显示出对溶剂极性敏感的双重发光。从298 K冷却到155 K后，在丁腈溶液1中观察到剧烈的颜色，UV / Vis和发光变化，并归因于通过（PtPt）-Pt -...和pi- pi堆叠交互。已经进行了DFT和时变DFT（TD-DFT）计算，以验证和阐明电化学和光物理性质的结果。

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