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首页> 外文期刊>Langmuir: The ACS Journal of Surfaces and Colloids >Facile reduction of zeolite-encapsulated viologens with solvated electrons and selective dispersion of inter- and intramolecular dimers of propylene-bridged bisviologen radical cation
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Facile reduction of zeolite-encapsulated viologens with solvated electrons and selective dispersion of inter- and intramolecular dimers of propylene-bridged bisviologen radical cation

机译：用溶剂化的电子轻松还原沸石包封的紫精，并选择性分散丙烯桥双紫精自由基阳离子的分子间和分子内二聚体

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Zeolite-Y (Y), zeolite-L (L), mordenite (M), and ZSM-5 exchanged with methyl viologen C1VC12+ and N',N "-trimethylenebis( 1-methyl-4,4'-bipyridinium) thenceforth bisviologen) C1V2+-C-3-VC12+ were prepared. Treatment of the dried, viologen-doped zeolites with solvated electrons in diethyl ether readily yields the corresponding viologen radical cation, i.e., C1VC1.+ and C1V.+-C-3-VC1.+ within the zeolite pores. Although C1V.+-C-3-VC1(.+) readily folds to its intramolecular dimer C-3[C1V.+](2) in solution, it remains in the open form in the four zeolites. C1VC1.+ readily dimerizes to [C1VC1.+](2) at high concentrations in L but not; in other zeolites. However, C1V.+-C-3-VC1.+ does not dimerize by itself in any of the four zeolites even at high concentrations. C1VC1.+ readily dimerizes in Y, L, and M when the pores are filled with water. The hydration-induced dimerization also works well for C1V.+-C-3-VC1.+ in L and M. This leads to selective formation of the unprecedented intermolecular dimer of bisviologen radical cation, i.e., [C1V.+-C-3-VC1.+](2) in L and M. The intramolecular analogue C-3[C1V.+](2) can also be dispersed into Y, L, and M by direct occlusion of its bisperchlorate salt from the acetonitrile solution. The broad similar to 530 nm band of the viologen radical dimer splits into two when the viologen radical moieties are forced to juxtapose in the collinear conformation within the narrow and straight channels oft and M. The near infrared band of the viologen radical dimer Progressively blue shifts with decreasing the interannular distance. This paper thus demonstrates a novel use of zeolites to selectively disperse inter- and intramolecular dimers of diradical dication and to lock the viologen radical dimers into the collinear conformation which allows us to delineate the spectral variation of viologen radical dimers with changing the interannular conformation and distance. [References: 98]
机译：沸石-Y（Y），沸石-L（L），丝光沸石（M）和ZSM-5与甲基紫精C1VC12 +和N'，N“-三亚甲基双（1-甲基-4,4'-联吡啶）交换后）制备C1V2 + -C-3-VC12 +，用乙醚中的溶剂化电子处理干燥的，掺杂紫精的沸石，可轻松产生相应的紫精自由基阳离子，即C1VC1。+和C1V。+-C-3-VC1。尽管C1V。+-C-3-VC1（。+）易于折叠成溶液中的分子内二聚体C-3 [C1V。+]（2），但在四种沸石中仍保持开放状态。 。C1VC1。+在L中很容易在高浓度下二聚为[C1VC1。+]（2），但在其他沸石中则不。沸石即使在高浓度下也是如此，当孔中充满水时，C1VC1。+在Y，L和M中易于二聚;水合诱导的二聚化对于C1V。+-C-3-VC1。+在L和M中也很有效。这导致了前所未有的分子间d的选择性形成bisviologen自由基阳离子，即L和M中的[C1V。+-C-3-VC1。+]（2）。分子内类似物C-3 [C1V。+]（2）也可以分散到Y中， L和M通过直接从乙腈溶液中吸收其双高氯酸盐而得到。当强迫力基团在t和M的狭窄和笔直通道内的共线构象中并置时，力基团二聚体的类似于530 nm的宽条带分成两部分。力基团二聚体的近红外带逐渐蓝移减小环间距。因此，本文证明了一种新颖的沸石用途，可选择性地分散双自由基药物的分子间和分子内二聚体，并将紫精自由基二聚体锁定为共线构象，这使我们能够通过改变环内构象和距离来描绘紫精自由基二聚体的光谱变化。 [参考：98]

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