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首页> 外文学位 >Photophysical and photochemical characterization of platinum(II) complexes intercalated into zirconium phosphate layers for chemosensing applications.
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Photophysical and photochemical characterization of platinum(II) complexes intercalated into zirconium phosphate layers for chemosensing applications.

机译：铂（II）配合物的光物理和光化学特性，可插入到磷酸锆层中进行化学传感。

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摘要

The intercalation of platinum(II) complexes, such as chloro(2,6-bis(N-methylbenzimidazol-2-yl)pyridine)platinum(II) ([Pt(Me2bzimpy)Cl]+), chloro(2,2':6',2"-terpyridine)platinum(II) ([Pt(tpy)Cl]+), 2,4,6-trimethyl-phenyl(2,2':6',2"-terpyridine)platinum(II) ([Pt(tpy)mes]+), di-(mu-pyrazolate)-bis(4,4'-dimethyl-2,2'-bipyridine)platinum(II) ([{Pt(4,4-dmbpy)(mu-pz)}2]2+), and 1,4,7-trithiacyclononane(2,2'-bipyridine)platinum(II) ([Pt(bpy)ttcn]2+) into zirconium phosphate layers have been investigated for future use as chemosensors.;[Pt(Me2bzimpy)Cl]+, [Pt(tpy)Cl]+ and [Pt(tpy)mes] + are readily ion-exchanged into 10.3 A-ZrP to give novel luminescent materials. Spectroscopic measurements show that the physical and chemical structures of the complexes and the layers are maintained. The results are consistent with an expansion of the interlayer spacing to ∼18 A in order to accommodate aggregates of closely interacting platinum complexes. [Pt(Me2bzimpy)Cl]+-exchanged ZrP exhibits distinct absorption and emission spectroscopic signatures that are independent of loading levels and characteristic of low-lying MMLCT states resulting from short Pt···Pt spacings. By contrast, the spectroscopic properties of [Pt(tpy)Cl] +-exchanged ZrP are dependent on loading levels, suggesting the existence of more than one type of intercalated platinum aggregate.;In order to ensure the presence of Pt···Pt interactions and tune the photophysical properties, we also accomplished the direct ion-exchange of [{Pt(4,4-dmbpy)(mu-pz)}2]2+ into 10.3 A-ZrP layers. The zirconium phosphate layers promote the formation of a mixed-valence platinum system incorporated in a rigid-framework matrix and interesting photophysical differences between powders and colloidal suspensions. The spectroscopic properties of this new system are consistent with little-to-no metal-metal interactions. The "platinum blues" are not known to be emissive and the [{Pt(4,4'-dmbpy)(mu-pz)} 2]2+-exchanged ZrP materials are brightly emissive in colloidal suspensions and powders at room temperature. We have achieved blue-green, blue, and near-UV emission from suspensions of the intercalated material in different solvents suggesting that they play key roles that facilitate structural changing processes within the ZrP microenvironment.;To better access the influence of axial interactions on the electronic structures and tune the photophysical properties, we also accomplished the direct ion-exchange of [Pt(bpy)ttcn]2+ into 10.3 A-ZrP layers. The zirconium phosphate layers promote a fluxional behavior of the apical Pt-S distances, which accounts for interesting photophysical differences between powders and colloidal suspensions.;Powders and thin films of the platinum(II) complexes-exchanged ZrP materials exhibit distinctive colors and show intense emission at room temperature, depending on their stacking properties within the layers. These intercalated materials exhibit reversible vapochromic and vapoluminescent behavior upon exposure to polar and non-polar VOCs, such as methylene chloride, methanol, acetonitrile, tetrahydrofurane, benzene, and hexane.
机译：铂（II）配合物的插入，例如氯（2,6-双（N-甲基苯并咪唑-2-基）吡啶）铂（II）（[Pt（Me2bzimpy）Cl] +），氯（2,2' ：6'，2“-吡啶（R）（II）（[Pt（tpy）Cl] +），2,4,6-三甲基-苯基（2,2'：6'，2”-吡啶（R） ）（[Pt（tpy）mes] +），二-（mu-pyrazolate）-bis（4,4'-dimethyl-2,2'-bipyridine）platinum（II）（[{Pt（4,4-dmbpy ）（mu-pz）} 2] 2+）和1,4,7-三硫代环壬烷（2,2'-联吡啶）铂（II）（[Pt（bpy）ttcn] 2+）已进入磷酸锆层[Pt（Me2bzimpy）Cl] +，[Pt（tpy）Cl] +和[Pt（tpy）mes] +易于离子交换成10.3 A-ZrP，从而提供新颖的发光材料。光谱测量表明配合物和各层的物理和化学结构得以保持。结果与层间间距扩展至约18 A一致，以适应紧密相互作用的铂络合物的聚集体。 [Pt（Me2bzimpy）Cl] +交换的ZrP表现出明显的吸收和发射光谱特征，与载荷水平和低Pt···Pt间距导致的低洼MMLCT状态的特征无关。相比之下，[Pt（tpy）Cl] +交换的ZrP的光谱性质取决于负载水平，表明存在一种以上类型的插层铂聚集体。为了确保Pt···Pt的存在相互作用并调节光物理性质，我们还完成了[{Pt（4,4-dmbpy）（mu-pz）} 2] 2+的直接离子交换成10.3 A-ZrP层。磷酸锆层促进了混合价铂体系的形成，该体系结合在刚性骨架基质中，并促进了粉末和胶体悬浮液之间有趣的光物理差异。该新系统的光谱性质与几乎没有金属-金属相互作用相一致。众所周知，“铂蓝”是发光的，在室温下，[{Pt（4,4'-dmbpy）（mu-pz）} 2] 2+交换的ZrP材料在胶体悬浮液和粉末中明亮地发光。我们已经从插层材料在不同溶剂中的悬浮液中获得了蓝绿色，蓝色和近紫外线发射光，这表明它们在ZrP微环境中起着促进结构变化过程的关键作用。电子结构和调整光物理性质，我们还完成了[Pt（bpy）ttcn] 2+的直接离子交换成10.3 A-ZrP层。磷酸锆层促进了顶部Pt-S距离的通量行为，这解释了粉末和胶体悬浮液之间有趣的光物理差异。;铂（II）配合物交换的ZrP材料的粉末和薄膜呈现出独特的颜色并显示出强烈的在室温下发射，取决于它们在各层中的堆叠特性。这些插层材料在暴露于极性和非极性VOC（例如二氯甲烷，甲醇，乙腈，四氢呋喃，苯和己烷）时显示出可逆的变色和蒸发发光行为。

著录项

  • 作者

    Rivera Orellano, Eladio J.;

  • 作者单位

    University of Puerto Rico, Rio Piedras (Puerto Rico).;

  • 授予单位 University of Puerto Rico, Rio Piedras (Puerto Rico).;
  • 学科 Inorganic chemistry.
  • 学位 Ph.D.
  • 年度 2008
  • 页码 155 p.
  • 总页数 155
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

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