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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >A redox-active porous coordination network film based on a Ru complex as a building block on an ITO electrode
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A redox-active porous coordination network film based on a Ru complex as a building block on an ITO electrode

机译：基于Ru络合物作为ITO电极上的结构单元的氧化还原活性多孔配位网络膜

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摘要

The combination of self-assembled monolayer (SAM) and layer-by-layer (LbL) growth methods for the construction of a surface porous film has the potential to incorporate a wide range of chemical functionalities on a solid surface. A novel redox-active Ru complex with 2,6-bis(N-pyridylbenzimidazolyl)-pyridine ligands (Ru complex 1), in which four peripheral pyridine groups act as coordination sites, was used as a building block for a porous coordination network film. By using (4-pyridyl)phenylphosphonic acid as a SAM primer layer on an ITO surface, the Ru complex 1 was immobilized by the successive reaction of PdCl_2 on the ITO electrode in the LbL growth method. Multilayer growth was monitored by UV-vis spectra and cyclic voltammetry, in which the linear increases of both absorbance and the peak current were observed. This result indicated that the regular accumulation of Ru complex 1 onto the ITO surface took place. The permselectivity of the present porous coordination network structure was examined using redox-active molecular probes with different sizes and charges such as ferrocene, trimethylaminomethylferrocene, the Os bis(2,6-bis(N-methylbenzimidazolyl)-pyridine) complex, and tetrathiofulvarene (TTF). With the Os complex and cationic ferrocene, only the catalytic peak was observed as a prewave of the adsorbed Ru(ii/iii) peak at +0.73 V. On the other hand, the oxidation peak of ferrocene was observed around 0 V vs. Fc~+/Fc even for nine-layered films in addition to the adsorbed Ru(ii/iii) peak. From these results, not only molecular size but also electrostatic interaction plays an important role in the permeation into the Ru complex 1 porous network film.
机译：自组装单层（SAM）和逐层（LbL）生长方法的组合用于构建表面多孔膜，具有在固体表面上结合多种化学功能的潜力。具有2,6-双（N-吡啶基苯并咪唑基）-吡啶配体的新型氧化还原活性Ru络合物（Ru络合物1），其中四个外围吡啶基团充当配位点，被用作多孔配位网络薄膜的结构单元。通过使用（4-吡啶基）苯基膦酸作为ITO表面上的SAM底漆层，通过LbL生长方法中PdCl_2在ITO电极上的连续反应将Ru配合物1固定化。通过UV-可见光谱和循环伏安法监测多层生长，其中观察到吸光度和峰值电流的线性增加。该结果表明Ru络合物1在ITO表面上的规则积累。使用具有不同大小和电荷的氧化还原活性分子探针，如二茂铁，三甲基氨基甲基二茂铁，Os双（2,6-双（N-甲基苯并咪唑基）-吡啶）络合物和四硫富瓦瓦烯（ TTF）。使用Os络合物和阳离子二茂铁时，仅在+0.73 V处观察到催化峰为Ru（ii / iii）吸附峰的预波。另一方面，在0 V vs. Fc附近观察到二茂铁的氧化峰除吸附的Ru（ii / iii）峰外，甚至对于九层膜也为〜+ / Fc。从这些结果，不仅分子大小而且静电相互作用在渗透到Ru络合物1多孔网络膜中都起重要作用。

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