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首页> 外文期刊>Chemistry: A European journal >Robust Self-Assembled Monolayers of RuII and OsII Polypyridines on Gold Surfaces: Exploring New Potentials
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Robust Self-Assembled Monolayers of RuII and OsII Polypyridines on Gold Surfaces: Exploring New Potentials

机译：RuII和OsII聚吡啶在金表面上的牢固的自组装单分子膜：开拓新的潜力

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摘要

Metal complexes [MACHTUNGTRENUNG(phtpy)-ACHTUNGTRENUNG(pztpy)]ACHTUNGTRENUNG(PF6)2 (phtpy=4’-phenyl- 2,2’:6’,2’’-terpyridine, pztpy=4’-(N-piperazinyl)- 2,2’:6’,2’’-terpyridine, M= Ru, Os) were prepared and examined spectroscopically and electrochemically. The piperazine attachment was found to significantly modify the photophysical and electrochemical properties compared to the parent bis-terpyridine complexes, causing a red-shift of the 1MLCT (23 nm, 53.9 eV) and a substantial cathodic shift of the redox potential (0.3 V for Ru, 0.23 V for Os). Self-assembled monolayers (SAMs) of the complexes on polished gold electrodes were generated simply by the in situ formation of a dithiocarbamate (DTC) anchoring group at the terminal piperazinyl nitrogen on the pztpy ligand. Cyclic voltammetry revealed that the monolayers show excellent reversible behaviour and exceptional stability. The high stability of the SAMs is attributed to the strong bidentate attachment to the gold surface of the DTC tether and the favourable low oxidation potentials of the complexes which result from the electron-rich piperazine nitrogen on the pztpy ligand. Such DTC-based SAMs demonstrate a substantial improvement over commonly- employed thiol-based systems, and offer new scope for future development.
机译：金属配合物[MACHTUNGTRENUNG（phtpy）-ACHTUNGTRENUNG（pztpy）] ACHTUNGTRENUNG（PF6）2（phtpy = 4'-苯基-2,2'：6'，2''-吡啶，pztpy = 4'-（N-哌嗪基）制备了2，2′：6′，2′-吡啶，M ＝ Ru，Os，并进行了光谱和电化学检查。与母体双-叔吡啶配合物相比，发现哌嗪附着显着改变了光物理和电化学性质，导致1MLCT（23 nm，53.9 eV）发生红移，氧化还原电势发生显着的阴极移位（对于C值为0.3 V Ru，对于Os为0.23 V）。通过在pztpy配体的末端哌嗪基氮上原位形成二硫代氨基甲酸酯（DTC）锚定基团，可以在抛光的金电极上生成复合物的自组装单层（SAMs）。循环伏安法表明，单分子层具有出色的可逆行为和出色的稳定性。 SAMs的高稳定性归因于DTC系链的金表面牢固的双齿连接以及pztpy配体上的富电子哌嗪氮导致的配合物的良好低氧化电位。这样的基于DTC的SAM证明了与常用的基于硫醇的系统相比有了实质性的改进，并为将来的开发提供了新的空间。

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