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首页> 外文期刊>Nanotechnology >1-(3 '-amino)propylsilatrane derivatives as covalent surface linkers to nanoparticulate metal oxide films for use in photoelectrochemical cells
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1-(3 '-amino)propylsilatrane derivatives as covalent surface linkers to nanoparticulate metal oxide films for use in photoelectrochemical cells

机译：1-（3'-氨基）丙基硅氧烷衍生物作为共价表面连接剂，用于光电化学电池中的纳米颗粒金属氧化物膜

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摘要

A triethanolamine-protected silane, 1-(3-amino)propylsilatrane, was incorporated into the structure of porphyrin- and ruthenium-based dyes and used to link them to transparent semiconductor nanoparticulate metal oxide films. Silatrane reacts with the metal oxide to form strong, covalent silyl ether bonds. In this study, silatrane-functionalized dyes and analogous carboxylate-functionalized dyes were used as visible light sensitizers for porous nanoparticulate SnO2 photoanodes. The performance of the dyes was compared in photoelectrochemical cells incorporating either non-regenerative or regenerative redox components. The non-regenerative cell used NADH (beta-nicotinamide adenine dinucleotide) as a sacrificial electron donor and Hg2SO4/Hg as a sacrificial cathode, whereas the regenerative cell used the iodide/triiodide redox couple. Experiments showed that the silyl ether bonding gave the electrodes increased stability toward sensitizer desorption compared to carboxylate surface linkages. Porphyrin-silatrane dyes also demonstrated similar or better performance than their carboxylate analogs in photoelectrochemical cells. The improvement correlates with the results from transient absorbance spectroscopy, which show that the longer linker on the silatrane porphyrins slows charge recombination between oxidized porphyrin and the electrode surface. The improved photoelectrochemical cell efficiency and stability of the silatrane-based dyes compared to carboxylates demonstrate that silatranes are promising agents for bonding organic molecules to metal oxide surfaces.
机译：将三乙醇胺保护的硅烷1-（3-氨基）丙基硅杂环丁烷并入卟啉和钌基染料的结构中，并用于将它们连接到透明的半导体纳米微粒金属氧化物膜上。 Silatrane与金属氧化物反应形成牢固的共价甲硅烷基醚键。在这项研究中，硅氮烷官能化的染料和类似的羧酸酯官能化的染料被用作多孔纳米颗粒SnO2光阳极的可见光敏化剂。在掺有非再生或再生氧化还原成分的光电化学电池中比较了染料的性能。非再生电池使用NADH（β-烟酰胺腺嘌呤二核苷酸）作为牺牲电子供体，Hg2SO4 / Hg作为牺牲阴极，而再生电池使用碘化物/三碘化物氧化还原对。实验表明，与羧酸盐表面键相比，甲硅烷基醚键使电极对敏化剂解吸的稳定性提高。卟啉-silatrane染料在光电化学电池中也表现出比其羧酸酯类似物相似或更好的性能。改进与瞬态吸收光谱法的结果相关，后者表明，硅烷基卟啉上的较长连接子减慢了氧化卟啉与电极表面之间的电荷重组。与羧酸盐相比，基于甲硅烷基的染料具有更高的光电化学电池效率和稳定性，证明了甲硅烷基是将有机分子结合至金属氧化物表面的有前途的试剂。

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