钌团簇配合物的合成与性能研究

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摘要

以含羰基和含胺有机双功能配体为基础,研究了钌簇配合物的合成方法。根据红外光谱数据、热重法和元素分析确定了获得的簇组合的结构。配体I和II是由环戊烷和环己烷的羧酸氯化物与乙烯缩合,然后用胺基取代氯原子得到的。为了得到钌与所合成配体的簇状配合物,将三氯化钌盐(RuCl3)溶解于水中,在氮气气氛中剧烈搅拌,将计算量的硼氢化钠按比例加入所得溶液中。迅速出现的黑色分散的金属钌纳米颗粒没有沉淀。当加入有机配体I和II时,形成相应的簇化合物III和IV,并在45分钟内逐渐从水溶液中析出。得到的深棕色沉淀物用蒸馏水洗涤,并在35-400℃的氮气气氛中干燥。测定了合成化合物的熔融温度,确定了III - 2060С和IV - 2220С簇的组分(已分解)。簇状化合物的红外光谱显示出强烈的吸收带,表征酮羰基和胺片段的存在。与初始配体相比,簇状化合物中酮基团的吸收带向更高的频率偏移。当比较初始配体和相应簇化合物中CN键的红外振动时,也观察到类似的图像。元素分析的结果证实了簇状化合物的结构,并与在水溶液中钌盐与金属氢化物还原形成簇状化合物的概念完全一致。显然,在这种情况下,形成了最稳定的具有四面体结构的钌团簇。热重分析可以确定在3180C温度下存在一个质量数为744.8的峰,对应于四个钌原子的簇组合。在分解的各个阶段,实验质量损失与计算值吻合较好。关键词:合成,钌,簇状配合物,含胺核配体,双功能配体,环戊基氨基酮,环己基氨基酮。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
SYNTHESIS AND PROPERTIES OF RUTHENIUM CLUSTER COMPLEXES
Methods for the synthesis of ruthenium cluster complexes based on carbonyl and amine-containing organic bifunctional ligands have been developed. The structure of the obtained combinations of clusters were determined on the basis of IR spectroscopy data, thermogravimetry, and elemental analysis. Samples of ligands I and II were obtained by condensation of carboxylic acid chlorides of cyclopentane and cyclohexane with ethylene followed by replacement of the chlorine atom by amine groups. To obtain cluster complexes of ruthenium with the synthesized ligands the ruthenium trichloride salt (RuCl3) was dissolved in water, and the calculated amount of sodium borohydride was added in portions to the resulting solution under vigorous stirring in nitrogen atmosphere. Rapidly emerging black-dispersed nanoparticles of metallic ruthenium did not precipitate. When organic ligands I and II are added, the corresponding cluster compounds III and IV are formed, which gradually over 45 min. precipitated from an aqueous solution. The resulting dark-brown precipitates were washed with distilled water and dried in a nitrogen atmosphere at a temperature of 35-400C. The melting temperatures of the synthesized compounds were determined, the components for cluster III - 2060С and cluster IV - 2220С (with decomposition). The IR spectra of cluster compounds show intense absorption bands characterizing the presence of both the ketone carbonyl group and the amine fragment. The absorption bands of ketone groups in cluster compounds are shifted towards higher frequencies compared to the initial ligands. A similar picture is also observed when comparing the IR vibrations of CN bonds in the initial ligands and the corresponding cluster compounds. The results of elemental analysis confirm the structures of cluster compounds and are in complete agreement with the concept that cluster compounds are formed upon the reduction of ruthenium salts with metal hydrides in an aqueous solution. Apparently, in this case, the most stable ruthenium clusters with tetrahedral structure are formed.. Thermogravimetric analysis made it possible to establish the presence of a peak at a temperature of 3180C with a mass number of 744.8 , corresponding to a cluster combination of four ruthenium atoms. At each stage of decomposition, the experimental mass losses are in good agreement with the calculated values. Keywords: synthesis, ruthenium, cluster complexes, amine and caryonyl containing ligands, bifunctional ligands, cyclopentyl amino ketone, cyclohexyl amino ketone.
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