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首页> 外文期刊>The journal of physical chemistry, C. Nanomaterials and interfaces >Transient Spectroscopic Characterization of the Genesis of a Ruthenium Complex Catalyst Supported on Zeolite Y
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Transient Spectroscopic Characterization of the Genesis of a Ruthenium Complex Catalyst Supported on Zeolite Y

机译:沸石Y负载钌配合物催化剂成因的瞬态光谱表征

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摘要

A mononuclear ruthenium complex anchored to dealuminated zeolite HY, Ru(acac)(C2H4)_2~+ (acac = acetylacetonate, C5H7O2~-), was characterized in flow reactors by transient infrared (IR) spectroscopy and Ru K edge X-ray absorption spectroscopy. The combined results show how the supported complex was converted into a form that catalyzes ethene conversion to butene. The formation of these species resulted from the removal of acac ligands from the ruthenium (as shown by IR and extended X-ray absorption fine structure (EXAFS) spectra) and the simultaneous decrease in the symmetry of the ruthenium complex, with the ruthenium .Remaining mononuclear and its oxidation state remaining essentially unchanged (as shown by EXAFS and X-ray absorption near-edge structure spectra). The removal of anionic acac ligands from the ruthenium was evidently compensated by the bonding of other anionic ligands, such as hydride from H2 in the feed stream, to form species suggested to be Ru(H)(C2H4)_2~+, which is coordinatively unsaturated and inferred to react with ethene, leading to the observed formation of butene in a catalytic process.
机译:固定在脱铝沸石HY上的单核钌配合物Ru(acac)(C2H4)_2〜+(acac =乙酰丙酮酸,C5H7O2〜-)在流动反应器中通过瞬态红外(IR)光谱和Ru K边X射线吸收进行表征光谱学。合并结果表明,负载型配合物如何转化为催化乙烯转化为丁烯的形式。这些物种的形成是由于从钌中去除了acac配体(如IR和扩展X射线吸收精细结构(EXAFS)光谱所示)以及钌络合物同时降低了钌配合物的对称性。单核及其氧化态基本保持不变(如EXAFS和X射线吸收近边缘结构光谱所示)。从钌中去除阴离子的acac配体显然是通过其他阴离子配体的键合(例如进料流中H2的氢化物)的键合来补偿的,从而形成建议为Ru(H)(C2H4)_2〜+的物种。不饱和的并且推断与乙烯反应,导致在催化过程中观察到丁烯的形成。

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