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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Studies on bis(halogeno) dioxomolybdenum(VI)-bipyridine complexes: Synthesis and catalytic activity
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Studies on bis(halogeno) dioxomolybdenum(VI)-bipyridine complexes: Synthesis and catalytic activity

机译：双（卤素）二氧钼（VI）-联吡啶配合物的研究：合成和催化活性

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摘要

Dioxomolybdenum(VI) complexes with the general formula [MoO2Cl2L2] (L-2= 3,3'-dimethyl-2,2'-bipyridine, 5,5'-dimethyl-2,2'-bipyridine, 6,6'-dimethyl-2,2'-bipyridine, 4,4'-dibromo-2,2'-bipyridine, 5,5'-dibromo-2,2'-bipyridine, 5,5'-diamino-2,2'-bipyridine; 5,5'-dinitro-2,2'-bipyridine; 5,5'-di-ethoxycarbonyl-2,2'-bipyridine; 6-phenyl-2,2'-bipyridine; 2,2':6', 2 ''-terpyridine) have been prepared and characterised. [MoO2Cl2(5,5'-diethoxycarbonyl-2,2'-bipyridine)] has been examined by single crystal X-ray analysis. The complexes were applied as homogenous catalysts for the epoxidation of cyclooctene with tert-butyl hydroperoxide (TBHP) as oxidising agent. The new compounds show an overall high activity and are highly selective catalysts in the epoxidation of cyclooctene. The stability of the complexes and differences in the catalytic activity can be clearly attributed to electronic contributions of the functional groups on bipyridine ligands and to steric restrictions. DFT calculations have assisted in a better understanding of the stability of the complexes and are in agreement with experiment. The influence of the terminal oxo ligands and the Lewis base ligands on the Mo center keep the compounds on quite a stable level of electron density.
机译：通式为[MoO2Cl2L2]（L-2 = 3,3'-二甲基-2,2'-联吡啶，5,5'-二甲基-2,2'-联吡啶，6,6'-二甲基-2,2'-联吡啶，4,4'-二溴-2,2'-联吡啶，5,5'-二溴-2,2'-联吡啶，5,5'-二氨基-2,2'-联吡啶; 5，5′-二硝基-2，2′-联吡啶; 5，5′-二乙氧基羰基-2，2′-联吡啶; 6-苯基-2，2′-联吡啶; 2，2′：6′，已制备并表征了2''-叔吡啶）。 [MoO2Cl2（5,5'-二乙氧基羰基-2,2'-联吡啶）]已经通过单晶X射线分析进行了检查。该配合物用作均相催化剂，用于环辛烯与叔丁基氢过氧化物（TBHP）作为氧化剂的环氧化。在环辛烯的环氧化中，这些新化合物表现出总体高活性，是高度选择性的催化剂。配合物的稳定性和催化活性的差异可以清楚地归因于联吡啶配体上官能团的电子贡献和空间限制。 DFT计算有助于更好地理解配合物的稳定性，并与实验相符。末端氧代配体和路易斯碱配体对Mo中心的影响使化合物保持在相当稳定的电子密度水平。

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