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首页> 外文期刊>Chemistry: A European journal >Increasing the Ketone Selectivity of the Cobalt-Catalyzed Radical Chain Oxidation of Cyclohexane
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Increasing the Ketone Selectivity of the Cobalt-Catalyzed Radical Chain Oxidation of Cyclohexane

机译：提高钴催化环己烷的自由基催化自由基氧化的酮选择性

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摘要

A variety of heterogeneous catalysts for the radical chain oxidation of cyclohexane has been prepared by immobilization of the well-defined cobalt acetate oligomers [py_3Co_3(mu_3-O)(OH)(O_2CCH_3)_5](PF_6) (1) and [py_4Co_2(OH)_2(O_2CH_3)_3](PF_6) (2) on carboxy-modified mesoporous silica supports A-D by carboxylate exchange. The catalytic oxidation of cyclohexane with tert-butyl hydroperoxide (TBHP) in the presence of these homogeneous and immobilized cobalt acetate complexes afforded the corresponding alcohol and ketone in high yield. The immobilization of 1 and 2 results in a significant increase of catalytic cavity. TBHP acts as a radical initiator and as source of molecular oxygen, which is also involved in the overall oxidation process. The rate of cyclohexane conversion is limited by the diffusion of molecular oxygen, and steady-state concentrations of cyclohexanone (K, ketone) and cyclohexanol (A, alcohol) are established; these determine the maximum K:A ratio.
机译：通过固定明确定义的乙酸钴低聚物[py_3Co_3（mu_3-O）（OH）（O_2CCH_3）_5]（PF_6）（1）和[py_4Co_2（在羧基改性的中孔二氧化硅上的OH）_2（O_2CH_3）_3]（PF_6）（2）通过羧酸酯交换来支持AD。在这些均相且固定化的乙酸钴络合物的存在下，用叔丁基氢过氧化物（TBHP）催化氧化环己烷，可以高收率得到相应的醇和酮。 1和2的固定化导致催化腔的显着增加。 TBHP充当自由基引发剂和分子氧源，这也参与了整个氧化过程。环己烷的转化率受到分子氧的扩散的限制，并建立了环己酮（K，酮）和环己醇（A，醇）的稳态浓度。这些决定了最大的K：A比值。

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