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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Heterometallic Cu-II/Ln(III) polymers active in the catalytic aerobic oxidation of cycloalkenes under solvent-free conditions
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Heterometallic Cu-II/Ln(III) polymers active in the catalytic aerobic oxidation of cycloalkenes under solvent-free conditions

机译：在无溶剂条件下，杂动机Cu-II / LN（III）聚合物活性在催化有氧氧化中的环烯烃

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摘要

Heterometallic 3d-4f inorganic polymers were prepared using 3,5 pyridinedicarboxylic acid (H2PDC), {[CuLn(2)(PDC)(2)(SO4)(2)(H2O)(6)]H2O}(n) (Ln: Sm-III, CuSmPDC, Eu-III, CuEuPDC, Gd-III, and CuGdPDC). These catalysts are active in the aerobic oxidation of cycloalkenes under solvent-free conditions, with a conversion for the oxidation of cyclohexene of 71% after one hour of the reaction, and a TOF value of 1438 h(-1) for CuSmPDC. On the other hand, the oxidation of cycloheptene and cyclooctene exhibited slightly lower conversions of 52% and 47%, and TOF values of 1053 and 159 h(-1) after 1 and 6 hours of the reaction, respectively. The radical mechanism for the oxidation reaction of cyclohexene was assessed by Raman and EPR spectroscopy. The first evidenced the formation of Cu-O-2 adducts and the second permitted is to observe the presence of the oxygen centered radical species, which act as initiators of the reaction chain to generate the products. An increase in the temperature of the reaction correlates with the adduct formation, and with the enhancement of the oxidation reaction.
机译：使用3,5吡啶二羧酸（H2PDC）制备杂动机3D-4F无机聚合物，{[CULN（2）（PDC）（2）（SO 4）（2）（2）（H2O）（6）] H 2 O}（N）（LN ：SM-III，CUSMPDC，EU-III，CUEUPDC，GD-III和CUGDPDC）。在无溶剂条件下，这些催化剂在环烷烃的有氧氧化中活跃，在反应1小时后的环己氧化的环己烯的转化率为71％，CUSMPDC的TOF值为1438 H（-1）。另一方面，在反应的反应后，环庚烯和环庚烯的氧化略低于52％和47％，以及1053和159h（-1）的TOF值。通过拉曼和EPR光谱评估环己烯的氧化反应的自由基机制。首先证明了Cu-O-2加合物的形成，第二个允许的是观察氧中心自由基物质的存在，其充当反应链的引发剂以产生产品。反应温度的增加与加合物形成相关，并随着氧化反应的增强。

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