Catalytic oxidation of cyclic hydrocarbons with hydrogen peroxide using Fe complexes immobilized into montmorillonite

Catalytic oxidation of cyclic hydrocarbons with hydrogen peroxide using Fe complexes immobilized into montmorillonite
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使用固定在蒙脱土中的铁配合物用过氧化氢催化氧化环烃

DOI:
10.1016/j.cattod.2019.12.023
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发表时间:
2020
期刊:
影响因子:
5.3
通讯作者:
Yahiro Hidenori
Yahiro Hidenori
中科院分区:
化学2区
文献类型:
--
作者:
Yamaguchi Syuhei;Ihara Daijiro;Yamashita Yuki;Uemoto Yudai;Yahiro Hidenori

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[Fe(配体)x]2+与蒙脱土([Fe(配体)x]2+@Mont,配体:2,2‘;采用离子交换法制备了6‘,2’-三联吡啶(x = 2)、1,10-邻菲咯啉(x = 3)和2,2‘-联吡啶(x = 3),用[Fe(配体)x](ClO4)2提供的[Fe(配体)x]2+络合物取代蒙脱石中的阳离子(可能是钙离子)。在[Fe(Ligand)x]2+@Mont催化剂上进行了环己烷和苯的催化氧化反应,得到了所需的醇作为主要反应产物,而整齐的蒙脱石没有表现出催化活性。无论反应条件如何,在所考察的所有催化剂中,[Fe(Terpy)2]2+@Mont(terpy代表2,2‘;6’,2‘-联吡啶)对上述底物的H_2O_2氧化反应表现出最好的催化性能。
[Fe(Ligand)x]2+complexes immobilized into montmorillonite ([Fe(Ligand)x]2+@Mont, Ligand: 2,2′;6′,2′'-terpyridine (x = 2), 1,10-phenanthroline (x = 3), and 2,2′-bipyridine (x = 3)) were prepared by an ion-exchange method whereby cations present within montmorillonite (probably Ca2+) were replaced by [Fe(Ligand)x]2+complexes provided by [Fe(Ligand)x](ClO4)2. The catalytic properties of the species obtained were then investigated in the oxidation of cyclic hydrocarbons, such as cyclohexane and benzene, with H2O2. The catalytic oxidation of cyclohexane and benzene with H2O2over [Fe(Ligand)x]2+@Mont catalysts proceeded, and the desired alcohols were obtained as the main reaction products, whereas no catalytic activity was displayed by neat montmorillonite. Regardless of the reaction conditions, [Fe(terpy)2]2+@Mont (terpy stands for 2,2′;6′,2′'-terpyridine) exhibited the best catalytic performance in the oxidation of the mentioned substrates by H2O2, among all the catalysts tested.
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