甲烷单加氧酶的模型化合物:以树脂为载体的双铁(Ⅲ) 催化剂的合成、表征及催化性能的研究(英文)

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使用树脂为载体,合成了6种新的双铁(Ⅲ)催化剂,成功的模拟了可溶性甲烷单加氧酶(MMO)的双核铁中心。这是首次使用树脂作为载体合成模拟MMO的非均相催化剂。在室温下以乙腈为溶剂,30%的过氧化氢或特丁基过氧化氢做氧化剂,环己烷或乙苯作为底物的反应中,催化剂具有MMO相似的催化活性。其中,使用大孔氨甲基树脂为载体合成的催化剂能有效地催化乙苯氧化得到较好的转化率(总收率达69.9%,TON值达55.3)。同时研究了树脂的颗粒大小及阴离子供体对催化性能的影响。使用粒径0.675~0.280mm的树脂和ClO4-的阴离子供体所合成的催化剂具有很好的催化活性。最后探讨了催化剂的回收和再利用。 Six kinds of new double iron (Ⅲ) catalysts were synthesized by using resin as carrier, and the double iron core of soluble methane monooxygenase (MMO) was successfully simulated. This is the first time a heterogeneous catalyst for the synthesis of mimetic MMO using a resin as a support. The catalyst has similar MMO catalytic activity in the reaction of acetonitrile as solvent, 30% hydrogen peroxide or t-butyl hydroperoxide as oxidant and cyclohexane or ethylbenzene as substrates at room temperature. Among them, the catalyst synthesized by using macroporous ammonia methyl resin as catalyst can effectively catalyze the oxidation of ethylbenzene to obtain a good conversion (total yield of 69.9% and TON value of 55.3). At the same time, the influence of the particle size of the resin and the anion donor on the catalytic performance was studied. The catalyst synthesized by using resin with particle size of 0.675-0.280 mm and anion donor of ClO4- has good catalytic activity. Finally, the catalyst recovery and reuse was discussed.
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