FSM-16系列改性中孔分子筛的制备及其对2-甲基吲哚和环己烯-2-酮的Michael加成催化作用

Synthesis of Modified Mesoporous Zeolites FSM-16 Series and their Catalytic Performance for Michael Addition of 2-Methyl Indole to Cyclohex-2-enone

以十六烷基三甲基溴化铵(CTMAB)为模板剂,制备了改性中孔分子筛Zr-FSM-16、Al-FSM-16和Zr-Al-FSM-16,并用XRD、SEM、IR及BET等技术手段对分子筛进行表征。在无溶剂条件下,考察了它们对2-甲基吲哚与环己烯-2-酮的Michael加成反应合成药物中间体3-(2-甲基-1H-吲哚-3-基)环己酮的催化活性。实验结果表明,Al、Zr掺杂进入分子筛骨架中,导致分子筛孔道变大,而骨架结构没有明显改变;Al、Zr掺杂改性的FSM-16分子筛催化剂活性有了较大提高,其中Zr-FSM-16分子筛催化剂表现出较好的活性。在催化剂用量7.5%、2-甲基吲哚与环己烯-2-酮的摩尔比1.0∶1.1、反应温度80℃、反应时间120 min的较优条件下,2-甲基吲哚转化率达到75.4%。

The modified mesoporous zeolites A1-FSM-16,Zr-FSM-16,and A1-Zr-ESM-16 were synthesized using cetyltrimethyl ammonium bromide （CTMAB） as the template,and characterized by XRD,IR,SEM,and BET.These catalysts were evaluated for synthesis of 3-（2-methyl-lH-indol-3-yl） cyclohexanone by catalytic Michael addition of 2-methylindole to cyclohex-2-enone under a solvent free condition.Al and Zr doping into the skeleton of the molecular sieve leads to larger pores molecular sieve,but the skeleton structure does not change significantly.A1 or Zr doping increases the catalytic activity of FSM-16 molecular sieves and the Zr-FSM-16 molecular sieve has better activity.Under the following optimum reaction conditions：catalyst dosage 7.5 ％,molar ratio of cyclohex-2-enone to 2-methylindole being 1∶1.1,reaction temperature 80 ℃ and reaction time 120 min,the yield of 3-（2-methyl-1H-indol-3-yl） cyclohexanone is up to 75.4％.