文章摘要
胡炜杰,陈亚举,梁中秀,任清刚,周贤太,纪红兵.离子液体功能化salen Mn催化苯乙烯与CO2一锅合成碳酸苯乙烯酯[J].精细化工,2021,38(2):
离子液体功能化salen Mn催化苯乙烯与CO2一锅合成碳酸苯乙烯酯
Ionic liquid functionalized salen Mn catalyst for one-pot transformation of styrene with CO2 into styrene carbonate
投稿时间:2020-07-29  修订日期:2020-10-12
DOI:
中文关键词: 二氧化碳,催化,环氧化,环状碳酸酯,离子液体,salen Mn
英文关键词: carbon dioxide  catalysis  epoxidation  cyclic carbonate  ionic liquid  salen Mn
基金项目:
作者单位E-mail
胡炜杰 广东石油化工学院  
陈亚举 广东石油化工学院  
梁中秀 中山大学  
任清刚 广东石油化工学院  
周贤太 中山大学  
纪红兵 中山大学精细化工研究院 jihb@mail.sysu.edu.cn 
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中文摘要:
      合成了咪唑离子液体功能化salen Mn配合物(IL-salen Mn),并作为唯一催化剂成功应用于苯乙烯与二氧化碳一锅合成碳酸苯乙烯酯反应中。首先,以尿素过氧化氢(UHP)为氧化剂、吡啶氮氧化物(PyNO)为助剂,催化苯乙烯高效制备环氧苯乙烷,继而催化环氧苯乙烷与二氧化碳发生环加成反应合成碳酸苯乙烯酯。分别考察了催化剂的种类和用量、助剂用量、氧化剂种类和用量、反应时间以及反应温度等因素对上述反应的影响。当催化剂用量为8 mol%(以反应物总的物质的量记),n(苯乙烯)∶n(UHP)∶n(PyNO)=1.0∶3.0∶0.2,环氧化反应温度和时间分别为30 ℃和5 h,环加成反应温度和时间分别为80 ℃和12 h,二氧化碳压力为1 MPa时,苯乙烯的转化率为90%,碳酸苯乙烯酯收率达到32%。结合前期研究与反应时间动力学结果,推测了该串联反应可能的机理。
英文摘要:
      Imidazolium-based ionic liquid functionalized salen Mn complex (IL-salen Mn) was synthesized and employed as the only catalyst for the one-pot transformation of styrene and CO2 into styrene carbonate. First, styrene was converted efficiently into styrene oxide by using urea hydrogen peroxide (UHP) as an oxide in the presence of pyridine N-oxide (PyNO). Subsequently, the as-obtained styrene oxide was transformed into styrene carbonate via cycloaddition with CO2. The effects of reaction parameters such as catalyst type and dosage, additive amount, oxide type and amount, reaction temperature, reaction time, and pressure of CO2 were studied detailedly. When 8 mol% (based on the total mol of reactant) IL-salen Mn was used as catalyst, the molar ratio of styrene, UHP and PyNO was 1:3:0.2, epoxidation temperature was 30 ℃, epoxidation time was 5 h, the cycloaddition temperature was 80 ℃, cycloaddition time was 12 h, CO2 pressure was 1 MPa, the conversion of styrene (90 %) and selectivity of cyclic carbonate (32 %) were obtained. Furthermore, according to previous studies and in combination with the kinetic results, we proposed the possible mechanism for the tandem reaction.
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