CAJ | 학술논문

以CuBr2和4-甲基喹啉为原料，在乙醇溶剂中制备了含溴铜（Ⅱ）配合物。通过FTIR、EA、XRD和ICP-AES表征，初步确定了配合物分子结构为[C10H9N]2CuBr2；采用密度泛函理论计算对其结构、自然原子电荷和前线轨道进行分析，进一步确定分子结构的可靠性，并将该配合物应用于乙醇氧化羰化合成碳酸二乙酯催化反应中。结果表明，在催化剂浓度为0.075 g·ml?1，反应温度为100℃，反应压力为3.5 MPa，反应时间为4 h的条件下，乙醇的转化率达到21.5%。通过探讨反应机理，认为该配合物催化剂稳定性适中，有利于主反应控制步骤 CO的插入反应，有助于中间体的形成，从而使催化活性得到提高。
이CuBr2화4-갑기규람위원료，재을순용제중제비료함추동（Ⅱ）배합물。통과FTIR、EA、XRD화ICP-AES표정，초보학정료배합물분자결구위[C10H9N]2CuBr2；채용밀도범함이론계산대기결구、자연원자전하화전선궤도진행분석，진일보학정분자결구적가고성，병장해배합물응용우을순양화탄화합성탄산이을지최화반응중。결과표명，재최화제농도위0.075 g·ml?1，반응온도위100℃，반응압력위3.5 MPa，반응시간위4 h적조건하，을순적전화솔체도21.5%。통과탐토반응궤리，인위해배합물최화제은정성괄중，유리우주반응공제보취 CO적삽입반응，유조우중간체적형성，종이사최화활성득도제고。
The copper coordination compound [C10H9N]2CuBr2 was prepared by the reaction of 4-methylchinolin with copper bromide in ethanol solution. The compound was characterized with FTIR, EA, ICP-AES and XRD, and its catalytic performance in oxidative carbonylation of ethanol was investigated. The density functional theory (DFT) calculations were performed to analyze its structure, natural atomic charges and frontier orbital energy levels. The introduction of ligand could improve catalytic activity to prepare diethyl carbonate. The per pass conversion of ethanol could reach 21.5%under the reaction conditions of temperature 373 K, pressure 3.5 MPa, time 4 h and mass concentration of catalyst in ethanol 0.075 g·ml?1. Reaction mechanism study showed that the compound had moderate stability, which benefited insertion of CO (the rate-controlling step) and formation of intermediate. Therefore, reaction activity was enhanced.