常温常压下分别在离子液体 1-丁基-3-甲基咪唑四氟硼酸盐([bmim]BF4)-MeCN混合溶剂和纯MeCN溶剂中研究了CO2在Cu电极上的循环伏安行为. 结果表明, CO2均发生不可逆还原反应生成CO-2. 与纯MeCN溶剂相比,在混合溶剂中CO2还原峰电位均有正移. 这表明溶剂中的咪唑型离子液体对活化CO2有催化作用. 在混合溶剂中,以CO2和MeOH为原料合成碳酸二甲酯(DMC), 考察了[bmim]BF4/MeCN体积比、工作电极材料、 MeOH浓度和电解电位等对DMC产物收率的影响. 与其他DMC合成方法相比,本法反应条件温和、设备简单、合成产物收率较高. 在优化的条件下, DMC产物收率可达79.6%. 并提出了合成DMC可能的反应机理.
参考文献
[1] | Cipris D;Mador I L .[J].Journal of the Electrochemical Society,1978,125(12):1954. |
[2] | Bell R A .[P].US 4 310 393,1982. |
[3] | Otsuka K;Yagi T;Yamanaka I.[J].Chemistry Letters,1994(03):495. |
[4] | Otsuka K;Yagi T;Yamanaka I .[J].Electrochimica Acta,1994,39(14):2109. |
[5] | Casadei M A;Cesa S;Rossi L.[J].European Journal of Organic Chemistry,2000(13):2445. |
[6] | 张丽,罗仪文,钮东方,虞新迪,陆嘉星.温和条件下电催化CO2与环氧丙烷合成碳酸丙烯酯[J].催化学报,2007(02):100-102. |
[7] | 钮东方,徐承天,张丽,罗仪文,张凯,陆嘉星.电催化活化二氧化碳合成苯氨基甲酸乙酯[J].催化学报,2007(10):880-884. |
[8] | Welton T .[J].Chemical Reviews,1999,99(08):2071. |
[9] | Wasserscheid P.;Keim W. .Ionic liquids - New "solutions" for transition metal catalysis [Review][J].Angewandte Chemie International Edition,2000(21):3773-3789. |
[10] | Suarez P A Z;Selbach V M;Dullius J E L;Einloft S Piatnicki C M S Azambuja D S de Souza R F Dupont J .[J].Electrochimica Acta,1997,42(16):2533. |
[11] | Olivier H .[J].Journal of Molecular Catalysis A:Chemical,1999,146(1/2):285. |
[12] | Sheldon R.[J].Chemical Communications,2001(23):2399. |
[13] | Gordon C M .[J].Applied Catalysis A:General,2001,222(1/2):101. |
[14] | Cadena C;Anthony J L;Shah J K;Morrow T I Brennecke J F Maginn E J .[J].Journal of the American Chemical Society,2004,126(16):5301. |
[15] | Bonhote P.;Papageorgiou N.;Kalyanasundaram K.;Gratzel M.;Dias AP. .HYDROPHOBIC, HIGHLY CONDUCTIVE AMBIENT-TEMPERATURE MOLTEN SALTS[J].Inorganic Chemistry: A Research Journal that Includes Bioinorganic, Catalytic, Organometallic, Solid-State, and Synthetic Chemistry and Reaction Dynamics,1996(5):1168-1178. |
[16] | Okoturo OO;VanderNoot TJ .Temperature dependence of viscosity for room temperature ionic liquids[J].Journal of Electroanalytical Chemistry: An International Journal Devoted to All Aspects of Electrode Kinetics, Interfacial Structure, Properties of Electrolytes, Colloid and Biological Electrochemistry,2004(1/2):167-181. |
[17] | Kazarian S G;Briscoe B J;Welton T.[J].Chemical Communications,2000(20):2047. |
[18] | Wang J J;Tian Y;Zhao Y;Zhou K L .[J].Green Chemistry,2003,5(05):618. |
[19] | 钮东方,罗仪文,张丽,肖丽平,陆嘉星.温和条件下CO2为原料电合成碳酸二甲酯[J].有机化学,2008(05):832-836. |
[20] | Zhang L;Niu DF;Zhang K;Zhang GR;Luo YW;Lu JX .Electrochemical activation of CO2 in ionic liquid ( BMIMBF4): synthesis of organic carbonates under mild conditions[J].Green chemistry,2008(2):202-206. |
[21] | Nishida T;Tashiro Y;Yamamoto M .[J].Journal of Fluorine Chemistry,2003,120(02):135. |
[22] | Kamekawa H;Senboku H;Tokuda M .[J].Tetrahedron Letters,1998,39(12):1591. |
[23] | Islam MM;Ferdousi BN;Okajima T;Ohsaka T .A catalytic activity of a mercury electrode towards dioxygen reduction in room-temperature ionic liquids[J].Electrochemistry communications,2005(7):789-795. |
[24] | Fang S N;Fujimoto K .[J].Applied Catalysis A:General,1996,142(01):L1. |
上一张
下一张
上一张
下一张
计量
- 下载量()
- 访问量()
文章评分
- 您的评分:
-
10%
-
20%
-
30%
-
40%
-
50%