制备了表面修饰多壁碳纳米管负载TiO2的催化剂，并将其应用于碳酸二甲酯与苯酚的酯交换反应.采用X射线电子能谱、透射电子显微镜、低温N2吸附-脱附和X射线衍射等对催化剂进行了表征.结果表明，以低浓度的氨水(0.4%)代替去离子水作为沉淀剂时，制备的催化剂显示出更好的催化活性、分离性与重复使用性.考察了TiO2负载量、催化剂用量及反应时间对反应性能的影响.在最佳反应条件下，苯酚转化率为42.5%，碳酸甲苯酯与碳酸二苯酯的总选择性达到99.9%以上.经过4次重复使用后，催化剂的活性略有下降.
Modified multi-walled carbon nanotube-supported TiO2 samples were prepared and used as an efficient heterogeneous catalyst for the transesterification of dimethyl carbonate with phenol. The catalysts were characterized by X-ray photoelectron spectroscopy, transmission electron micros-copy, N2 adsorption-desorption, and X-ray powder diffraction. The results showed that the catalyst, which was prepared using a low concentration (0.4%) of ammonium hydroxide as the precipitant instead of ionized water, had better catalytic activity, separability, and reusability properties. The effects of the TiO2 loading, amount of catalyst and reaction time on the performance of the trans-esterification reaction were also studied. Under the optimum reaction conditions, the conversion of phenol reached 42.5% with over 99.9% selectivity for methyl phenyl carbonate and diphenyl car-bonate. The catalyst could be reused for the transesterification in four runs with only slight loss of its catalytic activity.
参考文献
| [1] | Shaikh A A G;Sivaram S .[J].CHEMICAL REVIEWS,1996,96:951. |
| [2] | Ronchin L;Vavasori A;Amadio E;Cavinato G Toniolo L .[J].Journal of Molecular Catalysis A:Chemical,2009,298:23. |
| [3] | Yang X J;Han J Y;Du Z P;Yuan H Jin F Wu Y X .[J].CATALYSIS COMMUNICATIONS,2010,11:643. |
| [4] | Yalfani M S;Lolli G;Wolf A;Mleczko L Müller T E Leitner W .[J].Green Chemistry,2013,15:1146. |
| [5] | Yuan X L;Zhang M;Chen X D;An N H Liu G Liu Y Zhang W X Yan W F Jia M J .[J].Applied Catalysis A:General,2012,439-440:149. |
| [6] | 曹平,杨建,杨先贵,姚洁,王越,王公应.有机钛化合物催化碳酸二甲酯与乙酸苯酯合成碳酸二苯酯[J].催化学报,2009(01):65-68. |
| [7] | Chen T;Han H J;Yao J;Wang G Y .[J].CATALYSIS COMMUNICATIONS,2007,8:1361. |
| [8] | Deshmukh K M;Qureshi Z S;Dhake K P;Bhanage B M .[J].Catal Com-mun,2010,12:207. |
| [9] | Niu H Y;Yao J;Wang Y;Wang G Y .[J].CATALYSIS COMMUNICATIONS,2007,8:355. |
| [10] | Du Z P;Xiao Y H;Chen T;Wang G Y .[J].CATALYSIS COMMUNICATIONS,2008,9:239. |
| [11] | Niu HY;Guo HM;Yao H;Wang Y;Wang GY .Transesterification of dimethyl carbonate and phenol to diphenyl carbonate catalyzed by samariurn diiodide[J].Journal of molecular catalysis, A. Chemical,2006(1/2):292-295. |
| [12] | Kim W B;Lee J S .[J].Journal of Catalysis,1999,185:307. |
| [13] | 童东绅,陈彤,姚洁,王越,王公应,石大川,李正,陈志明.钒-铜复合氧化物催化碳酸二甲酯和苯酚酯交换合成碳酸二苯酯[J].催化学报,2007(03):190-192. |
| [14] | Tong D S;Yao J;Wang Y;Niu H Y Wang G Y .[J].Journal of Molecular Catalysis A:Chemical,2007,268:120. |
| [15] | Cao M;Meng Y Z;Lu Y X .[J].CATALYSIS COMMUNICATIONS,2005,6:802. |
| [16] | Li Z H;Wang Y J;Ding X S;Zhao X Q .[J].Journal of Natural Gas Chemistry,2009,18:104. |
| [17] | Li Z H;Cheng B W;Su K M;Gu Y Xi P Guo M L .[J].Journal of Molecular Catalysis A:Chemical,2008,289:100. |
| [18] | Zhou W Q;Zhao X Q;Wang Y J;Zhang J Y .[J].Applied Catalysis A:General,2004,260:19. |
| [19] | Wang S;Bai R X;Mei F M;Li G X .[J].CATALYSIS COMMUNICATIONS,2009,11:202. |
| [20] | Kim Y T;Park E D .[J].Applied Catalysis A:General,2009,356:211. |
| [21] | 李碧静,唐荣芝,陈彤,王公应.乙酰丙酮氧钛催化苯酚和碳酸二甲酯的酯交换反应[J].催化学报,2012(04):601-604. |
| [22] | Zhang X Y;Ma Q;Cheng B B;Wang J Li J S Nie F D .[J].Journal of Natural Gas Chemistry,2012,21:774. |
| [23] | Intarapong P;Iangthanarat S;Phanthong P;Luengnaruemitchai A Jai-In S .[J].J Energy Chem,2013,22:690. |
| [24] | Nigrovski B;Zavyalova U;Scholz P;Pollok K Müller M Ondruschka B .[J].CARBON,2008,46:1678. |
| [25] | Kang J C;Deng W P;Zhang Q H;Wang Y .[J].J Energy Chem,2013,22:321. |
| [26] | Karimi A;Nasernejad B;Rashidi A M .[J].J Energy Chem,2013,22:582. |
| [27] | 葛鑫,李碧静,胡静,陈彤,王公应,胡徐腾.表面活性剂对TiO_2/CNT苯酚与碳酸二甲酯酯交换活性的影响[J].化学学报,2011(19):2328-2334. |
| [28] | 葛鑫,李碧静,胡静,陈彤,王公应,胡徐腾.焙烧温度对二氧化钛催化性能的影响[J].化学工程,2011(11):61-65. |
| [29] | Kim W B;Lee J S .[J].Catalysis Letters,1999,59:83. |
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