表面修饰多壁碳纳米管负载二氧化钛的制备及催化碳酸二甲酯与苯酚酯交换反应的性能

引用本文: 周喜, 葛鑫, 唐荣芝, 陈彤, 王公应. 表面修饰多壁碳纳米管负载二氧化钛的制备及催化碳酸二甲酯与苯酚酯交换反应的性能[J]. 催化学报, 2014, 35(4): 481-489. doi: 10.1016/S1872-2067(14)60010-3 shu

Citation: Xi Zhou, Xin Ge, Rongzhi Tang, Tong Chen, Gongying Wang. Preparation and catalytic property of modified multi-walled carbon nanotube-supported TiO₂ for the transesterification of dimethyl carbonate with phenol[J]. Chinese Journal of Catalysis, 2014, 35(4): 481-489. doi: 10.1016/S1872-2067(14)60010-3 shu

表面修饰多壁碳纳米管负载二氧化钛的制备及催化碳酸二甲酯与苯酚酯交换反应的性能

周喜 ^a,b, ,
葛鑫 ^a, ,
唐荣芝 ^a, ,
陈彤 ^{a,
,} ,
王公应 ^{a,
,}

通讯作者: 陈彤, 王公应; 陈彤, 王公应

基金项目:
国家高技术研究发展计划(863计划, SS2013AA031703) (863计划, SS2013AA031703)

四川省青年科技创新研究团队(2013TD0010). (2013TD0010)

摘要: 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.

关键词:

English

Preparation and catalytic property of modified multi-walled carbon nanotube-supported TiO₂ for the transesterification of dimethyl carbonate with phenol

Xi Zhou ^a,b, ,
Xin Ge ^a, ,
Rongzhi Tang ^a, ,
Tong Chen ^{a,
,} ,
Gongying Wang ^{a,
,}

1.
a Chengdu Institute of Organic Chemistry, Chinese Academy of Sciences, Chengdu 610041, Sichuan, China;

Corresponding author: 陈彤, 王公应; 陈彤, 王公应

Received Date: 07 November 2013
Available Online: 20 April 2014
Fund Project:
国家高技术研究发展计划(863计划, SS2013AA031703)

四川省青年科技创新研究团队(2013TD0010).

Abstract: 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 microscopy, 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 transesterification 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 carbonate. The catalyst could be reused for the transesterification in four runs with only slight loss of its catalytic activity.

Key words:

1. [1] Shaikh A A G, Sivaram S. Chem Rev, 1996, 96: 951[1] Shaikh A A G, Sivaram S. Chem Rev, 1996, 96: 951
2. [2] Ronchin L, Vavasori A, Amadio E, Cavinato G, Toniolo L. J Mol Catal A, 2009, 298: 23[2] Ronchin L, Vavasori A, Amadio E, Cavinato G, Toniolo L. J Mol Catal A, 2009, 298: 23
3. [3] Yang X J, Han J Y, Du Z P, Yuan H, Jin F, Wu Y X. Catal Commun, 2010, 11: 643[3] Yang X J, Han J Y, Du Z P, Yuan H, Jin F, Wu Y X. Catal Commun, 2010, 11: 643
4. [4] Yalfani M S, Lolli G, Wolf A, Mleczko L, Müller T E, Leitner W. Green Chem, 2013, 15: 1146[4] Yalfani M S, Lolli G, Wolf A, Mleczko L, Müller T E, Leitner W. Green Chem, 2013, 15: 1146
5. [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. Appl Catal A, 2012, 439-440: 149[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. Appl Catal A, 2012, 439-440: 149
6. [6] Cao P, Yang J, Yang X G, Yao J, Wang Y, Wang G Y. Chin J Catal (曹平, 杨建, 杨先贵, 姚洁, 王越, 王公应. 催化学报), 2009, 30: 65[6] Cao P, Yang J, Yang X G, Yao J, Wang Y, Wang G Y. Chin J Catal (曹平, 杨建, 杨先贵, 姚洁, 王越, 王公应. 催化学报), 2009, 30: 65
7. [7] Chen T, Han H J, Yao J, Wang G Y. Catal Commun, 2007, 8: 1361[7] Chen T, Han H J, Yao J, Wang G Y. Catal Commun, 2007, 8: 1361
8. [8] Deshmukh K M, Qureshi Z S, Dhake K P, Bhanage B M. Catal Commun, 2010, 12: 207[8] Deshmukh K M, Qureshi Z S, Dhake K P, Bhanage B M. Catal Commun, 2010, 12: 207
9. [9] Niu H Y, Yao J, Wang Y, Wang G Y. Catal Commun, 2007, 8: 355[9] Niu H Y, Yao J, Wang Y, Wang G Y. Catal Commun, 2007, 8: 355
10. [10] Du Z P, Xiao Y H, Chen T, Wang G Y. Catal Commun, 2008, 9: 239.[10] Du Z P, Xiao Y H, Chen T, Wang G Y. Catal Commun, 2008, 9: 239.
11. [11] Niu H Y, Guo H M, Yao J, Wang Y, Wang G Y. J Mol Catal A, 2006, 259: 292[11] Niu H Y, Guo H M, Yao J, Wang Y, Wang G Y. J Mol Catal A, 2006, 259: 292
12. [12] Kim W B, Lee J S. J Catal, 1999, 185: 307[12] Kim W B, Lee J S. J Catal, 1999, 185: 307
13. [13] Tong D S, Chen T, Yao J, Wang Y, Wang G Y, Shi D C, Li Z, Chen Z M. Chin J Catal (童东绅, 陈彤, 姚洁, 王越, 王公应, 石大川, 李正, 陈志明. 催化学报), 2007, 28: 190[13] Tong D S, Chen T, Yao J, Wang Y, Wang G Y, Shi D C, Li Z, Chen Z M. Chin J Catal (童东绅, 陈彤, 姚洁, 王越, 王公应, 石大川, 李正, 陈志明. 催化学报), 2007, 28: 190
14. [14] Tong D S, Yao J, Wang Y, Niu H Y, Wang G Y. J Mol Catal A, 2007, 268: 120[14] Tong D S, Yao J, Wang Y, Niu H Y, Wang G Y. J Mol Catal A, 2007, 268: 120
15. [15] Cao M, Meng Y Z, Lu Y X. Catal Commun, 2005, 6: 802[15] Cao M, Meng Y Z, Lu Y X. Catal Commun, 2005, 6: 802
16. [16] Li Z H, Wang Y J, Ding X S, Zhao X Q. J Nat Gas Chem, 2009, 18: 104[16] Li Z H, Wang Y J, Ding X S, Zhao X Q. J Nat Gas Chem, 2009, 18: 104
17. [17] Li Z H, Cheng B W, Su K M, Gu Y, Xi P, Guo M L. J Mol Catal A, 2008, 289: 100[17] Li Z H, Cheng B W, Su K M, Gu Y, Xi P, Guo M L. J Mol Catal A, 2008, 289: 100
18. [18] Zhou W Q, Zhao X Q, Wang Y J, Zhang J Y. Appl Catal A, 2004, 260: 19[18] Zhou W Q, Zhao X Q, Wang Y J, Zhang J Y. Appl Catal A, 2004, 260: 19
19. [19] Wang S, Bai R X, Mei F M, Li G X. Catal Commun, 2009, 11: 202[19] Wang S, Bai R X, Mei F M, Li G X. Catal Commun, 2009, 11: 202
20. [20] Kim Y T, Park E D. Appl Catal A, 2009, 356: 211[20] Kim Y T, Park E D. Appl Catal A, 2009, 356: 211
21. [21] Li B J, Tang R Z, Chen T, Wang G Y. Chin J Catal (李碧静, 唐荣芝, 陈彤, 王公应. 催化学报), 2012, 33: 601[21] Li B J, Tang R Z, Chen T, Wang G Y. Chin J Catal (李碧静, 唐荣芝, 陈彤, 王公应. 催化学报), 2012, 33: 601
22. [22] Zhang X Y, Ma Q, Cheng B B, Wang J, Li J S, Nie F D. J Nat Gas Chem, 2012, 21: 774[22] Zhang X Y, Ma Q, Cheng B B, Wang J, Li J S, Nie F D. J Nat Gas Chem, 2012, 21: 774
23. [23] Intarapong P, Iangthanarat S, Phanthong P, Luengnaruemitchai A, Jai-In S. J Energy Chem, 2013, 22: 690[23] Intarapong P, Iangthanarat S, Phanthong P, Luengnaruemitchai A, Jai-In S. J Energy Chem, 2013, 22: 690
24. [24] Nigrovski B, Zavyalova U, Scholz P, Pollok K, Müller M, Ondruschka B. Carbon, 2008, 46: 1678[24] Nigrovski B, Zavyalova U, Scholz P, Pollok K, Müller M, Ondruschka B. Carbon, 2008, 46: 1678
25. [25] Kang J C, Deng W P, Zhang Q H, Wang Y. J Energy Chem, 2013, 22: 321[25] Kang J C, Deng W P, Zhang Q H, Wang Y. J Energy Chem, 2013, 22: 321
26. [26] Karimi A, Nasernejad B, Rashidi A M. J Energy Chem, 2013, 22: 582[26] Karimi A, Nasernejad B, Rashidi A M. J Energy Chem, 2013, 22: 582
27. [27] Ge X, Li B J, Hu J, Chen T, Wang G Y, Hu X T. Acta Chim Sin (葛鑫, 李碧静, 胡静, 陈彤, 王公应, 胡徐腾. 化学学报), 2011, 69: 2328[27] Ge X, Li B J, Hu J, Chen T, Wang G Y, Hu X T. Acta Chim Sin (葛鑫, 李碧静, 胡静, 陈彤, 王公应, 胡徐腾. 化学学报), 2011, 69: 2328
28. [28] Ge X, Li B J, Hu J, Chen T, Wang G Y, Hu X T. Chem Eng (China) (葛鑫, 李碧静, 胡静, 陈彤, 王公应, 胡徐腾. 化学工程), 2011, 39: 61.[28] Ge X, Li B J, Hu J, Chen T, Wang G Y, Hu X T. Chem Eng (China) (葛鑫, 李碧静, 胡静, 陈彤, 王公应, 胡徐腾. 化学工程), 2011, 39: 61.
29. [29] Kim W B, Lee J S. Catal lett, 1999, 59: 83[29] Kim W B, Lee J S. Catal lett, 1999, 59: 83

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1.
沈阳化工大学材料科学与工程学院沈阳 110142

表面修饰多壁碳纳米管负载二氧化钛的制备及催化碳酸二甲酯与苯酚酯交换反应的性能

通讯作者: 陈彤, 王公应; 陈彤, 王公应

English

Preparation and catalytic property of modified multi-walled carbon nanotube-supported TiO₂ for the transesterification of dimethyl carbonate with phenol

Corresponding author: 陈彤, 王公应; 陈彤, 王公应

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

表面修饰多壁碳纳米管负载二氧化钛的制备及催化碳酸二甲酯与苯酚酯交换反应的性能

通讯作者: 陈彤, 王公应; 陈彤, 王公应

English

Preparation and catalytic property of modified multi-walled carbon nanotube-supported TiO2 for the transesterification of dimethyl carbonate with phenol

Corresponding author: 陈彤, 王公应; 陈彤, 王公应

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

Preparation and catalytic property of modified multi-walled carbon nanotube-supported TiO₂ for the transesterification of dimethyl carbonate with phenol

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs