Pd/Fe3O4-MCNT磁性催化剂的制备、表征及催化性能

doi:10.3866/PKU.WHXB20110721

物理化学学报 >> 2011, Vol. 27 >> Issue (08): 1956-1960.doi: 10.3866/PKU.WHXB20110721

Pd/Fe₃O₄-MCNT磁性催化剂的制备、表征及催化性能

徐玲¹, 沈晓旭¹, 肖强¹, 钟依均¹, 叶素芳², 叶向荣³, 朱伟东¹

1. 浙江师范大学物理化学研究所, 先进催化材料省部共建教育部重点实验室, 浙江金华 321004;
2. 金华职业技术学院, 浙江金华 321007;
3. Pacific Northwest National Laboratory, P.O. Box 999, Richland, Washington 99352, USA

收稿日期:2011-02-25 修回日期:2011-04-19 发布日期:2011-07-19
通讯作者: 肖强, 钟依均 E-mail:xiaoq@zjnu.cn. yjzhong@zjnu.cn
基金资助:
浙江省自然科学基金 (Y4100295), 浙江省高校重大科技攻关项目(ZD2007002)及浙江省新苗人才计划项目(2009R404014) 资助

Preparation, Characterization and Catalytic Properties of Pd/Fe₃O₄-MCNT Magnetically Recyclable Catalysts

XU Ling¹, SHEN Xiao-Xu¹, XIAO Qiang¹, ZHONG Yi-Jun¹, YE Su-Fang², YE Xiang-Rong³, ZHU Wei-Dong¹

1. Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, Institute of Physical Chemistry, Zhejiang Normal University, Jinhua 321004, Zhejiang Province, P. R. China;
2. Jinhua College of Vocation and Technology, Jinhua 321007, Zhejiang Province, P. R. China;
3. Pacific Northwest National Laboratory, P.O. Box 999, Richland, Washington 99352, USA

Received:2011-02-25 Revised:2011-04-19 Published:2011-07-19
Contact: XIAO Qiang, ZHONG Yi-Jun E-mail:xiaoq@zjnu.cn. yjzhong@zjnu.cn
Supported by:
The project was supported by the Natural Science Foundation of Zhejiang Province, China (Y4100295), Key Science and Technology Program of Zhejiang Provincial Colleges, China (ZD2007002), and Young Seeding Talent Plan of Zhejiang Province, China (2009R404014).

摘要/Abstract

摘要：

利用多元醇法制备了单分散Fe₃O₄纳米粒子修饰多壁碳纳米管(MCNT)的磁性复合材料, 并以X射线衍射(XRD)、透射电镜(TEM)和X射线能量色散谱(EDS)对碳纳米管磁性复合材料的结构和组成进行了表征. 研究发现, 通过调控Fe₃O₄前驱体与MCNT载体的质量比, 可以很好地控制沉积的磁性纳米粒子大小. 以碳纳米管磁性复合材料为载体, 采用多元醇法成功制备了Pd负载量为3.0% (w)的Pd/Fe₃O₄-MCNT磁性催化剂. 磁性质测试表明碳纳米管磁性复合材料在负载Pd前后都具有良好的超顺磁性. 以肉桂醛加氢为探针反应研究了Pd/Fe₃O₄-MCNT的催化性能, 结果表明该催化剂表现出良好的催化加氢性能, 在外加磁场下催化剂能与液相反应体系高效分离, 循环使用4次后, 催化性能没有明显下降, 显示了良好的循环利用性能.

关键词: 多壁碳纳米管, 磁性复合催化剂, 多元醇法, 肉桂醛, 选择性加氢

Abstract:

A magnetic composite of multi-walled carbon nanotubes (MCNT) decorated with mono-dispersed Fe₃O₄ nanoparticles was prepared by a polyol method. The structure and composition of the resultant composite were characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM) and energy dispersive spectroscopy (EDS) techniques. We found that the size of the Fe₃O₄ nanoparticles supported on the MCNT could be easily controlled by changing the mass ratio of the Fe₃O₄ precursor to the MCNT. By a subsequent polyol process, 3% (w) Pd was loaded onto a Fe₃O₄-MCNT composite to form Pd/Fe₃O₄-MCNT magnetic catalysts. The results from magnetic measurements indicated that the prepared composites before and after Pd loading possess superparamagnetic characteristics at room temperature. The prepared Pd/Fe₃O₄-MCNT catalysts were evaluated by the selective hydrogenation of cinnamaldehyde as a probe reaction and it showed high activity toward the conversion of cinnamaldehyde to hydrocinnamaldehyde. Under a magnetic field, the catalyst powder was easily separated from the liquid-phase reaction system. The catalyst did not show any significant degradation after four cycles indicating the good recyclability of the prepared composite catalyst.

Key words: Multi-walled carbon nanotubes, Magnetic composite catalyst, Polyol method, Cinnamaldehyde, Selective hydrogenation

徐玲, 沈晓旭, 肖强, 钟依均, 叶素芳, 叶向荣, 朱伟东. Pd/Fe₃O₄-MCNT磁性催化剂的制备、表征及催化性能[J]. 物理化学学报, 2011, 27(08), 1956-1960. doi: 10.3866/PKU.WHXB20110721

XU Ling, SHEN Xiao-Xu, XIAO Qiang, ZHONG Yi-Jun, YE Su-Fang, YE Xiang-Rong, ZHU Wei-Dong. Preparation, Characterization and Catalytic Properties of Pd/Fe₃O₄-MCNT Magnetically Recyclable Catalysts[J]. Acta Phys. -Chim. Sin. 2011, 27(08), 1956-1960. doi: 10.3866/PKU.WHXB20110721

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB20110721

https://www.whxb.pku.edu.cn/CN/Y2011/V27/I08/1956

参考文献

(1) Iijima, S. Nature 1991, 354, 56.
(2) Wang, M.W.; Li, F. Y.; Peng, N. C. New Carbon Mater. 2002, 17, 75. [王敏炜, 李凤仪, 彭年才. 新型炭材料, 2002, 17, 75.]
(3) Planeix, J. M.; Coustel, N.; Coq, B.; Brotons, V.; Kumbhar, P. S.; Dutartre, R.; Geneste, P.; Bernier, P.; Ajayan, P. M. J. Am. Chem. Soc. 1994, 116, 7935.
(4) Tessonnier, J. P.; Pesant, L.; Ehret, G.; Ledoux, M. J.; Pham-Huu, C. Appl. Catal. A 2005, 288, 203.
(5) Plomp, A. J.; Vuori, H.; Krause, A. O. I.; de Jong, K. P.; Bitter, J. H. Appl. Catal. A 2008, 351, 9.
(6) Xu, X. Z.; Yang, J. F.; Li, X. N.; Yan, X. H. Acta Phys. -Chim. Sin. 2008, 24, 121. [许兴中, 杨建锋, 李小年, 严新焕. 物理化学学报, 2008, 24, 121.]
(7) Yoon, B.; Pan, H. B.;Wai, C. M. J. Phys. Chem. C 2009, 113, 1521.
(8) Chen, X. C.; Hou, Y. Q.;Wang, H.; Cao, Y.; He, J. H. J. Phys. Chem. C 2008, 112, 8176.
(9) Zhu, J.; Zhao, T. J.; Kvande, I.; Chen, D.; Zhou, X. G.; Yuan,W. K. Chin. J. Catal. 2008, 29, 1145. [朱俊, 赵铁均, Kvande, I., 陈德, 周兴贵, 袁渭康. 催化学报, 2008, 29, 1145.]
(10) Utsumi, S.; Urita, K.; Kanoh, H.; Yudasaka, M.; Suenaga, K.; Iijima, S.; Kaneko, K. J. Phys. Chem. B 2006, 110, 7165.
(11) Grzelczak, M.; Correa-Duarte, M. A.; Salgueirino-Maceira, V.; Rodriguez-Gonzalez, B.; Rivas, J.; Liz-Marzan, L. M. Angew. Chem. Int. Edit. 2007, 46, 7026.
(12) Wu, H. Q.; Xu, D. M.;Wang, Q.;Wang, Q. Y.; Su, G. Q.;Wei, X.W. J. Alloy. Compd. 2008, 463, 78.
(13) Cao, H. Q.; Zhu, M. F.; Li, Y. G.; Liu, J. H.; Ni, Z.; Qin, Z. Y. J. Solid State Chem. 2007, 180, 3218.
(14) Zhang, H.; Du, N.;Wu, P.; Chen, B. D.; Yang, D. R. Nanotechnology 2008, 19, 315604.
(15) Qiu, H. X.;Wang, Z. Y.; Shi, Z. J.; Gu, Z. N.; Qiu, J. S. Acta Phys. -Chim. Sin. 2007, 23, 1451. [邱汉迅, 王志永, 施祖进, 顾镇南, 邱介山. 物理化学学报, 2007, 23, 1451.]
(16) Su, X. Z.; Xiao, D. S; Zhou. G. Y. Mater. Rev. 2009, 23, 82. [苏秀芝, 肖定寿, 周国玉. 材料导报, 2009, 23, 82.]
(17) Sun, Z. Y.; Liu, Z. M.;Wang, Y.; Han, B. X.; Du, J. M.; Zhang, J. L. J. Mater. Chem. 2005, 15, 4497.
(18) Zhao, D. L.; Zeng, X.W.; Shen, Z. M. Synthesis of Magnetic Carbon Nanotube Composites Coated with Nanosized Ferriferous Oxide. CN Patent 1 791 780.A, 2007-05-30. [赵东林, 曾宪伟, 沈曾明. 纳米四氧化三铁包覆碳纳米管磁性复合材料的制备方法: 中国, CN1 791 780.A[P]. 2007-05-30.]
(19) Li, Y. G.; Zhang, Q.;Wang, H. Z.; Zhu, M. F.; Zhang, Q. H. Synthesis of Magnetic Ferriferous Oxide/Multiwalled Carbon Nanotube Composites. CN Patent 101 320 607.A, 2008-12-10. [李耀刚, 张祺, 王宏志, 朱美芳, 张青红. 四氧化三铁/多壁碳纳米管磁性纳米复合材料的制备方法: 中国, CN101 320 607.A[P]. 2008-12-10.]
(20) Cao, H. Q.; Zhu, M. F.; Li, Y. G. J. Solid State Chem. 2006, 179, 1208.
(21) Zhu, H.; Lin, H. Y.; Guo, H. F.; Yu, L. F. Mater. Sci. Eng. B 2007, 138, 101.
(22) Cheng, G. F.; Zhao, J.; Tu, Y. H.; He, P. G.; Fang, Y. Z. Anal. Chim. Acta 2005, 533, 11.
(23) Qu, S.;Wang, J.; Kong, J. L.; Yang, P. Y.; Chen, G. Talanta 2007, 71, 1096.
(24) Jin, J.; Li, R.;Wang, H. L.; Chen, H. N.; Liang, K.; Ma, J. T. Chem. Commun. 2007, No. 4, 386.
(25) Xiong, Z. H.;Wang, L.; Zhou, J. G.; Liu, J. M. Acta Phys. -Chim. Sin. 2010, 26, 2890. [熊振湖, 王璐, 周建国, 刘建明. 物理化学学报, 2010, 26, 2890.]
(26) Guo, D. B.; Yang, L. F.; Zhang, G. Q.; Fang, R. Q.; Cai, J. X. J. Fujian Forestry Sci. Tech. 2006, 33, 25. [郭德波, 杨乐夫, 张国强, 方荣谦, 蔡俊修. 福建林业科技, 2006, 33, 25.]
(27) Wan, J. Q.; Cai,W.; Feng, J. T.; Meng, X. X.; Liu, E. Z. J. Mater. Chem. 2007, 17, 1188.

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Pd/Fe₃O₄-MCNT磁性催化剂的制备、表征及催化性能

Preparation, Characterization and Catalytic Properties of Pd/Fe₃O₄-MCNT Magnetically Recyclable Catalysts

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