流化床-化学气相沉积法制备CNT/Fe-Ni/ TiO2及其光催化性能研究

doi:10.3724/SP.J.1077.2012.00033

无机材料学报 ›› 2012, Vol. 27 ›› Issue (1): 33-38.DOI: 10.3724/SP.J.1077.2012.00033

流化床-化学气相沉积法制备CNT/Fe-Ni/ TiO₂及其光催化性能研究

马磊, 陈爱平, 陆金东, 何洪波, 李春忠

(华东理工大学材料科学与工程学院, 超细材料制备与应用教育部重点实验室上海 200237)

收稿日期:2011-05-05 修回日期:2011-07-03 出版日期:2012-01-09 网络出版日期:2011-12-19
作者简介:马磊(1984-), 男, 博士研究生. E-mail: ecrolham@sina.com.cn
基金资助:
上海市科委纳米专项(1052nm02400);国家自然科学基金(20925621)

Synthesis and Photocatalytic Properties of CNT/Fe-Ni/TiO₂ by Fluidized Bed-chemical Vapor Deposition Method

MA Lei, CHEN Ai-Ping, LU Jin-Dong, HE Hong-Bo, LI Chun-Zhong

(Key Laboratory for Ultrafine Materials of Ministry of Education, School of Materials Science and Engineering, East China University of Science and Technology, Shanghai 200237, China)

Received:2011-05-05 Revised:2011-07-03 Published:2012-01-09 Online:2011-12-19
Supported by:
Nanotechnology Special Projects of Science and Technology Commission of Shanghai Municipality (1052nm02400);National Natural Science Foundation of China (20925621)

摘要/Abstract

摘要：

以Fe-Ni/TiO₂为催化剂, 采用流化床化学气相沉积法(FBCVD)在TiO₂表面原位生长碳纳米管(CNT), 得到CNT/Fe-Ni/ TiO₂复合光催化剂. 通过SEM、XRD、UV-Vis等方法表征其结构和性能, 以亚甲基蓝溶液降解为模型考察其光催化性能. 结果表明: Fe-Ni/TiO₂催化剂在FBCVD过程中, 镍主要起到了CNT生长催化活性位的作用; 在生长CNT后的复合光催化剂中, 比例较低的Fe³⁺主要作为电子俘获剂, 抑制TiO₂光生电子空穴的复合; Ni和CNT共同起到将电子迅速地从TiO₂中导出, 从而降低光生电子-空穴复合几率的作用. 三者的协同作用显著改善了TiO₂的光催化性能. 其中Fe和Ni掺杂量分别为0.25mol%和4.75mol%样品的光催化活性较高, 生长CNT后得到的复合光催化剂对亚甲基蓝的降解效率较纯TiO₂提高约70%.

关键词: 过渡金属, TiO₂, 光催化, 流化床, CNT

Abstract:

Fe-Ni/TiO₂ was used as catalyst to synthesize carbon nanotube(CNT)/Fe-Ni/TiO₂ composite photocatalyst by fluidized bed chemical vapor deposition (FBCVD) method. Carbon nanotube grew in situ on TiO₂ surface. The CNT/Fe-Ni/TiO₂composite photocatalyst were characterized by X-ray diffraction (XRD), UV-Vis absorption spectroscope and field emission scanning electron microscope (FESEM). The photocatalytic activities of prepared samples were investigated by the photodegradation of methylene blue (MB). The results showed that Ni was characterized as catalytic center for CNT growth in FBCVD process. In CNT/Fe-Ni/TiO₂ composite photocatalyst, Fe (III) cation was characterized as an electron capture center and efficiently promoted the separation of photogenerated holes and electrons. The electron transfer from TiO₂ was facilitated by Ni particles and CNTs, which could reduce the electron - hole recombination. The synergistic effects of Fe-Ni and CNT significantly enhanced the photocatalytic activity of the catalysts. The degradation ratio of MB of CNT/Fe-Ni/TiO₂ doped with 0.25mol% Fe and 4.75mol% Ni was increased about 70% than that of pure TiO₂.

Key words: transition metal, TiO₂, photocatalysis, fluidized bed, CNT

中图分类号:

TB383

马磊, 陈爱平, 陆金东, 何洪波, 李春忠. 流化床-化学气相沉积法制备CNT/Fe-Ni/ TiO₂及其光催化性能研究[J]. 无机材料学报, 2012, 27(1): 33-38.

MA Lei, CHEN Ai-Ping, LU Jin-Dong, HE Hong-Bo, LI Chun-Zhong. Synthesis and Photocatalytic Properties of CNT/Fe-Ni/TiO₂ by Fluidized Bed-chemical Vapor Deposition Method[J]. Journal of Inorganic Materials, 2012, 27(1): 33-38.

图/表 5

图1 Fe-Ni/TiO2和CNT/Fe-Ni/TiO2 的XRD图谱

Fig. 1 XRD patterns of Fe-Ni/TiO2 and CNT/Fe-Ni/TiO2

图2 CNT/Fe-Ni/TiO2的FESEM照片

Fig. 2 FESEM images of CNT/Fe-Ni/TiO2

图3 样品的紫外-可见吸收光谱

Fig. 3 UV-Vis absorption spectra of the samples

图4 不同样品的亚甲基蓝降解曲线

Fig. 4 Photocatalytic degradation of different sample on methylene blue

图5 Fe-Ni/TiO2催化剂FBCVD生长CNT后的光催化作用机理图

Fig. 5 Mechanism for the synergistic effects after growing CNT

参考文献 17

[1]	ZHAO Yin, LI Chun-Zhong, LIU Xiu-Hong, et al. Photosensitized degradation activity of dye by Fe-doped TiO2 nanocrystals synthesize via gas combustion flames. Journal of Inorganic Materials, 2007, 22(6): 1070-1074.
[2]	YU Xiang-Yang, CHENG Ji-Jian. Photocatalytic activities of iron and chromium ion doped TiO2 films. Journal of Inorganic Materials, 2001, 16(4): 742-764.
[3]	LIU Shao-You, WU Lin-Dong, ZHAO Zhong-Xing, et al. Synthesis of Ni-doped TiO2 mesoporous material via solid-state reaction at low temperature and its kinetics of methyl orange photodegradation. Journal of Inorganic Materials, 2009, 24(5): 902-908.
[4]	Choi W, Termin A, Hoffmann M R. The role of metal ion dopants in quantum-sized TiO2: correlation between photoreactivity and charge carrier recombination dynamics. J. Phys. Chem., 1994, 98(51): 13669-13679.
[5]	Zhang jinlong, Wu Yongmei, Xiao Ling, et al. Properties of carbon and iron modified TiO2 photocatalyst synthesized at low temperature and photo degradation of acid orange 7 under visible light. Applied Surface Science, 2010, 256(13): 4260-4268.
[6]	Garun Narungsun, Worapon Kiatkittipong, Hiroshi Yamada, et al. Hydroxylation of benzene to phenol on Fe /TiO2 catalysts loaded with different types of second metal. Catalysis Communications, 2008, 9(9): 1886-1890.
[7]	Wei Fei, Wang Yao, Luo Guohua, et al. The large-scale production of carbon nanotubes in a nano-agglomerate fluidized-bed reactor. Chemical Physics Letters, 2002, 364(10): 568-572.
[8]	Jung Minjae, Kwang Yong Eun, Jong Wan Park, et al. Growth of carbon nanotubes by chemical vapor deposition. Diamond and Related Materials, 2001, 10(3-7): 1235-1240.
[9]	Yao Yuan, Li Gonghu, Shannon Ciston, et al. Photoreactive TiO2/carbon nanotube composites: synthesis and reactivity. Environmental Science &Technology, 2008, 42(13): 4952-4957.
[10]	Gao Bin, George Z Chen, Li Gianluca. Carbon nanotubes/ titanium dioxide (CNTs/TiO2) nanocomposites prepared by conventional and novel surfactant wrapping Sol-Gel methods exhibiting enhanced photocatalytic activity. Applied Catalysis B: Environmental, 2009, 89(3/4): 503-509.
[11]	Wang C Y, Bottcher C, Bahnemann D W, et al. A comparative study of nanometer sized Fe(III)-doped TiO2 photocatalysts: synthesis, characterization and activity. J. Mater. Chem., 2003, 13(9): 2322-2329.
[12]	Zhu Jiefang, Zheng Wei, He Bin, et al. Characterization of Fe-TiO2 photocatalysts synthesized by hydrothermal method and their photocatalytic reactivity for photodegradation of XRG dye diluted in water. Journal of Molecular Catalysis, 2004, 216(1): 35-43.
[13]	吴玉琪, 吕功煊, 李树本, 等(WU Yu-Qi, et al). TiO2表面NiO光催化活性中心的构建及其光催化析氢性能研究. 无机化学学报(Chinese Journal of Inorganic Chemistry), 2010, 26(3): 476-482.
[14]	Yao Na, Chen Jixiang, Zhang Jianxiang, et al. Influence of support calcination temperature on properties of Ni/TiO2 for catalytic hydrogenation of ochloronitrobenzene to ochloroaniline. Catalysis Communications, 2008, 9(6): 1510-1516.
[15]	Zhou Minghua, Yu Jiaguo, Chen Bei, et al. Effects of Fe-doping on the photocatalytic activity of mesoporous TiO2 powders prepared by an ultrasonic method. Journal of Hazardous Materials, 2006, 137(3): 1838-1847.
[16]	Nur Azimah Jamalluddin, Ahmad Zuhairi Abdullah. Reactive dye degradation by combined Fe (III)/TiO2 catalyst and ultrasonic irradiation: effect of Fe(III) loading and calcination temperature. Ultrasonics Sonochemistry, 2011, 18(2): 669-678.
[17]	Zhang Kan, Meng Zeda, Wonchun OH. Degradation of rhodamine B by Fe-carbon nanotubes/TiO2 composites under UV light in aerated solution. Chinese Journal of Catalysis, 2010, 31(7): 751-758.

流化床-化学气相沉积法制备CNT/Fe-Ni/ TiO₂及其光催化性能研究

Synthesis and Photocatalytic Properties of CNT/Fe-Ni/TiO₂ by Fluidized Bed-chemical Vapor Deposition Method

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