超临界干燥法制备催化剂合成单壁纳米碳管及表征

无机材料学报

超临界干燥法制备催化剂合成单壁纳米碳管及表征

罗君航^1,2; 张孝彬^1,2; 李昱¹; 程继鹏¹; 刘芙¹

1. 浙江大学材料物理与微结构所; 2. 硅材料国家重点实验室, 杭州 310027

收稿日期:2004-10-21 修回日期:2004-12-15 出版日期:2005-11-20 网络出版日期:2005-11-20

Synthesis and Characterization of Single-walled Carbon Nanotubes Using Catalysts Prepared by The Supercritical Drying Method

LUO Jun-Hang^1,2; ZHANG Xiao-Bin^1,2; LI Yu¹; CHEN Ji-Peng¹; LIU Fu¹

1. Material Physics and Microstructure Institute; 2. State Key Laboratory of Silicon Materials; Zhejiang University; Hangzhou 310027, China

Received:2004-10-21 Revised:2004-12-15 Published:2005-11-20 Online:2005-11-20

摘要/Abstract

摘要： 采用超临界干燥法制备了活性高、比表面大的Fe/Mo/Al₂O₃催化剂.通过超临界干燥,催化剂的比表面由294m²/g提高到401m²/g.在1000℃下用该催化剂催化裂解甲烷, 合成了大产量、高质量的单壁纳米碳管(SWNTs).利用SEM、TEM、HRTEM、TGA 和Raman等手段对所制备的SWNTs进行了表征.结果表明:超临界法制备催化剂合成的粗产品中SWNTs含量在30%以上,大大高于同一配方催化剂采用常规干燥法的产率(约2%); SWNTs的管径分布在0.8-1.0nm之间,其形态以束状为主.

关键词: 超临界干燥法, 单壁纳米碳管, 化学气相沉积, TEM

Abstract: The highly active Fe/Mo/Al2O3 catalyst with the large specific surface area was prepared by the supercritical drying method. The BET specific surface area of the as-prepared catalyst was increased from 294m2/g to 401m2/g. High quality single-walled carbon nanotubes (SWNTs) were synthesized by catalytic decomposition of CH4/H2 at 1000℃ using the catalyst. SEM, TEM, HRTEM, TGA and Raman spectroscopy were used to characterize the SWNTs. The content of SWNTs in the product propared is over 30wt%, which is much higher than that by using the conventional drying method, i.e. 2wt%. The mean diameter of the as-prepared SWNTs is in 0.8-1.0nm and they are usually bundles.

Key words: supercritical drying method, single-walled carbon nanotubes, chemical vapor deposition, TEM

中图分类号:

O613
TQ426

罗君航,张孝彬,李昱,程继鹏,刘芙. 超临界干燥法制备催化剂合成单壁纳米碳管及表征[J]. 无机材料学报.

LUO Jun-Hang,ZHANG Xiao-Bin,LI Yu,CHEN Ji-Peng,LIU Fu. Synthesis and Characterization of Single-walled Carbon Nanotubes Using Catalysts Prepared by The Supercritical Drying Method[J]. Journal of Inorganic Materials.

参考文献

[1] Iijima S, Ichihashi T. Nature, 1993, 363 (6430): 603-605.
[2] Salvetat J P, Briggs G A D, Bonard J M, et al. Phys. Rev. Lett., 1999, 82 (5): 944-947.
[3] de Pablo P J, Martinez M T, Colchero J, et al. Mat. Sci. Eng. C, 2001, 15 (1-2): 149-151.
[4] Dillon A C, Jones K M, Bekkedahi T A, et al. Nature, 1997, 386 (6623): 377-379.
[5] Stanisalus S W, Emesto J, Adam T W, et al. Nature, 1998, 394 (6688): 52-55.
[6] Yahachi S, Sashiro U. Carbon, 2000, 38 (2): 169-182.
[7] Kong J, Franklin N R, Zhou C W, et al. Science, 2000, 287 (5453): 622-625.
[8] 钟蓉, 丛洪涛, 成会明, 等. 材料研究学报, 2002, 16 (4): 344-348.
[9] Journet C, Maser W K, Berner P, et al. Nature, 1997, 388 (6644): 756-758
[10] Thess A, Lee R, Nikolaev P, et al. Science, 1996, 273 (5274): 483-487.
[11] Dai H J, Rinzler A G, Nikalaev P. Chem. Phys. Lett., 1996, 260 (3-4): 471-475.
[12] Hafner J H, Bronikowski M J, Azamian B R, et al. Chem. Phys. Lett., 1998, 296 (1-2): 195-202.
[13] Kong J, Cassell A M, Dai H J. Chem. Phys. Lett., 1998, 292 (4-6): 567-574.
[14] Cassell A M, Raymakers J A, Kong J. J. Phys. Chem., B, 1999, 103 (31): 6484-6492.
[15] Li Q W, Hao Y, Li X H, et al. Chem. Mater, 2002, 14 (10): 4262-4266.
[16] Heley J R, Jackson D, James P F. Journal of Non-Crystalline Solids, 1995, 186: 30-36.
[17] Novak Z, Knez Z, Drofenik M, et al. Journal of Non-Crystalline Solids[J], 2001, 285: 44-49.
[18] Kitiyanan B, Alvarez W E, Harwell J H, et al. Chem. Phys. Lett., 2000, 317 (3-5): 497-503.
[19] Ruoff R S, Tersoff J, Lorents D C, et al. Nature, 1993, 364 (6437): 514-516.
[20] Rao A M, Richter E, Bandow S, et al. Science, 1997, 275 (5297): 187-191.
[21] Alvarez L, Righi A, Guillard T, et al. Chem. Phys. Lett., 2000, 316 (3-4): 186-190.
[22] 相宏伟, 钟炳, 彭少逸, 等. 材料科学与工程, 1995, 13 (2): 38-42.