催化学报 ›› 2008, Vol. 29 ›› Issue (11): 1138-1144.

• 研究论文 • 上一篇    下一篇

MgO负载Fe基催化剂选择性合成单/双/多壁碳纳米管

张强, 赵梦强, 黄佳琦, 骞伟中, 魏飞   

  1. 清华大学化学工程系绿色反应工程与工艺北京市重点实验室, 北京 100084
  • 收稿日期:2008-11-25 出版日期:2008-11-25 发布日期:2012-08-17

Selective Synthesis of Single/Double/Multi-walled Carbon Nanotubes on MgO-Supported Fe Catalyst

ZHANG Qiang, ZHAO Mengqiang, HUANG Jiaqi, QIAN Weizhong, WEI Fei*   

  1. Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing 100084, China
  • Received:2008-11-25 Online:2008-11-25 Published:2012-08-17

摘要: 通过浸渍及水热处理获得MgO负载的Fe基催化剂,并将其用于化学气相沉积过程裂解甲烷获得碳纳米管. 结果表明,单/双/多壁碳纳米管可选择性地生长在Fe负载量不同的Fe/MgO催化剂上. 当Fe负载量仅为0.5%时,铁原子在载体表面烧结为0.8~1.2 nm的铁颗粒,碳在这种小颗粒上以表面扩散为主,导致单壁碳纳米管形成,并且单壁碳纳米管的选择性高达90%. 当Fe负载量提高到3%时,铁原子聚集成约2.0 nm的颗粒,在化学气相沉积中生长碳纳米管时,碳在Fe催化剂颗粒中的体相扩散的贡献增大,在表相扩散和体相扩散的共同作用下,双壁碳纳米管的选择性显著增高. 当进一步增加Fe负载量时,铁原子烧结形成1~8 nm的颗粒,经过化学气相沉积,在催化剂上生长了单、双、多壁碳纳米管. 随着Fe在MgO载体上负载量的增加,管径、管壁数以及半导体管的含量都增加. 本研究提供了一种适合大批量选择性生长单/双/多壁碳纳米管的方法.

关键词: 碳纳米管, 化学气相沉积, 铁, 氧化镁, 负载型催化剂, 微结构, 拉曼光谱

Abstract: Single/double/multi-walled carbon nanotubes (S/D/MWCNTs) were selectively syn the sized on a MgO-supported iron catalyst by chemical vapor deposition from methan e . The selectivities for SWCNTs and DWCNTs on 0.5%Fe/MgO and 3.0%Fe/MgO were over 90 % and 75%, respectively. This provides a controlled way to selectively synthesiz e CNTs on a large scale in a fluidized bed.

Key words: carbon nanotube, chemical vapor deposition, iron, magnesia, supported catalyst, mirostructure, Raman spectroscopy