物理化学学报 >> 2002, Vol. 18 >> Issue (08): 692-698.doi: 10.3866/PKU.WHXB20020805

研究论文 上一篇    下一篇

氢气在碳纳米管基材料上的吸附-脱附特性

周振华;武小满;王毅;林国栋;张鸿斌   

  1. 厦门大学化学化工学院,固体表面物理化学国家重点实验室,厦门 361005
  • 收稿日期:2001-12-19 修回日期:2002-02-28 发布日期:2002-08-15
  • 通讯作者: 张鸿斌 E-mail:hbzhang@xmu.edu.cn

Characteristics of Adsorption and Desorption of Hydrogen on Multi-walled Carbon Nanotubes

Zhou Zhen-Hua;Wu Xiao-Man;Wang Yi;Lin Guo-Dong;Zhang Hong-Bin   

  1. College of Chemistry and Chemical Engineering, State Key Laboratory of Physical Chemistry for the Solid Surfaces, Xiamen University, Xiamen 361005
  • Received:2001-12-19 Revised:2002-02-28 Published:2002-08-15
  • Contact: Zhang Hong-Bin E-mail:hbzhang@xmu.edu.cn

摘要: 利用高压容积法测定多壁碳纳米管(MWCNTs)及钾盐修饰的相应体系(K+-MWCNTs)的储氢容量,并用程序升温脱附(TPD)方法表征研究氢气在MWCNTs基材料上的吸附-脱附特性.结果表明,在经纯化MWCNTs上,室温、9.0 MPa实验条件下氢的储量可达1.51%(质量分数);K+盐对MWCNTs的修饰对增加其储氢容量并无促进效应,但相应化学吸附氢物种的脱附温度有所升高;K+的修饰也改变了MWCNTs表面原有的疏水性质.在低于723 K的温度下,H2/MWCNTs体系的脱附产物几乎全为氢气;773 K以上高温脱附产物不仅含H2,也含有CH4、C2H4、C2H2等C1/C2烃混合物;H2/K+-MWCNTs储氢试样的脱附产物除占主体量的H2及少量C1/C2烃混合物外,还含水汽,其量与吸附质H2源水汽含量密切相关.H2在碳纳米管基材料上吸附兼具非解离 (即分子态) 和解离(即原子态)两种形式.

关键词: 多壁碳纳米管, 碳纳米管基储氢材料, 氢吸附-脱附特性, H2-TPD

Abstract: Storage capacities of H2 in a kind of multi-walled carbon nanotubes (MWCNTs) and its corresponding system modified with K+ salt were measured using volumetric method, and characteristics of adsorption and desorption of hydrogen on MWCNTs were studied by means of temperature-programmed desorption (TPD) method. The results showed that the storage capacities of H2 in the purified MWCNTs could reach 1.51% (mass fraction) under condition of room temperature and 9.0 MPa, with adsorption of ~99% of the H2 being reversible. A comparative study indicated that the modification of the K+ salt to the MWCNTs did not improve its storage capacity of hydrogen, but led to elevating of desorption temperature of adsorbed hydrogen H2(a) to a certain extent; in addition, the K+ modification resulted also in changing of surface property of the MWCNTs from original hydrophobicity to hydrophilicity. The products desorbed on H2/MWCNTs involved exclusively H2 at T≤ 723 K, and main part of H2 and small amount of CH4,C2H4,and C2H2 at T ≥ 773 K; whereas on H2/K+-MWCNTs,H2O was also involved in the desorbed products, in addition to H2 and small amount of C1/C2-hydrocarbons.The adsorption of H2 on the MWCNTs-based materials is in the two models: associative (molecular state) and dissociative (atomic state).

Key words: Multi-walled carbon nanotubes, MWCNTs-based H2-storage material, Adsorption-desorption characteristics of H2, H2-TPD