物理化学学报 >> 2012, Vol. 28 >> Issue (08): 1854-1860.doi: 10.3866/PKU.WHXB201205151

理论与计算化学 上一篇    下一篇

B12Sc4和B12Ti4团簇的储氢性质

马丽娟, 王剑锋, 贾建峰, 武海顺   

  1. 山西师范大学化学与材料科学学院, 山西 临汾 041004
  • 收稿日期:2012-01-15 修回日期:2012-05-14 发布日期:2012-07-10
  • 通讯作者: 贾建峰 E-mail:jjf_sxtu@yahoo.com.cn
  • 基金资助:

    973计划前期研究专项课题(2010CB635110)与山西省自然科学基金(2010011012-2)资助项目

Hydrogen Storage Properties of B12Sc4 and B12Ti4 Clusters

MA Li-Juan, WANG Jian-Feng, JIA Jian-feng, WU Hai-Shun   

  1. School of Chemistry and Materials Science, Shanxi Normal University, Linfen 041004, Shanxi Province, P. R. China
  • Received:2012-01-15 Revised:2012-05-14 Published:2012-07-10
  • Contact: JIA Jian-feng E-mail:jjf_sxtu@yahoo.com.cn
  • Supported by:

    This work was supported by the National Basic Research 973 Pre-research Progr?am of China (2010CB635110) and Nature Science Foundation of Shanxi Province, China (2010011012-2).

摘要:

提出了两个稳定的团簇B12Sc4和B12Ti4, 基于理论计算, 研究了它们的结构与储氢性质. 结果发现, 在这两个稳定的团簇中, 过渡金属原子不会聚合在一起而影响它们对氢气的吸附. B12Sc4最多可以吸附12个氢分子, 达到7.25% (质量分数)的储氢量. 它的平均每氢分子吸附能量为10.5 kJ·mol-1. B12Ti4最多只能吸附8个氢分子, 储氢量为4.78%. 但平均每氢分子吸附能量可达50.2 kJ·mol-1. 进一步计算表明, 即使在77 K,也需要很高的氢气压力才能使12个氢分子都吸附到B12Sc4上. 电子结构分析表明, B12Ti4-nH2吸附结构中的Kubas作用要大于相应B12Sc4-nH2结构中的Kubas作用.

关键词: 硼团簇, 金属掺杂, 储氢, 吸附, 从头算

Abstract:

The structures and hydrogen storage properties of two stable B12Sc4 and B12Ti4 clusters have been investigated using ab initio calculations. No metal atom clustering occurs in the clusters. The B12Sc4 hosts 12 H2 to achieve 7.25% (mass fraction) hydrogen storage capacity with an average binding energy (ABE) of -10.4 kJ·mol-1 per H2, while the B12Ti4 can only host 8 H2 (4.78%, mass fraction) with a higher ABE (-50.2 kJ·mol-1 per H2). High hydrogen pressure is needed for B12Sc4 to hold 12 H2, even at 77 K. Electronic structure analysis indicates that the Kubas interaction in the B12Ti4-nH2 complex is much stronger than that in the B12Sc4-nH2 complex.

Key words: Boron cluster, Metal doped, Hydrogen storage, Adsorption, Ab initio calculation

MSC2000: 

  • O641