Mg原子修饰的封闭型六硼烷B6H62-储氢性质的研究

卢其亮; 黄守国; 李宜德

doi:10.7498/aps.62.213601

摘要

利用密度泛函理论的方法研究了Mg原子修饰的封闭型六硼烷B6H62-吸附氢的性能. Mg可以稳定地结合在B6H62-上, 它可以吸附六个氢分子. 电荷转移所导致的Mg周围电场的增强和体系更大的偶极矩使得MgB6H62-比MgB6H6具有更好的储氢性能, 储氢密度达到11.1 wt%, 氢分子的平均结合能在0.23 eV/H2至0.34 eV/H2之间. 结果表明可以通过控制金属-有机物体系的电荷态来增强电场, 进而改善其储氢性能.

关键词:

Abstract

Hydrogen storage capacity of Mg-decorated closo-hexaborate B6H62- has been studied using density functional theory. The binding strength of Mg atom is sufficiently large to ensure the stability of MgB6H62-. Each Mg atom can adsorb six H2 molecules. Moreover, the larger dipole moment combined with enhanced electrostatic field around the Mg atom originates from the charge transfer from B6H62- to Mg, accounting for the higher adsorption capacity of MgB6H62- than that of MgB6H6. Hydrogen storage capacity of MgB6H62- can be up to 11.1 wt% with an average binding energy between 0.23 eV and 0.34 eV. The electrostatic field around the Mg atom can be enhanced by controlling the charge state of the metal-organic complex, thereby significantly improving the hydrogen adsorption capacity.

Keywords:

作者及机构信息

1.
安徽大学物理与材料科学学院, 合肥 230601

基金项目: 安徽省自然科学基金 (批准号: 090414186)、安徽省教育厅自然科学基金重点项目 (批准号: KJ2010A029)和安徽大学211工程学术创新团队项目资助的课题.

Authors and contacts

1.
School of Physics and Material Science, Anhui University, Hefei 230601, China

Funds: Project supported by the Natural Science Foundation of Anhui Province, China (Grant No. 090414186), the Key Research Project of Natural Science Foundation of Anhui Provincial Universities, China (Grant No. KJ2010A029), and the 211 Project of Anhui University.

参考文献

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[29]	Delley B 1990 J. Chem. Phys. 92 508
[30]	Perdew J P, Burke K, Ernzerhof M, 1996 Phys. Rev. Lett. 77 3865
[31]	Perdew J P, Wang Y 1992 Phys. Rev. B 45 13244
[32]	Kalvoda S, Paulus B, Dolg M, Stoll H, Werner H J 2001 Phys. Chem. Chem. Phys. 3 514
[33]	Lide D R 2000 CRC Handbook of Chemistry and Physics (CRC Press: New York)
[34]	Kim Y H, Zhao Y F, Williamson, Heben M J, Zhang S B 2006 Phys. Rev. Lett. 96 016102
[35]	Sun Q, Wang Q, Jena P, Kawazoe Y 2005 J. Am. Chem. Soc. 127 14582
[36]	Krasnov P O, Ding F, Singh A K, Yakobson B I 2007 J. Phys. Chem. C 111 17977

施引文献

[1]	Orimo S, Nakamori Y, Eliseo J R, Zttel A, Jensen C M 2007 Chem. Rev. 107 4111
[2]	Hamilton C W, Baker R T, Staubitz A, Manners I 2009 Chem. Soc. Rev. 38 279
[3]	Struzhkin V V, Militzer B, Mao W L, Mao H K, Hemley R J 2007 Chem. Rev. 107 4133
[4]	van den Berg A W C, Areán C O 2008 Chem. Commun. 6 668
[5]	Weber J, Antonietti M, Thomas A 2008 Macromolecules 41 2880
[6]	Rosi N L, Eckert J, Eddaoudi M, Vodak D T, Kim J, O’Keeffe M, Yaghi O M 2003 Science 300 1127
[7]	Rowsell J L C, Yaghi O M 2005 Angew. Chem. Int. Ed. 44 4670
[8]	Fichtner M 2005 Adv. Eng. Mater. 7 443
[9]	Andrievski R A 2007 Phys. Usp. 50 691
[10]	Bhihia M, Lakhala M, Labrimb H, Benyoussef A, El Kenza A, Mounkachic O, Hlil E K 2012 Chin. Phys. B 21 097501
[11]	Ruan W, Xie A D, Yu X G, Wu D L 2011 Chin. Phys. B 20 116801
[12]	Han S S, Goddard W A 2007 J. Am. Chem. Soc. 129 8422
[13]	Zhao Y F, Kim Y H, Dillon A C, Heben M J, Zhang S B 2005 Phys. Rev Lett. 94 155504
[14]	Sun Q, Wang Q, Jena P 2005 Nano Lett. 5 1273
[15]	Li H, Ihm J, Cohen M L, Louie S G 2010 Nano Lett. 10 793
[16]	Sun Q, Jena P, Wang Q, Marquez M 2006 J. Am. Chem. Soc. 128 9741
[17]	Yoon M, Yang S Y, Hicke C, Wang E G, Geohegan D, Zhang Z Y 2008 Phys. Rev. Lett. 100 206806
[18]	Zhao Y F, Lusk M T, Dillon A C, Heben M J, Zhang S B 2008 Nano Lett. 8 157
[19]	Chandrakumar K R S, Ghosh S 2008 Nano Lett. 8 13
[20]	Lan J H, Cao D P, Wang W C 2009 ACS Nano 3 3294
[21]	Li M, Li Y, Zhou Z, Shen P, Chen Z 2009 Nano Lett. 9 1944
[22]	Li J L, Hu Z S, Yang G W 2012 Chem. Phys. 392 16
[23]	Gopalsamy K, Prakash M, Kumar R M, Subramanian V 2012 Int. J. Hydrogen Energy 37 9730
[24]	Wu G, Wang J, Zhang X, Zhu L 2009 J. Phys. Chem. C 113 7052
[25]	Zhang Y, Zheng X, Zhang S, Huang S, Wang P, Tian H 2012 Int. J. Hydrogen Energy 7 12411
[26]	Huang H S, Wang X M, Zhao D Q, Wu L F, Huang X W, Li Y C 2012 Acta Phys. Sin. 61 073101 (in Chinese) [黄海深, 王小满, 赵东秋, 伍良福, 黄晓伟, 李蕴才 2012 61 073101]
[27]	Ruan W, Luo W L, Yu X, Xie A D, Wu D L 2013 Acta Phys. Sin. 62 053103 (in Chinese) [阮文, 罗文浪, 余晓光, 谢安东, 伍冬兰 2013 62 053103]
[28]	Zhao Y C, Dai Z H, Sui P F, Zhang X L 2013 Acta Phys. Sin. 62 137301 (in Chinese) [赵银昌, 戴振宏, 隋鹏飞, 张晓玲 2013 62 137301]
[29]	Delley B 1990 J. Chem. Phys. 92 508
[30]	Perdew J P, Burke K, Ernzerhof M, 1996 Phys. Rev. Lett. 77 3865
[31]	Perdew J P, Wang Y 1992 Phys. Rev. B 45 13244
[32]	Kalvoda S, Paulus B, Dolg M, Stoll H, Werner H J 2001 Phys. Chem. Chem. Phys. 3 514
[33]	Lide D R 2000 CRC Handbook of Chemistry and Physics (CRC Press: New York)
[34]	Kim Y H, Zhao Y F, Williamson, Heben M J, Zhang S B 2006 Phys. Rev. Lett. 96 016102
[35]	Sun Q, Wang Q, Jena P, Kawazoe Y 2005 J. Am. Chem. Soc. 127 14582
[36]	Krasnov P O, Ding F, Singh A K, Yakobson B I 2007 J. Phys. Chem. C 111 17977

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