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

[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

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

[1]	董肖. P掺杂LiNH₂团簇与LiH反应机理的密度泛函理论研究及一种新储放氢机制. , 2023, 72(15): 153101. doi: 10.7498/aps.72.20230374
[2]	祁鹏堂, 陈宏善. Li修饰的C24团簇的储氢性能. , 2015, 64(23): 238102. doi: 10.7498/aps.64.238102
[3]	唐春梅, 王成杰, 高凤志, 张轶杰, 徐燕, 巩江峰. 碳硼富勒烯衍生物C18B2M(M=Li, Ti, Fe)的储氢性能计算研究. , 2015, 64(9): 096103. doi: 10.7498/aps.64.096103
[4]	梁昌慧, 张小安, 李耀宗, 赵永涛, 梅策香, 周贤明, 肖国青. 不同电荷态的129Xeq+激发Au的X射线发射研究. , 2015, 64(5): 053201. doi: 10.7498/aps.64.053201
[5]	郑圆圆, 任桂明, 陈锐, 王兴明, 谌晓洪, 王玲, 袁丽, 黄晓凤. 氢化铁的自旋极化效应及势能函数. , 2014, 63(21): 213101. doi: 10.7498/aps.63.213101
[6]	阮文, 罗文浪, 余晓光, 谢安东, 伍冬兰. 锂原子修饰B6团簇的储氢性能研究. , 2013, 62(5): 053103. doi: 10.7498/aps.62.053103
[7]	张辉, 肖明珠, 张国英, 路广霞, 朱圣龙. 基于密度泛函理论解读不同高密度储氢材料释氢能力. , 2011, 60(2): 026103. doi: 10.7498/aps.60.026103
[8]	卢其亮, 罗其全, 陈莉莉. C@Al12团簇吸附H的密度泛函理论研究. , 2010, 59(1): 234-238. doi: 10.7498/aps.59.234
[9]	冯选旗, 冯雪红, 姜振益. 关于AlnC和AlnC+(n=1—8)团簇结构和稳定性的研究. , 2010, 59(11): 7838-7844. doi: 10.7498/aps.59.7838
[10]	葛桂贤, 曹海滨, 井群, 罗有华. 密度泛函理论研究H2与Rhn（n=1—8）团簇的相互作用. , 2009, 58(12): 8236-8242. doi: 10.7498/aps.58.8236
[11]	葛桂贤, 杨增强, 曹海滨. 密度泛函理论研究CO与Nin（n=1—6）团簇的相互作用. , 2009, 58(9): 6128-6133. doi: 10.7498/aps.58.6128
[12]	柏于杰, 付石友, 邓开明, 唐春梅, 陈宣, 谭伟石, 刘玉真, 黄德财. 密度泛函理论计算内掺氢分子富勒烯H2＠C60及其二聚体的几何结构和电子结构. , 2008, 57(6): 3684-3689. doi: 10.7498/aps.57.3684
[13]	雷雪玲, 祝恒江, 葛桂贤, 王先明, 罗有华. 密度泛函理论研究BnNi(n=6—12)团簇的结构和磁性. , 2008, 57(9): 5491-5499. doi: 10.7498/aps.57.5491
[14]	陈琨, 范广涵, 章勇. Mn掺杂ZnO光学特性的第一性原理计算. , 2008, 57(2): 1054-1060. doi: 10.7498/aps.57.1054
[15]	陈琨, 范广涵, 章勇, 丁少锋. In-N共掺杂ZnO第一性原理计算. , 2008, 57(5): 3138-3147. doi: 10.7498/aps.57.3138
[16]	王清林, 葛桂贤, 赵文杰, 雷雪玲, 闫玉丽, 杨致, 罗有华. 密度泛函理论对CoBen(n=1—12)团簇结构和性质的研究. , 2007, 56(6): 3219-3226. doi: 10.7498/aps.56.3219
[17]	赵文杰, 杨致, 闫玉丽, 雷雪玲, 葛桂贤, 王清林, 罗有华. 密度泛函理论计算GenFe(n=1—8)团簇的基态结构及其磁性. , 2007, 56(5): 2596-2602. doi: 10.7498/aps.56.2596
[18]	何开华, 郑广, 吕涛, 陈刚, 姬广富. 高压对氮化硼纳米管的几何结构、电子结构和光学性质的影响. , 2006, 55(6): 2908-2913. doi: 10.7498/aps.55.2908
[19]	李恩玲, 王雪雯, 陈贵灿, 马红, 薛英. GanN－m阴离子团簇的结构及稳定性的研究. , 2006, 55(5): 2249-2256. doi: 10.7498/aps.55.2249
[20]	易双萍, 张海燕, 欧阳玉, 王银海, 庞晋山. 真空热处理碳纳米管的储氢性能研究. , 2006, 55(5): 2644-2650. doi: 10.7498/aps.55.2644

计量

文章访问数: 6409
PDF下载量: 461
被引次数: 0

姓名
邮箱
手机号码
标题
留言内容
验证码

搜索

留言板