H2在Al7-团簇解离吸附的理论研究

李文杰; 杨慧慧; 陈宏善

doi:10.7498/aps.62.053601

摘要

利用高精度从头计算方法研究了H2分子在Al7-阴离子团簇上的吸附及解离过程, 确定了分子吸附及解离吸附的稳定结构,并分析了各结构的光电子能谱. 计算表明H2在Al7-上为弱的物理吸附,吸附能约为0.02 eV;解离过程的能垒约为0.75 eV. 对团簇及解离吸附结构的态密度与实验得到的光电子能谱的比较表明二者能够很好地符合, 确定H2与激光烧蚀产生的团簇直接反应时能在Al7-上发生解离.

关键词:

Al7- /
H2 /
解离吸附 /
从头计算

With the accurate ab initio method, the adsorption and dissociation process of H2 molecule on Al7- cluster anion are investigated. The stable structures of molecular adsorption and dissociative adsorption are confirmed. The photoelectron spectra of different structures are further analyzed. The calculations indicate that the adsorption of H2 on Al7- is weak physical adsorption with the adsorption energy about 0.02 eV. The investigation of the dissociation process shows that the energy barrier of dissociation is about 0.75 eV. The densities of states of the Al7- cluster and the dissociative adsorption complex Al7H2- are in good agreement with those obtained by the photoelectron spectroscopy. It suggests that H2 can be dissociated when it is absorbed on Al7- anions produced by laser ablation.

Keywords:

作者及机构信息

1.
西北师范大学物理与电子工程学院,甘肃省原子分子物理与功能材料重点实验室, 兰州 730070

基金项目: 国家自然科学基金(批准号: 11164024)和西北师范大学科技创新工程 (批准号: NWNU-KJCXGC03-62)资助的课题.

Authors and contacts

1.
College of Physics and Electronic Engineering, Northwest Normal University, Key Laboratory of Atomic and Molecular Physics & Functional Materials of Gansu Province, Lanzhou 730070, China

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 11164024), and the Northwest Normal University (Grant No. NWNU-KJCXGC03-62).

参考文献

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[9]	Kodama T, Gokon N 2007 Chem. Rev. 107 4048
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[25]	Kawamura H, Kumar V, Sun Q, Kawazoe Y 2001 Phys. Rev. B 65 045406
[26]	Pino I, Kroes G J, van Hemert M C 2010 J. Chem. Phys. 133 184304
[27]	Cui L F, Li X, Wang L S 2006 J. Chem. Phys. 124 054308
[28]	Becke A D 1993 J. Chem. Phys. 98 5648
[29]	McDouall J J, Peasley K, Robb M A 1988 Chem. Phys. Lett. 148 183
[30]	Pople J A, Head-Gordon M, Raghavachari K 1987 J. Chem. Phys. 87 5968
[31]	Frisch M J, Trucks G W, Schlegel H B 2004 Gaussian 03. Revision E.01. Wallingford CT: Gaussian Inc.
[32]	Sun J, Lu W C, Wang H, Li Z S, Sun C C 2006 J. Phys. Chem. A 110 2729
[33]	Chen M X, Yan X H 2007 Chemical Physics Letters 439 270
[34]	Rao B K, Jena P 1999 J. Chem. Phys. 111 1890
[35]	Harrington J E, Weisshaar J C 1990 J. Chem. Phys. 93 854
[36]	Fu Zh W, Lemire G W, Bishea G A, Morse M D 1990 J. Chem. Phys. 93 8420

施引文献

[1]	Lubitz W, Tumas W 2007 Chem. Rev. 107 3900
[2]	Zhou J J, Chen Y G, Wu Z L, Zhen X, Fang Y C, Gao T 2009 Acta Phys. Sin. 58 4853 (in Chinese) [周晶晶, 陈云贵, 吴朝玲, 郑欣, 房玉超, 高涛 2009 58 4853]
[3]	Borup R, Meyers J, Pivovar B, Kim Y S, Mukundan R, Garland N 2007 Chem. Rev. 107 3904
[4]	Jayashree R S, Mitchell M, Natarajan D, Markoski L J, Kenis P J A 2007 Langmuir 23 6871
[5]	Palo D R, Dagle R A, Holladay J D 2007 Chem. Rev. 107 3992
[6]	Navarro R M, Peña M A, Fierro J L G 2007 Chem. Rev. 107 3952
[7]	Cortright R D, Davda R R, Dumesic J A 2002 Nature 418 964
[8]	Esswein A J, Nocera D G 2007 Chem. Rev. 107 4022
[9]	Kodama T, Gokon N 2007 Chem. Rev. 107 4048
[10]	Nocera D G 2012 Accounts of Chemical Research 45 767
[11]	Yilanci A, Dincer I, Ozturk H K 2009 Progress in Energy and Combustion Science 35 231
[12]	Mandal T K, Gregory D H 2009 Annu. Rep. Prog. Chem., Sect. A 105 21
[13]	Schlapbach L, Zttel A 2001 Nature 414 353
[14]	Eberle U, Felderhoff M, Schth F 2009 Angew. Chem. Int. Ed. 48 6608
[15]	Dai W, Luo J S, Tang Y J, Wang Z Y, Chen S J, Sun W G 2009 Acta Phys. Sin. 58 1890 (in Chinese) [戴伟, 罗江山, 唐永建, 王朝阳, 陈善俊, 孙卫国 2009 58 1890]
[16]	Struzhkin V V, Militzer B, Mao W L, Mao Ho-k, Hemley R J 2007 Chem. Rev. 107 4133
[17]	Rowsell J L C, Yaghi O M 2005 Angew. Chem. Int. Ed. 44 4670
[18]	Orimo S, Nakamori Y, Eliseo J R, Zttel A, Jensen C M 2007 Chem. Rev. 107 4111
[19]	Ye J Y, Liu Y L, Wang J L, He Y 2010 Acta Phys. Sin. 59 4178 (in Chinese) [叶佳宇, 刘亚丽, 王靖林, 何垚 2010 59 4178]
[20]	Zhang H, Qi K Z, Zhang G Y, Wu D, Zhu S L 2009 Acta Phys. Sin. 58 8077 (in Chinese) [张辉, 戚克振, 张国英, 吴迪, 朱圣龙 2009 58 8077]
[21]	Ruan W, Xie An-D, Yu X G, Wu D L 2011 Chin. Phys. B 20 043104
[22]	Cox D M, Trevor D J, Whetten R L, Rohlfing E A, Kaldor A 1986 J. Chem. Phys. 84 4651
[23]	Cox D M, Trevor D J, Whetten R L, Kaldor A 1988 J. Phys. Chem. 92 421
[24]	Upton T H 1986 Phys. Rev. Lett. 56 2168
[25]	Kawamura H, Kumar V, Sun Q, Kawazoe Y 2001 Phys. Rev. B 65 045406
[26]	Pino I, Kroes G J, van Hemert M C 2010 J. Chem. Phys. 133 184304
[27]	Cui L F, Li X, Wang L S 2006 J. Chem. Phys. 124 054308
[28]	Becke A D 1993 J. Chem. Phys. 98 5648
[29]	McDouall J J, Peasley K, Robb M A 1988 Chem. Phys. Lett. 148 183
[30]	Pople J A, Head-Gordon M, Raghavachari K 1987 J. Chem. Phys. 87 5968
[31]	Frisch M J, Trucks G W, Schlegel H B 2004 Gaussian 03. Revision E.01. Wallingford CT: Gaussian Inc.
[32]	Sun J, Lu W C, Wang H, Li Z S, Sun C C 2006 J. Phys. Chem. A 110 2729
[33]	Chen M X, Yan X H 2007 Chemical Physics Letters 439 270
[34]	Rao B K, Jena P 1999 J. Chem. Phys. 111 1890
[35]	Harrington J E, Weisshaar J C 1990 J. Chem. Phys. 93 854
[36]	Fu Zh W, Lemire G W, Bishea G A, Morse M D 1990 J. Chem. Phys. 93 8420

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