Sr2+和Ba2+水分子体系结构和结合能的从头算和ABEEM/MM研究

doi:10.3866/PKU.WHXB20110233

物理化学学报 >> 2011, Vol. 27 >> Issue (02): 379-387.doi: 10.3866/PKU.WHXB20110233

Sr²⁺和Ba²⁺水分子体系结构和结合能的从头算和ABEEM/MM研究

刘燕¹, 王芳芳^1,2, 于春阳¹, 刘翠¹, 宫利东¹, 杨忠志¹

1. 辽宁师范大学化学化工学院, 辽宁大连 116029;
2. 济南大学化学化工学院, 济南 250022

收稿日期:2010-10-07 修回日期:2010-12-02 发布日期:2011-01-25
通讯作者: 宫利东 E-mail:gongjw@lnnu.edu.cn
基金资助:
国家自然科学基金(20633050, 20703022, 21011120087)和辽宁省教育厅基金(2009T057)资助项目

Structures and Binding Energies of Sr²⁺/Ba²⁺-Water Systems by Ab initio and ABEEM/MM Method

LIU Yan¹, WANG Fang-Fang^1,2, YU Chun-Yang¹, LIU Cui¹, Gong Li-Dong¹, YANG Zhong-Zhi¹

1. School of Chemistry and Chemical Engineering, Liaoning Normal University, Dalian 116029, Liaoning Province, P. R. China;
2. School of Chemistry and Chemical Engineering, University of Jinan, Jinan 250022, P. R. China

Received:2010-10-07 Revised:2010-12-02 Published:2011-01-25
Contact: Gong Li-Dong E-mail:gongjw@lnnu.edu.cn
Supported by:
The project was supported by the National Natural Science Foundation of China (20633050, 20703022, 21011120087) and Foundation of Education Bureau of Liaoning Province, China (2009T057).

摘要/Abstract

摘要：

应用从头算方法和ABEEM/MM浮动电荷分子力场, 研究了水合碱土离子团簇Sr²⁺/Ba²⁺(H₂O)_n (n=1-6), 构建了离子-水相互作用的ABEEM/MM势能函数, 获得了水合离子团簇的稳定结构, 计算了结合能. 计算结果表明, ABEEM/MM方法的结果和从头算方法的结果有很好的一致性. 进一步应用ABEEM/MM对Sr²⁺和Ba²⁺水溶液进行了分子动力学模拟. 对Sr²⁺水溶液, 得到的Sr²⁺-水中氧原子的径向分布函数的第一和第二最高峰分别位于0.257和0.464 nm处, 第一和第二水合层的配位水分子数分别为9.2和11.4; 对Ba²⁺水溶液, 得到的Ba²⁺与水中氧原子的径向分布函数的第一和第二最高峰分别位于0.269和0.467 nm处, 第一和第二水合层的配位水分子数分别为9.9和12.4. 这与实验值或其它理论模拟结果有较好的一致性. 对比外层的水分子, 金属离子的极化作用使得溶液中第一水合层中水分子的O―H键长增长, HOH键角减小.

关键词: 水合金属离子团簇, 离子溶剂化, 从头算方法, ABEEM/MM浮动电荷分子力场, 相互作用能

Abstract:

Hydrated clusters of Sr²⁺/Ba²⁺(H₂O)_n (n=1-6) were investigated by the ab initio method and the ABEEM/MM fluctuating charge molecular force field. ABEEM/MM potential functions of cation-water interactions were constructed based on the stable structures and binding energies of the hydrated clusters were obtained. The results from ABEEM/MM are consistent with those from the ab initio method. Furthermore, Sr²⁺ and Ba²⁺ aqueous solutions were studied by ABEEM/MM molecular dynamic simulations. Results show that for the Sr²⁺ aqueous solution the first and second peaks of the SrO radial distribution function (RDF) are located at 0.257 and 0.464 nm, respectively. The coordination numbers of the water molecules for the first and second hydration shells are 9.2 and 11.4, respectively. For the Ba²⁺ aqueous solution, the first and second peaks of the BaO RDF are located at 0.269 and 0.467 nm, respectively. The coordination numbers of water molecules for the first and second hydration shells are 9.9 and 12.4, respectively. These results also show good consistency with experimental observations and other theoretical simulations. Compared with the external water molecules, the water molecules in the first hydration shell are evidently polarized by the cation and their O―H bond lengths are stretched while the HOH bond angles are found to be reduced.

Key words: Hydrated metal cation cluster, Ion solvation, Ab initio method, ABEEM/MM fluctuating charge molecular force field, Interaction energy

刘燕, 王芳芳, 于春阳, 刘翠, 宫利东, 杨忠志. Sr²⁺和Ba²⁺水分子体系结构和结合能的从头算和ABEEM/MM研究[J]. 物理化学学报, 2011, 27(02), 379-387. doi: 10.3866/PKU.WHXB20110233

LIU Yan, WANG Fang-Fang, YU Chun-Yang, LIU Cui, Gong Li-Dong, YANG Zhong-Zhi. Structures and Binding Energies of Sr²⁺/Ba²⁺-Water Systems by Ab initio and ABEEM/MM Method[J]. Acta Phys. -Chim. Sin. 2011, 27(02), 379-387. doi: 10.3866/PKU.WHXB20110233

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB20110233

https://www.whxb.pku.edu.cn/CN/Y2011/V27/I02/379

参考文献

(1) Shimamura, T.; Weyand, S.; Beckstein, O.; Rutherford, N. G.; Hadden, J. M.; Sharples, D.; Sansom, M. S. P.; Iwata, S.; Henderson, P. J. F.; Cameron A. D. Science 2010, 328, 470.
(2) Ohtaki, H.; Radnai, T. Chem. Rev. 1993, 93, 1157.
(3) Richens, D. T. The Chemistry of Aqua Ions; John Wiley & Sons: New York, 1997.
(4) Vinogradov, E. V.; Smirnov, P. R.; Trostin, V. N. Russ. Chem. Bull. 2003, 52, 1.
(5) Liang, X. Y.; Campopiano, D. J.; Sadler, P. J. Chem. Soc. Rev. 2007, 36, 968.
(6) Marcus, Y. Chem. Rev. 2009, 109, 1346.
(7) Kankia, B. I.; Marky, L. A. J. Am. Chem. Soc. 2001, 123, 10799.
(8) Dunbar, R. C.; Steill, J. D.; Polfer, N. C.; Oomens, J. J. Phys. Chem. B 2009, 113, 10552.
(9) Shao, H. B.; Wang, X. Y.; Wang, J. M.; Wang, J. B.; Zhang, J. Q.; Cao, C. N. Acta Phys. -Chim. Sin. 2006, 22, 312.
[邵海波, 王晓艳, 王建明, 王俊波, 张鉴清, 曹楚南. 物理化学学报, 2006, 22, 312.]
(10) Rode, B. M.; Hofer, T. S. Pure Appl. Chem, 2006, 78, 525.
(11) Masia, M. J. Chem. Phys. 2008, 128, 184107.
(12) Jorgenson, W. L. J. Chem. Theory Comput. 2007, 3, 1877.
(13) Wang, Z. X.; Zhang, W.; Wu, C.; Lei, H.; Cieplak, P.; Duan, Y. J. Comput. Chem. 2006, 27, 781.
(14) Lamureux, G.; Roux, B. J. Chem. Phys. 2003, 119, 3025.
(15) Xie, W.; Pu, J.; MacKerell, A. D., Jr.; Gao, J. L. J. Chem. Theory Comput. 2007, 3, 1878.
(16) Jorgenson, W. L.; Jensen, K. P.; Alexandrova, A. N. J. Chem. Theory Comput. 2007, 3, 1987.
(17) Schnieders, M. J.; Ponder, J. W. J. Chem. Theory Comput. 2007, 3, 2083.
(18) Holt, A.; Karlström, G. J. Comput. Chem. 2008, 29, 1084.
(19) Holt, A.; Karlström, G. J. Comput. Chem. 2008, 29, 2033.
(20) Anisimov, V. M.; Vorobyov, I. V.; Roux, B.; MacKerell, A. D., Jr. J. Chem. Theory Comput. 2007, 3, 1927.
(21) Banks, J. L.; Kaminski, G. A.; Zhou, R.; Mainz, D. T.; Berne, B. J.; Friesner, R. A. J. Chem. Phys. 1999, 110, 741.
(22) Chelli, R.; Procacci, P. J. Chem. Phys. 2002, 117, 9175.
(23) Patel, S.; Brooks, C. L., III. J. Comput. Chem. 2004, 25, 1.
(24) Yang, Z. Z.; Wu, Y.; Zhao, D. X. J. Chem. Phys. 2004, 120, 2541.
(25) Mortier, W. J.; Ghosh, S. K.; Shankar, S. J. Am. Chem. Soc. 1986, 108, 4315.
(26) York, D. M.; Yang, W. T. J. Chem. Phys. 1996, 104, 159.
(27) Lopes, P. E. M.; MacKerell, A. D., Jr.; Roux, B. Theor. Chem. Acc. 2009, 124, 11.
(28) Grossfield, A.; Ren, P. Y.; Ponder, J. W. J. Am. Chem. Soc. 2003, 125, 15671.
(29) Lamoureux, G.; Roux, B. J. Phys. Chem. B 2006, 110, 3308.
(30) Warren, G. L.; Patel, S. J. Phys. Chem. B 2008, 112, 11679.
(31) Masia, M.; Probst, M. J. Chem. Phys. 2005, 123, 164505.
(32) Piquemal, J. P.; Perera, L.; Cisneros, G. A.; Ren, P. Y.; Pedersen, L. G.; Darden, T. A. J. Chem. Phys. 2006, 125, 054511.
(33) Jungwirth, P.; Tobias, T. J. Chem. Rev. 2006, 106, 159.
(34) D′Angleo, P.; Pavel, N. V.; Roccatano, D. Phys. Rev. B 1996, 54, 12129.
(35) Persson, I.; Sandstr?m, M.; Yokoyama, H.; Chaudhry, M. Z. Naturforsch. A 1995, 50, 21.
(36) Hofer, T. S.; Rode, B. M.; Randolf, B. R. Chem. Phys. 2005, 312, 81.
(37) Han, Y. K.; Jeong, Y. K. J. Phys. Chem. 1996, 100, 18004.
(38) Peschke, M.; Blades, A. T.; Kebarle, P. J. Phys. Chem. A 1998, 102, 9978.
(39) Rodriguez-Cruz, S. E.; Jockusch, R. A.; Williams, E. R. J. Am. Chem. Soc. 1999, 121, 8898.
(40) Harris, D. J.; Brodholt, J. P.; Sherman, D. M. J. Phys. Chem. B 2003, 107, 9056.
(41) Yang, Z. Z.; Wang, C. S. J. Phys. Chem. A 1997, 101, 6315.
(42) Wang, C. S.; Yang, Z. Z. J. Chem. Phys. 1999, 110, 6189.
(43) Wu, Y.; Yang, Z. Z. J. Phys. Chem. A 2004, 108, 7563.
(44) Yang, Z. Z.; Ye, Y. J.; Tang, A. Q. Quantum Chemistry of Macromolecular Systems, 2nd ed.; Jilin University Press: Changchun, 2005; pp 215-294.
[杨忠志, 叶元杰, 唐敖庆. 大分子体系的量子化学(第二版). 长春: 吉林大学出版社, 2005: 215-294.]
(45) Yang, Z. Z.; Li, X. J. Phys. Chem. A 2005, 109, 3517.
(46) Li, X.; Yang, Z. Z. J. Phys. Chem. A 2005, 109, 4102.
(47) Li, X.; Yang, Z. Z. J. Chem. Phys. 2005, 122, 084514.
(48) Yang, Z. Z.; Li, X. J. Chem. Phys. 2005, 123, 094507.
(49) Yang, Z. Z.; Zhang, Q. J. Comput. Chem. 2006, 27, 1.
(50) Li, X.; Gong, L. D.; Yang, Z. Z. Sci. China Ser. B-Chem. 2008, 51, 1221.
(51) Cui, B. Q.; Gong, L. D.; Zhao, D. X. Acta Phys. -Chim. Sin. 2008, 24, 1035.
[崔宝秋, 宫利东, 赵东霞. 物理化学学报, 2008, 24, 1035.]
(52) Wang, F. F.; Zhao, D. X.; Gong, L. D. Theor. Chem. Acc. 2009, 124, 139.
(53) Zhao, D. X.; Liu, C.; Wang, F. F.; Yu, C. Y.; Gong, L. D.; Liu, S. B.; Yang, Z. Z. J. Chem. Theory Comput. 2010, 6, 795.
(54) Frisch, M. J.; Trucks, G. W.; Schlegel, H. B.; et al. Gaussian 03, Revision D.01; Gaussian Inc.: Wallingford, CT, 2004.
(55) Berendsen, H. J. C.; Postma, J. P. M.; van Gunsteren, W. F.; DiNola, A.; Haak, J. R. J. Phys. Chem. 1984, 81, 3684.
(56) Hockney, R. W. Method Comput. Phys. 1970, 9, 136.
(57) CRC Handbook of Chemistry and Physics, 84th ed.; Lide, D. R. Ed. CRC Press: Boca Raton, 2003-2004.

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Sr²⁺和Ba²⁺水分子体系结构和结合能的从头算和ABEEM/MM研究

Structures and Binding Energies of Sr²⁺/Ba²⁺-Water Systems by Ab initio and ABEEM/MM Method

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