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OALib Journal期刊
ISSN: 2333-9721
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Pb(II)水合结构的密度泛函及分子动力学研究
DOI: 10.6023/A13040368, PP. 1307-1312
Keywords: Pb(II),水合结构,密度泛函理论,第一性原理分子动力学,态密度
Abstract:
水溶液中Pb(II)的水合结构缺乏实验数据,成键机理尚不明确.采用密度泛函理论、周期性边界计算水合物种Pb(H2O)1~92+的低能构象,探讨其结合能和稳定性,结合该离子在水溶液中的第一性原理分子动力学弛豫行为和扩展X射线吸收精细结构(EXAFS)谱特征,确定其最佳稳定构型和水合数,并通过Mulliken电荷布居、分波态密度及差分电荷密度分析其成键机理.低能优化结果表明,水合数6,7和8的构象均有可能存在,动力学弛豫过程Pb(II)的第一和第二水合层不存在明显分界,其优势构型的水合数为6,属于偏半方位构型.Pb(H2O)62+中Pb—O键的离子性较强,成键机理主要为Pb6p6d轨道与Pb6s-O2p反键态轨道进行耦合,存在反键态电子填充,表现为原子间电子密度的减少.
| [1] | Markus, J.; McBratney, A. B. Environ. Int. 2001, 27, 399.
|
| [2] | Loef, M.; Mendoza, L. F.; Walach, H. Toxin Rev. 2011, 30(4), 103.
|
| [3] | Olympio, K. P. K.; Goncalves, C.; Günther, W. M. R.; Bechara, E. J. H. Rev. Panam. Salud Publica/Pan. Am. J. Public Health 2009, 26(3), 266.
|
| [4] | Unuabonah, E. I.; Olu-Owolabi, B. I.; Oladoja, A. N.; Ofomaja, A. E.; Yang, Z. L. J. Soil. Sediment. 2010, 10, 1103.
|
| [5] | Zhang, D.; Hou, P. Acta Chim. Sinica 2009, 67(12), 1336. (张东, 侯平, 化学学报, 2009, 67(12), 1336.)
|
| [6] | Jiang, M. Q.; Wang, Q. P.; Jin, X. Y.; Chen, Z. L. J. Hazard. Mater. 2009, 170, 332.
|
| [7] | Parr, J. Polyhedron 1997, 16(4), 551.
|
| [8] | Shimoni-Livny, L.; Glusker, J. P.; Bock, C. W. Inorg. Chem. 1998, 37, 1853.
|
| [9] | Gourlaouen, C.; Gerard, H.; Piquemal, J.-P.; Parisel, O. Chem. Eur. J. 2008, 14, 2730.
|
| [10] | Swift, T. J.; Sayre, W. G. J. Chem. Phys. 1966, 44(9), 3567.
|
| [11] | Marcus, Y. J. Chem. Soc. Faraday Trans. 1991, 87, 2995.
|
| [12] | Hofer, T. S.; Rode, B. M. J. Chem. Phys. 2004, 121, 6406.
|
| [13] | Persson, I.; Lyczko, K.; Lundberg, D.; Eriksson, L.; Placzek, A. Inorg. Chem. 2011, 50, 1058.
|
| [14] | Hofer, T. S.; Randolf, B. R.; Rode, B. M. Chem. Phys. 2006, 323, 473.
|
| [15] | Gourlaouen, C.; Gerard, H.; Parisel, O. Chem. Eur. J. 2006, 12, 5024.
|
| [16] | Wander, M. C. F.; Clark, A. E. Inorg. Chem. 2008, 47, 8233.
|
| [17] | Bhattacharjee, A.; Hofer, T. S.; Pribil, A. B.; Randolf, B. R.; Lim, L. H. V.; Lichtenberger, A. F.; Rode, B. M. J. Phys. Chem. B 2009, 113, 13007.
|
| [18] | Li, F. M.S. Thesis. Hebei University of Technology, Tianjin, 2011. (李非, 硕士论文, 河北工业大学, 天津, 2011.)
|
| [19] | Sun, W.; Chen, Z.; Huang, S. Y. J. Wuhan Univ. Tech. 2005, 27(7), 26. (孙炜, 陈中, 黄素逸, 武汉理工大学学报, 2005, 27(7), 26.)
|
| [20] | Ji, Q.; Yang, X. Z. Chemistry Online 2005, 2, 111. (吉青, 杨小震, 化学通报, 2005, 2, 111.)
|
| [21] | Mulliken, R. S. J. Chem. Phys. 1955, 23, 1833.
|
| [22] | Mudring, A. V.; Rieger, F. Inorg. Chem. 2005, 44, 6240.
|
| [23] | Mudring, A. V. Eur. J. Inorg. Chem. 2007, 2007(6), 882.
|
| [24] | Walsh, A.; Watson, G. W. J. Solid State Chem. 2005, 178, 1422.
|
| [25] | Materials Studio 4. 3. San Diego, CA, Accelrys Inc., 2008.
|
| [26] | Clark, S. J.; Segall, M. D.; Pickard, C. J.; Hasnip, P. J.; Probert, M. J.; Refson, K. Z. Kristallogr. 2005, 220, 567.
|
| [27] | Hohenberg, P.; Kohn, W. Phys. Rev. 1964, 136(3B), B864.
|
| [28] | Kohn, W.; Sham, L. J. Phys. Rev. 1965, 140(4A), A1133.
|
| [29] | Perdew, J. P.; Burke, K.; Ernzerhof, M. Phys. Rev. Lett. 1996, 77, 3865.
|
| [30] | Vanderbilt, D. Phys. Rev. B 1990, 41(11), 7892.
|
| [31] | Pfrommer, B. G.; Cote, M.; Louie, S. G.; Cohen, M. L. J. Comput. Phys. 1997, 131, 233.
|
| [32] | Monkhorst, H. J.; Pack, J. D. Phys. Rev. B 1976, 13(12), 5188.
|
| [33] | Rappe, A. K.; Colwell, K. S.; Casewit, C. J. Inorg. Chem. 1993, 32, 3438.
|
| [34] | Casewit, C. J.; Colwell, K. S.; Rappe, A. K. J. Am. Chem. Soc. 1992, 114, 10046.
|
| [35] | Jorgensen, W. L.; Chandrasekhar, J.; Madura, J. D.; Impey, R. W.; Klein, M. L. J. Chem. Phys. 1983, 79, 926.
|
| [36] | Rappe, A. K.; Goddard, W. A. J. Phys. Chem. 1991, 95(8), 3358.
|
| [37] | Karasawa, N.; Goddard, W. A. Macromolecules 1992, 25, 7268.
|
| [38] | Ewald, P. P. Ann. Phys. 1921, 64, 253.
|
| [39] | Nose, S. Mol. Phys. 1984, 52, 255.
|
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