水溶液中碳酸铀酰化合物的电子结构

doi:10.3866/PKU.WHXB201201171

Abstract

Abstract: A systematic study of series of non-hydrated and hydrated Cn/m uranyl carbonate complexes (n is number of carbonate ligands, and m is number of water molecules) in the aqueous phase was carried out using relativistic density functional theory. The conductor-like screening model was used to calculate solvent effects. The zeroth-order regular approximation was used to account for scalar relativistic effects and spin-orbit coupling relativistic effects. Time-dependent density functional theory with the inclusion of spin-orbit coupling relativistic effects was used to calculate electronic transitions using the statistically averaged orbital potentials. The results indicate that carbonate ligands play an important role in the geometric and electronic transition properties of the complex. The stability of the C3/0 carbonate complex in the aqueous phase may be attributed to the involvement of 5f components in the highest occupied bonding orbital. The addition of carbonate ligands caused a blue shift in the maximum wavelength and high intensity absorptions in the near visible region.

Key words: Uranyl, UV-Vis, Solvent effect, Time-dependent density functional theory, Spin-orbit coupling relativistic effect

MSC2000:

O641

GU Jia-Fang, LU Chun-Hai, CHEN Wen-Kai, CHEN Yong, XU Ke, HUANG Xin, ZHANG Yong-Fan. Electronic Structures of Uranyl(VI) Carbonate Complexes in the Aqueous Phase[J].Acta Phys. -Chim. Sin., 2012, 28(04): 792-798.

References

(1) Clark, D. L.; Hobart, D. E.; Neu, M. P. Chem. Rev. 1995, 95, 25.

(2) Meinrath, G. J. Radioanal. Nucl. Chem. 1996, 211, 349.

(3) Nguyen Trung, C.; Begun, G. M.; Palmer, D. A. Inorg. Chem. 1992, 31, 5280.

(4) McGlynn, S. P.; Smith, J. K.; Neely,W. C. J. Chem. Phys. 1961, 35, 105.

(5) de Jong,W. A.; Aprà, E.;Windus, T. L.; Nichols, J. A.; Harrison, R. J.; Gutowski, K. E.; Dixon, D. A. J. Phys. Chem. A 2005, 109, 11568.

(6) Gu, J. F.; Lu, C. H.; Chen,W. K.; Xu, Y.; Zheng, J. D. Acta Phys. -Chim. Sin. 2009, 25, 655. [辜家芳, 陆春海, 陈文凯, 许莹, 郑金德. 物理化学学报, 2009, 25, 655.]
(7) Allen, P. G.; Bucher, J. J.; Clark, D. L.; Edelstein, N. M.; Ekberg, S. A.; Gohdes, J.W.; Hudson, E. A.; Kaltsoyannis, N.; Lukens,W.W. Inorg. Chem. 1995, 34, 4797.

(8) Docrat, T. I.; Mosselmans, J. F.W.; Charnock, J. M.; Whiteley, M.W.; Collison, D.; Livens, F. R.; Jones, C.; Edmiston, M. J. Inorg. Chem. 1999, 38, 1879.

(9) Su, J.; Li, J. Prog. Chem. 2011, 23, 1329. [苏静, 李隽. 化学进展, 2011, 23, 1329.]
(10) Wang, D. Q.; Gunsteren,W. F. v. Prog. Chem. 2011, 23, 1566. [王东琪, Gunsteren,W. F. v. 化学进展, 2011, 23, 1566.]
(11) Hu, H. S.;Wu, G. S.; Li, J. J. Nucl. Radiochem. 2009, 31, 25. [胡憾石, 吴国是, 李隽. 核化学与放射化学, 2009, 31, 25.]
(12) Liu,W. J. Prog. Chem. 2007, 19, 833. [刘文剑. 化学进展, 2007, 19, 833.]
(13) Cinnéide, S. ó.; Scanlan, J. P.; Hynes, M. J. J. Inorg. Nucl. Chem. 1975, 37, 1013.

(14) Scanlan, J. P. J. Inorg. Nucl. Chem. 1977, 39, 635.

(15) Su, J.; Zhang, K.; Schwarz,W. H. E.; Li, J. Inorg. Chem. 2011, 50, 2082.

(16) Matsika, S.; Pitzer, R. M.; Reed, D. T. J. Phys. Chem. A 2000, 104, 11983.

(17) Kaltsoyannis, N.; Hay, P. J.; Li, J.; Blaudeau, J. P.; Bursten, B. E. Theoretical Studies of the Electronic Structure of Compounds of the Actinide Elements. In The Chemistry of the Actinide and Transactinide Elements; Morss, L. R., Edelstein, N. M., Fuger, J., Eds.; Springer: Netherlands, 2006; p 1893.

(18) de Jong,W. A.; Harrison, R. J.; Nichols, J. A.; Dixon, D. A. Theor. Chem. Acc. 2001, 107, 22.

(19) ADF2010, SCM, Theoretical Chemistry; Vrije Universiteit: Amsterdam, The Netherlands; http://www.scm.com.
(20) Guerra, C. F.; Snijders, J. G.; Velde, G. T.; Baerends, E. J. Theor. Chem. Acc. 1998, 99, 391.
(21) Velde, G. T.; Bickelhaupt, F. M.; Baerends, E. J.; Guerra, C. F.; van Gisbergen, S. J. A.; Snijders, J. G.; Ziegler, T. J. Comput. Chem. 2001, 22, 931.

(22) Perdew, J. P.; Burke, K.; Ernzerhof, M. Phys. Rev. Lett. 1996, 77, 3865.

(23) van Lenthe, E.; Baerends, E. J. J. Comput. Chem. 2003, 24, 1142.

(24) van Lenthe, E.; Ehlers, A. E.; Baerends, E. J. J. Chem. Phys. 1999, 110, 8943.

(25) van Lenthe, E.; Baerends, E. J.; Snijders, J. G. J. Chem. Phys. 1994, 101, 9783.

(26) van Lenthe, E.; Baerends, E. J.; Snijders, J. G. J. Chem. Phys. 1993, 99, 4597.

(27) Lee, B.; Richards, F. M. J. Mol. Biol. 1971, 55, 379.

(28) Richards, F. M. Annu. Rev. Biophys. Bioeng. 1977, 6, 151.

(29) Perdew, J. P.; Ruzsinsky, A.; Tao, J.; Staroverov, V. N.; Scuseria, G. E.; Csonka, G. I. J. Chem. Phys. 2005, 123, 062201.

(30) Schipper, P. R. T.; Gritsenko, O. V.; van Gisbergen, S. J. A.; Baerends, E. J. J. Chem. Phys. 2000, 112, 1344.

(31) Vázquez, J.; Bo, C.; Poblet, J. M.; de Pablo, J.; Bruno, J. Inorg. Chem. 2003, 42, 6136.

(32) Graziani, R.; Bombieri, G.; Forsellini, E. J. Chem. Soc. Dalton Trans. 1972, 2059.

(33) Spencer, S.; Gagliardi, L.; Handy, N. C.; Ioannou, A. G.; Skylaris, C. K.;Willetts, A.; Simper, A. M. J. Phys. Chem. A 1999, 103, 1831.

(34) Bardin, N.; Rubini, P.; Madic, C. Radiochim. Acta 1998, 83, 189.
(35) Christ, C. L.; Clark, J. R.; Evans, H. T. J. Science 1955, 121, 472.

(36) Cromer, D. T.; Harper, P. E. Acta Crystallogr. 1955, 8, 847.
(37) Finch, R. J.; Cooper, M. A.; Hawthorne, F. C.; Ewing, R. C. Can. Mineral. 1999, 37, 929.
(38) Matar, S. F. Chem. Phys. 2010, 372, 46.

(39) Pashalidis, I.; Czerwinski, K. R.; Fanghanel, T.; Kim, J. I. Radiochim. Acta 1997, 76, 55.
(40) Rude,W. Los Alamos Science 2000, 26, 412.
(41) Meinrath, G. J. Radioanal. Nucl. Chem. 1997, 224, 119.

(42) Meinrath, G.; Klenze, R.; Kim, J. I. Radiochim. Acta 1996, 74, 81.
(43) Havel, J.; Soto-Guerrero, J.; Lubal, P. Polyhedron 2002, 21, 1411.

(44) Tian, G.; Rao, L. J. Chem. Thermodyn. 2009, 41, 569.

(45) Rao, L.; Tian, G. J. Chem. Thermodyn. 2008, 40, 1001.

(46) Tian, G.; Rao, L. Inorg. Chem. 2009, 48, 6748.

(47) Gong, C. M. S.; Poineau, F.; Czerwinski, K. R. Radiochim. Acta 2007, 95, 439.

[1]	Kang YANG,Xiaorui SHUAI,Huachao YANG,Jianhua YAN,Kefa CEN. Electrochemical Performance of Activated Graphene Powder Supercapacitors Using a Room Temperature Ionic Liquid Electrolyte [J]. Acta Phys. -Chim. Sin., 2019, 35(7): 755-765.
[2]	Tao-Na ZHANG,Xue-Wen XU,Liang DONG,Zhao-Yi TAN,Chun-Li LIU. Molecular Dynamics Simulations of Uranyl Species Adsorption and Diffusion Behavior on Pyrophyllite at Different Temperatures [J]. Acta Phys. -Chim. Sin., 2017, 33(10): 2013-2021.
[3]	Hai-Tao SUN,Cheng ZHONG,Zhen-Rong SUN. Recent Advances in the Optimally "Tuned" Range-Separated Density Functional Theory [J]. Acta Phys. -Chim. Sin., 2016, 32(9): 2197-2208.
[4]	Hai-Feng YIN. Plasmon Excitations in Silicene Quantum Dot Dimers [J]. Acta Phys. -Chim. Sin., 2016, 32(6): 1446-1452.
[5]	Jing ZOU,Zhi-Lin FAN,Li-Sha JIANG,Dan-Hong ZHOU. Theoretical Study of the Solvent Adsorption on Ti-Peroxo Active Center in Ti-MWW Zeolite [J]. Acta Phys. -Chim. Sin., 2016, 32(4): 935-942.
[6]	Sha GAO,Wen-Bo LAN,Ying-Wu LIN,Li-Fu LIAO,Chang-Ming NIE. Molecular Recognition of α, β-Unsaturated Carbonyl Compounds and Chiral Guests by Uranyl-Salophen Receptors [J]. Acta Phys. -Chim. Sin., 2016, 32(3): 683-690.
[7]	Dong ZHENG,Xiang-Ai YUAN,Jing MA. Rationalization of pH-Dependent Absorption Spectrum of o-Methyl Red in Aqueous Solutions: TD-DFT Calculation and Experiment Study [J]. Acta Phys. -Chim. Sin., 2016, 32(1): 290-300.
[8]	Chuan-Xiang YE,Hui-Li MA,Wan-Zhen LIANG. Two-Photon Absorption Properties of Chromophores of a Few Fluorescent Proteins: a Theoretical Investigation [J]. Acta Phys. -Chim. Sin., 2016, 32(1): 301-312.
[9]	Li-Mei. HOU,Zhi. WEN,Yin-Xiang. LI,Hua-You. HU,Yu-He. KAN,Zhong-Min. SU. Molecular Design of Indolizine Derivative as Sensitizers for Organic Dye-Sensitized Solar Cells [J]. Acta Phys. -Chim. Sin., 2015, 31(8): 1504-1512.
[10]	YIN Hai-Feng, XIANG Gong-Zhou, YUE Li, ZHANG Hong. Plasmon Excitation in Silicene Quantum Dots [J]. Acta Phys. -Chim. Sin., 2015, 31(1): 67-72.
[11]	YIN Hai-Feng, ZHANG Hong, YUE Li. Near-Infrared Plasmon Study on N-Doped Hexagonal Graphene Nanostructures [J]. Acta Phys. -Chim. Sin., 2014, 30(6): 1049-1054.
[12]	SUN Jin, LIANGWan-Zhen. Effects of External Field and Nanoribbon Length on the Electronic Structure and Properties of Graphene Nanoribbons [J]. Acta Phys. -Chim. Sin., 2014, 30(3): 439-445.
[13]	CHEN Xi-Ming, JIA Chun-Yang, WAN Zhong-Quan, YAO Xiao-Jun. Theoretical Investigations of Tetrathiafulvalene Derivative as Electron Donor in Organic Dye for Dye-Sensitized Solar Cells [J]. Acta Phys. -Chim. Sin., 2014, 30(2): 273-280.
[14]	ZHAO Cheng-Xiao, WANG Hai-Tao, LI Min. Research Progress in the Correlation between Gelation Properties and Solvent Parameters [J]. Acta Phys. -Chim. Sin., 2014, 30(12): 2197-2209.
[15]	HE Wen-Ying, YAO Xiao-Jun, HUA Ying-Jie, HUANG Guo-Lei, WU Xiu-Li, LI Xiao-Bao, HAN Chang-Ri, SONG Xiao-Ping . Effect of Kolavenic Acid on the Structure of Human Serum Albumin [J]. Acta Phys. -Chim. Sin., 2014, 30(11): 2142-2148.

Electronic Structures of Uranyl(VI) Carbonate Complexes in the Aqueous Phase

PDF (PC)

Like

Knowledge

Abstract

Cite this article

share this article

References

Related Articles 15

Metrics

Comments

Recommended 10