Citation: 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 Physico-Chimica Sinica, ;2012, 28(04): 792-798. doi: 10.3866/PKU.WHXB201201171 shu

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

1.
1. Department of Chemistry, Fuzhou University, Fuzhou 350108, P. R. China;
2. College of Nuclear Technology and Automation Engineering, Chengdu University of Technology, Chengdu 610059, P. R. China

Received Date: 26 September 2011
Available Online: 17 January 2012
Fund Project: 国家自然科学基金(10676007) (10676007)福建省高等学校新世纪优秀人才计划(HX2006-103)资助项目 (HX2006-103)

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.
- Uranyl,
- UV-Vis,
- Solvent effect,
- Time-dependent density functional theory,
- Spin-orbit coupling relativistic effect
1. [1]
  (1) Clark, D. L.; Hobart, D. E.; Neu, M. P. Chem. Rev. 1995, 95, 25.
2. [2]
  (2) Meinrath, G. J. Radioanal. Nucl. Chem. 1996, 211, 349.
3. [3]
  (3) Nguyen Trung, C.; Begun, G. M.; Palmer, D. A. Inorg. Chem. 1992, 31, 5280.
4. [4]
  (4) McGlynn, S. P.; Smith, J. K.; Neely,W. C. J. Chem. Phys. 1961, 35, 105.
5. [5]
  (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. [6]
  (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. [7]
  (7) Allen, P. G.; Bucher, J. J.; Clark, D. L.; Edelstein, N. M.; Ekberg, S. A.; hdes, J.W.; Hudson, E. A.; Kaltsoyannis, N.; Lukens,W.W. Inorg. Chem. 1995, 34, 4797.
8. [8]
  (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. [9]
  (9) Su, J.; Li, J. Prog. Chem. 2011, 23, 1329. [苏静, 李隽. 化学进展, 2011, 23, 1329.]
10. [10]
  (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. [11]
  (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. [12]
  (12) Liu,W. J. Prog. Chem. 2007, 19, 833. [刘文剑. 化学进展, 2007, 19, 833.]
13. [13]
  (13) Cinnéide, S. ó.; Scanlan, J. P.; Hynes, M. J. J. Inorg. Nucl. Chem. 1975, 37, 1013.
14. [14]
  (14) Scanlan, J. P. J. Inorg. Nucl. Chem. 1977, 39, 635.
15. [15]
  (15) Su, J.; Zhang, K.; Schwarz,W. H. E.; Li, J. Inorg. Chem. 2011, 50, 2082.
16. [16]
  (16) Matsika, S.; Pitzer, R. M.; Reed, D. T. J. Phys. Chem. A 2000, 104, 11983.
17. [17]
  (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. [18]
  (18) de Jong,W. A.; Harrison, R. J.; Nichols, J. A.; Dixon, D. A. Theor. Chem. Acc. 2001, 107, 22.
19. [19]
  (19) ADF2010, SCM, Theoretical Chemistry; Vrije Universiteit: Amsterdam, The Netherlands; http://www.scm.com.
20. [20]
  (20) Guerra, C. F.; Snijders, J. G.; Velde, G. T.; Baerends, E. J. Theor. Chem. Acc. 1998, 99, 391.
21. [21]
  (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. [22]
  (22) Perdew, J. P.; Burke, K.; Ernzerhof, M. Phys. Rev. Lett. 1996, 77, 3865.
23. [23]
  (23) van Lenthe, E.; Baerends, E. J. J. Comput. Chem. 2003, 24, 1142.
24. [24]
  (24) van Lenthe, E.; Ehlers, A. E.; Baerends, E. J. J. Chem. Phys. 1999, 110, 8943.
25. [25]
  (25) van Lenthe, E.; Baerends, E. J.; Snijders, J. G. J. Chem. Phys. 1994, 101, 9783.
26. [26]
  (26) van Lenthe, E.; Baerends, E. J.; Snijders, J. G. J. Chem. Phys. 1993, 99, 4597.
27. [27]
  (27) Lee, B.; Richards, F. M. J. Mol. Biol. 1971, 55, 379.
28. [28]
  (28) Richards, F. M. Annu. Rev. Biophys. Bioeng. 1977, 6, 151.
29. [29]
  (29) Perdew, J. P.; Ruzsinsky, A.; Tao, J.; Staroverov, V. N.; Scuseria, G. E.; Csonka, G. I. J. Chem. Phys. 2005, 123, 062201.
30. [30]
  (30) Schipper, P. R. T.; Gritsenko, O. V.; van Gisbergen, S. J. A.; Baerends, E. J. J. Chem. Phys. 2000, 112, 1344.
31. [31]
  (31) Vázquez, J.; Bo, C.; Poblet, J. M.; de Pablo, J.; Bruno, J. Inorg. Chem. 2003, 42, 6136.
32. [32]
  (32) Graziani, R.; Bombieri, G.; Forsellini, E. J. Chem. Soc. Dalton Trans. 1972, 2059.
33. [33]
  (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. [34]
  (34) Bardin, N.; Rubini, P.; Madic, C. Radiochim. Acta 1998, 83, 189.
35. [35]
  (35) Christ, C. L.; Clark, J. R.; Evans, H. T. J. Science 1955, 121, 472.
36. [36]
  (36) Cromer, D. T.; Harper, P. E. Acta Crystallogr. 1955, 8, 847.
37. [37]
  (37) Finch, R. J.; Cooper, M. A.; Hawthorne, F. C.; Ewing, R. C. Can. Mineral. 1999, 37, 929.
38. [38]
  (38) Matar, S. F. Chem. Phys. 2010, 372, 46.
39. [39]
  (39) Pashalidis, I.; Czerwinski, K. R.; Fanghanel, T.; Kim, J. I. Radiochim. Acta 1997, 76, 55.
40. [40]
  (40) Rude,W. Los Alamos Science 2000, 26, 412.
41. [41]
  (41) Meinrath, G. J. Radioanal. Nucl. Chem. 1997, 224, 119.
42. [42]
  (42) Meinrath, G.; Klenze, R.; Kim, J. I. Radiochim. Acta 1996, 74, 81.
43. [43]
  (43) Havel, J.; Soto-Guerrero, J.; Lubal, P. Polyhedron 2002, 21, 1411.
44. [44]
  (44) Tian, G.; Rao, L. J. Chem. Thermodyn. 2009, 41, 569.
45. [45]
  (45) Rao, L.; Tian, G. J. Chem. Thermodyn. 2008, 40, 1001.
46. [46]
  (46) Tian, G.; Rao, L. Inorg. Chem. 2009, 48, 6748.
47. [47]
  (47) ng, C. M. S.; Poineau, F.; Czerwinski, K. R. Radiochim. Acta 2007, 95, 439.
1. [1]
  Yaling Chen . Basic Theory and Competitive Exam Analysis of Dynamic Isotope Effect. University Chemistry, 2024, 39(8): 403-410. doi: 10.3866/PKU.DXHX202311093
2. [2]
  Shipeng WANG , Shangyu XIE , Luxian LIANG , Xuehong WANG , Jie WEI , Deqiang WANG . Piezoelectric effect of Mn, Bi co-doped sodium niobate for promoting cell proliferation and bacteriostasis. Chinese Journal of Inorganic Chemistry, 2024, 40(10): 1919-1931. doi: 10.11862/CJIC.20240094
3. [3]
  YanYuan Jia , Rong Rong , Jie Liu , Jing Guo , GuoYu Jiang , Shuo Guo . Unity is Strength, and Independence Shines: A Science Popularization Experiment on AIE and ACQ Effects. University Chemistry, 2024, 39(9): 349-358. doi: 10.12461/PKU.DXHX202402035
4. [4]
  Jiaxi Xu , Yuan Ma . Influence of Hyperconjugation on the Stability and Stable Conformation of Ethane, Hydrazine, and Hydrogen Peroxide. University Chemistry, 2024, 39(11): 374-377. doi: 10.3866/PKU.DXHX202402049
5. [5]
  Cheng PENG , Jianwei WEI , Yating CHEN , Nan HU , Hui ZENG . First principles investigation about interference effects of electronic and optical properties of inorganic and lead-free perovskite Cs₃Bi₂X₉ (X=Cl, Br, I). Chinese Journal of Inorganic Chemistry, 2024, 40(3): 555-560. doi: 10.11862/CJIC.20230282
6. [6]
  Kexin Dong , Chuqi Shen , Ruyu Yan , Yanping Liu , Chunqiang Zhuang , Shijie Li . Integration of Plasmonic Effect and S-Scheme Heterojunction into Ag/Ag₃PO₄/C₃N₅ Photocatalyst for Boosted Photocatalytic Levofloxacin Degradation. Acta Physico-Chimica Sinica, 2024, 40(10): 2310013-. doi: 10.3866/PKU.WHXB202310013
7. [7]
  Qiuyang LUO , Xiaoning TANG , Shu XIA , Junnan LIU , Xingfu YANG , Jie LEI . Application of a densely hydrophobic copper metal layer in-situ prepared with organic solvents for protecting zinc anodes. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1243-1253. doi: 10.11862/CJIC.20240110
8. [8]
  Fengrui Yang , Debing Wang , Xinying Zhang , Jie Zhang , Zhichao Wu , Qiaoying Wang . Synergistic effects of peroxydisulfate on UV/O₃ process for tetracycline degradation: Mechanism and pathways. Chinese Chemical Letters, 2024, 35(10): 109599-. doi: 10.1016/j.cclet.2024.109599
9. [9]
  Haojie Duan , Hejingying Niu , Lina Gan , Xiaodi Duan , Shuo Shi , Li Li . Reinterpret the heterogeneous reaction of α-Fe₂O₃ and NO₂ with 2D-COS: The role of SDS, UV and SO₂. Chinese Chemical Letters, 2024, 35(6): 109038-. doi: 10.1016/j.cclet.2023.109038
10. [10]
  Pu Zhang , Xiang Mao , Xuehua Dong , Ling Huang , Liling Cao , Daojiang Gao , Guohong Zou . Two UV organic-inorganic hybrid antimony-based materials with superior optical performance derived from cation-anion synergetic interactions. Chinese Chemical Letters, 2024, 35(9): 109235-. doi: 10.1016/j.cclet.2023.109235
11. [11]
  Yunxin Xu , Wenbo Zhang , Jing Yan , Wangchang Geng , Yi Yan . A Fascinating Saga of “Energetic Materials”. University Chemistry, 2024, 39(9): 266-272. doi: 10.3866/PKU.DXHX202307008
12. [12]
  Sifang Zhang , Yanli Tan , Yu Tao , Jiaoyan Zhao , Haihong Zhu . Exploration and Practice of Ideological and Political Cases in the Course of Chemistry History and Methodology. University Chemistry, 2024, 39(10): 377-388. doi: 10.12461/PKU.DXHX202312067
13. [13]
  Jing Wang , Pingping Li , Yuehui Wang , Yifan Xiu , Bingqian Zhang , Shuwen Wang , Hongtao Gao . Treatment and Discharge Evaluation of Phosphorus-Containing Wastewater. University Chemistry, 2024, 39(5): 52-62. doi: 10.3866/PKU.DXHX202309097
14. [14]
  Yanhui XUE , Shaofei CHAO , Man XU , Qiong WU , Fufa WU , Sufyan Javed Muhammad . Construction of high energy density hexagonal hole MXene aqueous supercapacitor by vacancy defect control strategy. Chinese Journal of Inorganic Chemistry, 2024, 40(9): 1640-1652. doi: 10.11862/CJIC.20240183
15. [15]
  Qingqing SHEN , Xiangbowen DU , Kaicheng QIAN , Zhikang JIN , Zheng FANG , Tong WEI , Renhong LI . Self-supporting Cu/α-FeOOH/foam nickel composite catalyst for efficient hydrogen production by coupling methanol oxidation and water electrolysis. Chinese Journal of Inorganic Chemistry, 2024, 40(10): 1953-1964. doi: 10.11862/CJIC.20240028
16. [16]
  Hua Hou , Baoshan Wang . Course Ideology and Politics Education in Theoretical and Computational Chemistry. University Chemistry, 2024, 39(2): 307-313. doi: 10.3866/PKU.DXHX202309045
17. [17]
  Jia Yao , Xiaogang Peng . Theory of Macroscopic Molecular Systems: Theoretical Framework of the Physical Chemistry Course in the Chemistry “101 Plan”. University Chemistry, 2024, 39(10): 27-37. doi: 10.12461/PKU.DXHX202408117
18. [18]
  Lu XU , Chengyu ZHANG , Wenjuan JI , Haiying YANG , Yunlong FU . Zinc metal-organic framework with high-density free carboxyl oxygen functionalized pore walls for targeted electrochemical sensing of paracetamol. Chinese Journal of Inorganic Chemistry, 2024, 40(5): 907-918. doi: 10.11862/CJIC.20230431
19. [19]
  Yunhao Zhang , Yinuo Wang , Siran Wang , Dazhen Xu . Progress in Selective Construction of Functional Aromatics from Nitrogenous Cycloalkanes. University Chemistry, 2024, 39(11): 136-145. doi: 10.3866/PKU.DXHX202401083
20. [20]
  Wendian XIE , Yuehua LONG , Jianyang XIE , Liqun XING , Shixiong SHE , Yan YANG , Zhihao HUANG . Preparation and ion separation performance of oligoether chains enriched covalent organic framework membrane. Chinese Journal of Inorganic Chemistry, 2024, 40(8): 1528-1536. doi: 10.11862/CJIC.20240050

Get Citation

PDF

XML

Metrics

PDF Downloads(1144)
Abstract views(2220)
HTML views(3)

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142