Citation: ZENG Xiu-Lin, HUANG Shan-Qi-Song, JU Xue-Hai. Density Functional Theory Study of the Gas-Phase Reaction of U⁺ with CO₂[J]. Acta Physico-Chimica Sinica, ;2013, 29(11): 2308-2312. doi: 10.3866/PKU.WHXB201309042 shu

Density Functional Theory Study of the Gas-Phase Reaction of U⁺ with CO₂

1.
1 Department of Chemistry and Chemical Engineering, Huainan Normal University, Huainan 232001, Anhui Province, P. R. China;
2 Department of Chemistry, Nanjing University of Science and Technology, Nanjing 210094, P. R. China

Received Date: 15 May 2013
Available Online: 4 September 2013
Fund Project: 国家自然科学基金(21101070)资助项目 (21101070)

The gas-phase reaction of U⁺ with CO₂ was investigated with B3LYP density functional theory (DFT) in conjunction with the relativistic effective core potential (ECP) of the SDD basis sets for Uand the 6-311 + G(d) basis set for C and O. The potential energy surfaces (PESs) of the reaction system were explored in detail for both doublet and quartet spin states. The geometries of reactants, intermediates, transition states, and products in the two reaction pathways were fully optimized. The reaction mechanism was analyzed using"two-state reactivity (TSR)."The calculations demonstrate that the reaction preferentially involves the high-spin state entrance channel and the low-spin state exit channel. The spin multiplicity transition from the quartet state to the doublet state enables the reaction system to find a lower energy pathway.
- Reaction mechanism,
- Density functional theory,
- Relativistic effective core potential,
- Potential energy surface,
- Spin state
1. [1]
  
  (1) Gagliardi, L.; Roos, B. O. Nature 2005, 433, 848. doi: 10.1038/nature03249
2. [2]
  (2) Tu, Z. Y.; Yang, D. D.;Wang, F.; Li, X. Y. Acta Phys. -Chim. Sin. 2012, 28, 1707. [涂喆研, 杨冬冬, 王繁, 李象远. 物理化学学报, 2012, 28, 1707.] doi: 10.3866/PKU.WHXB201205111
3. [3]
  (3) Morss, L. R.; Edelstein, N. M.; Fuger, J. The Chemistry of the Actinide and Transactinide Elements; Springer-Verlag: NewYork, 2006; p 65.
4. [4]
  (4) Meskaldji, S.; Zaiter, A.; Belkhiri, L.; Boucekkine, A. Theor. Chem. Acc. 2012, 131, 1151. doi: 10.1007/s00214-012-1151-9
5. [5]
  (5) Roos, B. O.; Malmqvist, P. A.; Gagliardi, L. J. Am. Chem. Soc.2006, 128, 17000. doi: 10.1021/ja066615z
6. [6]
  (6) Baichi, M.; Chatillon, C.; Ducros, G.; Froment, K. J. Nucl. Mater. 2006, 349, 57. doi: 10.1016/j.jnucmat.2005.10.001
7. [7]
  (7) Tiferet, E.; Zalkind, S.; Mintz, M. H.; Jacob, I.; Shamir, N. Surf. Sci. 2007, 601, 936. doi: 10.1016/j.susc.2006.11.033
8. [8]
  (8) Bazley, S. G.; Nunney, T. S.; Mormiche, C.; Hayden, B. E. Appl. Surf. Sci. 2008, 254, 6376. doi: 10.1016/j.apsusc.2008.03.177
9. [9]
  (9) Shuai, M.; Hu, H.;Wang, X.; Zhao, P.; Tian, A. J. Mol. Struct.-Theochem 2001, 536, 269. doi: 10.1016/S0166-1280(00)00720-X
10. [10]
  (10) Dholabhai, P. P.; Ray, A. K. J. Alloy. Compd. 2007, 445, 356.
11. [11]
  (11) Carley, A. F.; Nevitt, P.; Roussel, P. J. Alloy. Compd. 2008, 448,355. doi: 10.1016/j.jallcom.2007.05.028
12. [12]
  (12) Mintz, M. H.; Shamir, N. Appl. Surf. Sci. 2005, 252, 633. doi: 10.1016/j.apsusc.2005.02.077
13. [13]
  (13) Mclean,W.; Colmenares, C. A.; Smith, R. L.; Somorjai, G. A.Phys. Rev. B 1983, 87, 8.
14. [14]
  (14) uder, T.; Colmenares, C. A.; Naegele, J. R.; Spirlet, J. C.;Verbist, J. Surf. Sci. 1992, 264, 354. doi: 10.1016/0039-6028(92)90191-8
15. [15]
  (15) Koyanagi, G. K.; Bohme, D. K. J. Phys. Chem. A 2006, 110,1232. doi: 10.1021/jp0526602
16. [16]
  (16) Fiedler, A.; Schroer, D.; Zummack,W.; Schwarz, H. Inorg. Chim. Acta 1997, 259, 227. doi: 10.1016/S0020-1693(97)05450-9
17. [17]
  (17) Smith, K. M.; Poli, R.; Harvey, J. N. Chemistry 2001, 8, 1679.
18. [18]
  (18) Armentrout, P. B. Science 1991, 251, 175. doi: 10.1126/science.251.4990.175
19. [19]
  (19) Liu, L. L.;Wang, Y. C. Acta Phys. -Chim. Sin. 2010, 26, 441.[刘玲玲, 王永成. 物理化学学报, 2010, 26, 441.] doi: 10.3866/PKU.WHXB20100218
20. [20]
  (20) Zeng, X. L.; Ju, X. H.; Xu, S. Y. Adv. Mater. Res. 2012, 550,2810.
21. [21]
  (21) Zeng, X. L.; Xu, S. Y.; Ju, X. H. Chin. J. Chem. Phys. 2013, 26,51. doi: 10.1063/1674-0068/26/01/51-53
22. [22]
  (22) Zeng, X. L.; Huang, S. Q.; Ju, X. H. J. Radioanal. Nucl. Chem.2013, doi: 10.1007/s10967-013- 2442-x
23. [23]
  (23) Lee, C.; Yang,W. T.; Parr, R. G. Phys. Rev. B 1988, 37, 785. doi: 10.1103/PhysRevB.37.785
24. [24]
  (24) Becke, A. D. J. Chem. Phys. 1993, 98, 5648. doi: 10.1063/1.464913
25. [25]
  (25) Yang, X. Y.;Wang, Y. C.; Geng, Z. Y.; Liu, Z. Y.;Wang, H. Q.J. Mol. Struct. -Theochem 2007, 807, 49. doi: 10.1016/j.theochem.2006.12.017
26. [26]
  (26) Wang, Y. C.; Yang, X. Y.; Geng, Z. Y.; Liu, Z. Y. Chem. Phys. Lett. 2006, 431, 39. doi: 10.1016/j.cplett.2006.09.035
27. [27]
  (27) Leininger, T.; Stoll, H.; Dolg, M.; Schwerdtfeger, P.; Nicklass,A. J. Chem. Phys. 1996, 105, 1052. doi: 10.1063/1.471950
28. [28]
  (28) Frisch, M. J.; Trucks, G.W.; Schlegel, H. B.; et al. Gaussian 03,Revision A.01; Gaussian Inc.: Pittsburgh, PA, 2003.
29. [29]
  (29) Sodupe, M.; Branchadell, V.; Rosi, M.; Bausehllcher, C.W.J. Phys. Chem. A 1997, 101, 7854. doi: 10.1021/jp9711252
30. [30]
  (30) Yoshizawa, K.; Shiota, Y.; Yamabe, T. J. Am. Chem. Soc. 2006,128, 9873. doi: 10.1021/ja061604r
31. [31]
  (31) Gracia, L.; Sambrano, L. R.; Safont, V. S.; Calatayud, M.;Beltran, A.; Andres, J. J. Phys. Chem. A 2003, 107, 3107. doi: 10.1021/jp0222696
32. [32]
  (32) Gracia, L.; Andres, J.; Safont, V. S.; Beltran, A. Organometallics2004, 23, 730. doi: 10.1021/om0342098
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Density Functional Theory Study of the Gas-Phase Reaction of U+ with CO2

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通讯作者: 陈斌, bchen63@163.com

Density Functional Theory Study of the Gas-Phase Reaction of U⁺ with CO₂