从头算分子动力学研究O-与CH3F反应的产物通道

doi:10.3866/PKU.WHXB20100907

Abstract

Abstract:

H-atom abstraction and H₂O production channels for the reaction of O^- with CH₃F were reinvestigated using the ab initio molecular dynamics method at the B3LYP/6-31₊G(d,p) level of theory and based on the Born-Oppenheimer approximation. The reactive trajectories were initiated at the transition state of H-atom abstraction. Thermal sampling at 300 K was chosen to determine the initial conditions. Additionally, the energies added to the transition vector of the barrier were restricted to 2.1, 36.8, and 62.8 kJ·mol ^-1, separately, to reveal the impact of different initial collision energies on the reaction pathways. The results of all the trajectory calculations demonstrate that the H-atom abstraction channel is the dominant production channel. Therefore, our calculations are consistent with previous experimental conclusions. Furthermore, the dynamic reaction pathways for H-atom abstraction and the H₂O production channels on the exit-channel potential energy surface are described based on our calculations and thus a comprehensive reaction mechanismis revealed at the microscopic level.

Key words: Ab initio molecular dynamics, Atomic oxygen radical anion, Methyl fluoride, Reaction mechanism, Transition state

WU Li-Xia, YU Feng, LIU Jing, DAI Jing-Hua, ZHOU Xiao-Guo, LIU Shi-Lin. Ab initioMolecular Dynamics Investigation on the Production Channels for the Reaction of O^- with CH₃F[J]. Acta Phys. -Chim. Sin. 2010, 26(09), 2331-2336. doi: 10.3866/PKU.WHXB20100907

References

1. Bowers, M. T. Gas phase ion chemistry. Vol.1. New York: Academic Press, 1984: 45-82
2. Wayne, R. P. Chemistry of atmosphere. Oxford: Clarendon Press, 1991: 225-256
3. Fialkov, A. B. Prog. Energy Combust. Sci., 1997, 23: 399
4. DePuy, C. H. J. Org. Chem., 2002, 67: 2393
5. Lee, J.; Grabowski, J. J. Chem. Rev., 1992, 92: 1611, and references therein
6. Futrell, J. H.; Tiernan, T. O. Ion molecule reactions. Vol.2. Franklin, J. L. Ed. London: Butterworths, 1972: 485-551
7. Tanaka, K.; Mackay, G. I.; Payzant, J. D.; Bohme, D. K. Can. J. Chem., 1976, 54: 1643
8. Dawson, J. H. J.; Jennings, K. R. J. Chem. Soc. Faraday Trans 2, 1976, 72: 700
9. Peverall, R.; Kennedy, R. A.; Mayhew, C. A.; Watts, P. Int. J. Mass Spectrom. Ion Processes., 1997, 171: 51
10. Yamamoto, M.; Yamashita, K.; Sadakata, M. J. Mol. Struct. - Theochem, 2003, 634: 31
11. Yu, F.; Wu, L. X.; Liu, S. L.; Zhou, X. G. J. Mol. Struct. - Theochem, 2010, 947: 1
12. Frisch, M. J.; Trucks, G. W.; Schlegel, H. B.; et al. Gaussian 03. Reversion B.05. Pittsburgh, PA: Gaussian Inc., 2003
13. Lee, C.; Yang,W.; Parr, R. G. Phys. Rev. B, 1988, 37: 785
14. Becke, A. D. J. Chem. Phys., 1993, 98: 5648
15. MΦller, C.; Plesset, M. S. Phys. Rev., 1934, 46: 618
16. Frisch, M. J.; Head-Gordon, M.; Pople, J. A. Chem. Phys. Lett., 1990, 166: 281
17. Kendall, R. A.; Dunning, T. H.; Harrison, R. J. J. Chem. Phys., 1992, 96: 6796
18. Thompson, D. L. Modern methods for multidimensional dynamics computations in chemistry. Singapore: World Scientific, 1998: 143-189
19. Schlegel, H. B. J. Comput. Chem., 2003, 24: 1514
20. Schlegel, H. B. Bull. Korean Chem. Soc., 2003, 24: 837
21. Millam, J. M.; Bakken, V.; Chen, W.; Hase, W. L.; Schlegel, H. B. J. Chem. Phys., 1999, 111: 3800
22. Bakken, V.; Millam, J. M.; Schlegel, H. B. J. Chem. Phys., 1999, 111: 8773
23. Schleyer, P. v. R.; Allinger, N. L.; Clark, T.; Gasteiger, J.; Kollman, P. A.; Scheafer III, H. F.; Schreiner, P. R. Encyclopedia of computational chemistry. Chichester: Wiley, 1998: 402-407
24. Peslherbe, G. H.;Wang, H.; Hase, W. L. Adv. Chem. Phys., 1999, 105: 171
25. Mulliken, R. S. J. Chem. Phys., 1955, 23: 1833
26. Yu, F.; Zhao, Y. G.;Wang, Y.; Zhou, X. G.; Liu, S. L. Acta Chim. Sin., 2007, 65: 899 [于锋,赵英国,王勇,周晓国,刘世林. 化学学报, 2007, 65: 899]
27. Wang, X. L.; Yu, F.; Xie, D.; Liu, S. L.; Zhou, X. G. Acta Chim. Sin., 2008, 66: 2499 [王新磊,于锋, 谢丹,刘世林,周晓国. 化学学报, 2008, 66: 2499]
28. Wang, J. X.; Yu, F.; Liu, J.; Liu, S. L.; Zhou, X. G. Acta Phys. - Chim. Sin., 2008, 24: 1393 [王俊霞,于锋,刘静, 刘世林, 周晓国.物理化学学报, 2008, 24: 1393]

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Ab initioMolecular Dynamics Investigation on the Production Channels for the Reaction of O^- with CH₃F

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Ab initioMolecular Dynamics Investigation on the Production Channels for the Reaction of O^- with CH₃F