Citation: WANG Xiu-Jun, LONG Mi. Statistical Correction of Heat of Formation Calculated by the O3LYP Method[J]. Acta Physico-Chimica Sinica doi: 10.3866/PKU.WHXB201207172 shu

Statistical Correction of Heat of Formation Calculated by the O3LYP Method

WANG Xiu-Jun ,
LONG Mi

1.
Key Laboratory of Fuel Cell Techology of Guangdong, College of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510640, P. R. China

Received Date: 9 April 2012
Available Online: 17 July 2012
Fund Project: 国家自然科学基金(20975040) (20975040)广东省自然科学基金(10351064101000000)资助项目 (10351064101000000)

The results of density functional theory calculations are known to contain inherent numerical errors caused by various intrinsic approximations. In this paper, O3LYP/6-311+G(3df,2p)//O3LYP/6-31G(d) calculations were used to derive the heats of formation (Δ_fH_calc^Θ) of 220 small to medium-sized organic molecules, followed by the application of artificial neural network (ANN) and multiple linear regression (MLR) analyses to correct the values. The physical descriptors chosen were Δ_fH_calc^Θ and zero point energy as well as the total quantities of atoms, hydrogen atoms, 2-center bonds, 2-center antibonds, 1-center valence lone pairs and 1-center core pairs. The ANN and MLR systems were initially constructed using a 180 training set. The trained ANN and MLR systems were subsequently used to predict values of Δ_fH_calc^Θ for a 40 individual testing set. The results demonstrated that the root mean square (RMS) deviations between the calculated and experimental Δ_fH^Θ values in the training set were reduced from 24.7 to 11.8 and 13.0 kJ·mol^-1 after ANN and MLR corrections, respectively. For the individual testing set, the deviations (RMSD) were reduced from 21.3 to 10.4 and 12.1 kJ·mol^-1, respectively. Based on these results, it can be concluded that ANN exhibits superior fitting and predictive abilities compared with MLR.
- O3LYP,
- Neural network,
- Multiplelinear regression,
- Heat of formation,
- Root mean square deviation
1. [1]
  
  (1) Pedley, J. B.; Naylor, R. D.; Kirby, S. P. Thermochemical Data of Organic Compounds; Chapman and Hall: New York, 1986.
2. [2]
  (2) Yaws, C. L. Chemical Properties Handbook; McGraw-Hill:New York, 1999.
3. [3]
  (3) Lide, D. R. CRC Handbook of Chemistry and Physics, 3rd.electronic ed.; BocaRaton: FL, 2000.
4. [4]
  (4) Wu, J.; Xu, X. J. Chem. Phys. 2007, 127, 214105. doi: 10.1063/1.2800018
5. [5]
  (5) Curtiss, L. A.; Raghavachari, K.; Redfern, P. C.; Pople, J. A.Chem. Phys. Lett. 1997, 270, 419. doi: 10.1016/S0009-2614(97)00399-0
6. [6]
  (6) Schmitz, L. R.; Chen, K. H.; Labanowski, J.; Allinger, N. L.J. Phys. Org. Chem. 2001, 14, 90. doi: 10.1002/1099-1395(200102)14:2<90::AID-POC330>3.0.CO;2-O
7. [7]
  (7) Curtiss, L. A.; Raghavachari, K.; Trucks, G.W.; Pople, J. A.J. Chem. Phys. 1991, 94, 7221. doi: 10.1063/1.460205
8. [8]
  (8) Lado-Tourino, I.; Tsobnang, F. Comp. Mater. Sci. 1998, 11, 181.doi: 10.1016/S0927-0256(98)80004-9
9. [9]
  (9) Curtiss, L. A.; Raghavachari, K.; Redfern, P. C.; Pople, J. A.J. Chem. Phys. 2000, 112, 7374. doi: 10.1063/1.481336
10. [10]
  (10) Wodrich, M. D.; Corminboeuf, C.; Schleyer, P. v. R. Org. Lett.2006, 8, 3631. doi: 10.1021/ol061016i
11. [11]
  (11) Check, C. E.; Gilbert, T. M. J. Org. Chem. 2005, 70, 9828. doi: 10.1021/jo051545k
12. [12]
  (12) Iz rodina, E. I.; Coote, M. L.; Radom, L. J. Phys. Chem. A2005, 109, 7558. doi: 10.1021/jp052021r
13. [13]
  (13) Schreiner, P. R.; Fokin, A. A.; Pascal, R. A., Jr.; de Meijere, A.Org. Lett. 2006, 8, 3635. doi: 10.1021/ol0610486
14. [14]
  (14) Zhao, Y.; nzalez-Garcia, N.; Truhlar, D. G. J. Phys. Chem. A2005, 109, 2012. doi: 10.1021/jp045141s
15. [15]
  (15) Zhang, I. Y.; Luo, Y.; Xu, X. J. Chem. Phys. 2010, 132, 194105.doi: 10.1063/1.3424845
16. [16]
  (16) Cohen, A. J.; Handy, N. C. Mol. Phys. 2001, 99, 607. doi: 10.1080/00268970010023435
17. [17]
  (17) Yang, K.; Peverati, R.; Truhlar, D. G.; Valero, R. J. Chem. Phys.2011, 135, 044118. doi: 10.1063/1.3607312
18. [18]
  (18) Heerdt, G.; Mor n, N. H. Quimica Nova 2011, 34, 868. doi: 10.1590/S0100-40422011000500024
19. [19]
  (19) Bochevarov, A. D.; Friesner, R. A.; Lippard, S. J. J. Chem. Theory Comput. 2010, 6, 3735. doi: 10.1021/ct100398m
20. [20]
  (20) Dobado, J. A.; mez-Tamayo, J. C.; Calvo-Flores, F. G.;Martinez-Garcia, H.; Cardona,W.;Weiss-Lopez, B.; Ramirez-Rodriguez, O.; Pessoa-Mahana, H.; Araya-Maturana, R. Magn. Reson. Chem. 2011, 49, 358. doi: 10.1002/mrc.2745
21. [21]
  (21) Qian, Z. S.; Feng, H.; He, L. N.; Yang,W. J.; Bi, S. P. J. Phys. Chem. A 2009, 113, 5138. doi: 10.1021/jp810632f
22. [22]
  (22) Strassner, T.; Taige, M. A. J. Chem. Theory Comput. 2005, 1,848. doi: 10.1021/ct049846+
23. [23]
  (23) Baker, J.; Pulay, P. J. Comput. Chem. 2003, 24, 1184. doi: 10.1002/jcc.10280
24. [24]
  (24) Curtiss, L. A.; Jones, C.; Trucks, G.W.; Raghavachari, K.;Pople, J. A. J. Chem. Phys. 1990, 93, 2537. doi: 10.1063/1.458892
25. [25]
  (25) Curtiss, L. A.; Raghavachari, K.; Redfern, P. C.; Pople, J. A.J. Chem. Phys. 1997, 106, 1063. doi: 10.1063/1.473182
26. [26]
  (26) Curtiss, L. A.; Raghavachari, K.; Redfern, P. C.; Rassolov, V.;Pople, J. A. J. Chem. Phys. 1998, 109, 7764. doi: 10.1063/1.477422
27. [27]
  (27) Curtiss, L. A.; Raghavachari, K.; Redfern, P. C.; Pople, J. A.J. Chem. Phys. 2000, 112, 7374. doi: 10.1063/1.481336
28. [28]
  (28) Curtiss, L. A.; Redfern, P. C.; Raghavachari, K. Chem. Phys. Lett. 2010, 499, 168. doi: 10.1016/j.cplett.2010.09.012
29. [29]
  (29) Dorofeeva, O. V.; Kolesnikova, I. N.; Marochkin, I. I.; Ryzhova,O. N. J. Struct. Chem. 2011, 22, 1303. doi: 10.1007/s11224-011-9827-7
30. [30]
  (30) Hu, L. H.;Wang, X. J.;Wong, L. H.; Chen, G. H. J. Chem. Phys. 2003, 119, 11501. doi: 10.1063/1.1630951
31. [31]
  (31) Wang, X. J.;Wong, L. H.; Hu, L. H.; Chan, C. Y.; Su, Z. M.;Chen, G. H. J. Phys. Chem. A 2004, 108, 8514. doi: 10.1021/jp047263q
32. [32]
  (32) Duan, X. M.; Li, Z. H.; Song, G. L.;Wang,W. N.; Chen, G. H.;Fan, K. N. Chem. Phys. Lett. 2005, 410, 125. doi: 10.1016/j.cplett.2005.05.046
33. [33]
  (33) Duan, X. M.; Song, G. L.; Li, Z. H.;Wang, X. J.; Chen, G. H.;Fan, K. N. J. Chem. Phys. 2004, 121, 7086. doi: 10.1063/1.1786582
34. [34]
  (34) Yan, G. K.; Li, J. J.; Li, B. R.; Hu, J.; Guo,W. P. J. Theor. Comput. Chem. 2007, 6, 495. doi: 10.1142/S0219633607003118
35. [35]
  (35) Zheng, X.; Hu, L.;Wang, X.; Chen, G. Chem. Phys. Lett. 2004,390, 186. doi: 10.1016/j.cplett.2004.04.020
36. [36]
  (36) Zhang, J. H.;Wang, X. J. Acta Phys. -Chim. Sin. 2010, 26,188. [张家虎, 王秀军. 物理化学学报, 2010, 26, 188.]doi: 10.3866/PKU.WHXB20100116
37. [37]
  (37) Frisch, M. J.; Trucks, G.W.; Schlegel, H. B.; et al. Gaussian 09,Revision B.01; Gaussian Inc.:Wallingford, CT, 2010.
38. [38]
  (38) Zheng,W. F.; Tropsha, A. J. Chem. Inf. Comput. Sci. 2000, 40,185. doi: 10.1021/ci980033m
39. [39]
  (39) Cramer, R. D., III; Patterson, D. E.; Bunce, J. D. J. Am. Chem. Soc. 1988, 110, 5959. doi: 10.1021/ja00226a005
40. [40]
  (40) lbraikh, A.; Tropsha, A. J. Chem. Inf. Comput. Sci. 2003, 43,144. doi: 10.1021/ci025516b
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