Chem. J. Chinese Universities ›› 2022, Vol. 43 ›› Issue (6): 20220044.doi: 10.7503/cjcu20220044
• Physical Chemistry • Previous Articles Next Articles
DAI Wei, HOU Hua, WANG Baoshan()
Received:
2022-01-18
Online:
2022-06-10
Published:
2022-03-04
Contact:
WANG Baoshan
E-mail:baoshan@whu.edu.cn
Supported by:
CLC Number:
TrendMD:
DAI Wei, HOU Hua, WANG Baoshan. Theoretical Investigations on the Electronic Structures and Reactivity of Heptafluoro-iso-butyronitrile Anion[J]. Chem. J. Chinese Universities, 2022, 43(6): 20220044.
Species | EA/eV | VAE/eV | VDE/eV |
---|---|---|---|
M06?2X/AVTZ | 0.36(0.18) | -0.57(-0.82) | 1.50(1.29) |
ROCBS?Q | 0.22(0.22) | -0.74(-0.50) | 1.21(1.47) |
RCCSD(T)/CBS( | 0.21(0.22) | -0.59(-0.49) | 1.18(1.44) |
RCCSD(T)/CBS( | 0.21(0.22) | -0.56(-0.47) | 1.18(1.45) |
RCCSD(T)?F12/VDZ?F12 | 0.18(0.17) | -0.75(-0.73) | 1.11(1.37) |
RCCSD(T)?F12/VTZ?F12 | 0.21(0.20) | -0.67(-0.66) | 1.16(1.41) |
Table 1 Electron affinity of C4 calculated at various levels of theory*
Species | EA/eV | VAE/eV | VDE/eV |
---|---|---|---|
M06?2X/AVTZ | 0.36(0.18) | -0.57(-0.82) | 1.50(1.29) |
ROCBS?Q | 0.22(0.22) | -0.74(-0.50) | 1.21(1.47) |
RCCSD(T)/CBS( | 0.21(0.22) | -0.59(-0.49) | 1.18(1.44) |
RCCSD(T)/CBS( | 0.21(0.22) | -0.56(-0.47) | 1.18(1.45) |
RCCSD(T)?F12/VDZ?F12 | 0.18(0.17) | -0.75(-0.73) | 1.11(1.37) |
RCCSD(T)?F12/VTZ?F12 | 0.21(0.20) | -0.67(-0.66) | 1.16(1.41) |
Species | ΔZPE/(kJ·mol-1) | Relative energy/(kJ·mol-1) | ||||
---|---|---|---|---|---|---|
M06?2X/AVTZ | RCCSD(T)/CBS | ROCBS?Q | RCCSD(T)?F12A/ VDZ?F12 | RCCSD(T)?F12A/ VTZ?F12 | ||
TS1 | -3.43 | 11.25 | 13.72(12.51) | 11.59(9.92) | 12.68(11.76) | 12.76(11.92) |
IM1 | 0.21 | -75.94 | -75.69(-76.57) | -80.83(-81.38) | -77.86(-78.66) | -77.66(-78.58) |
F+(CF3)2CCN- | -5.10 | 92.59 | 91.76 | 98.11 | 91.21 | 92.01 |
TS2 | -2.59 | 1.55 | -11.30 | -11.38 | -13.26 | -13.01 |
IM2 | 0.88 | -59.79 | -53.39 | -52.51 | -54.10 | -53.72 |
FCN+C(CF3)2- | -8.49 | 185.14 | 187.82 | 196.94 | 185.64 | 186.15 |
TS3 | -0.84 | 15.02 | 15.82 | 15.69 | 15.65 | 15.77 |
C4-, cis | -0.75 | 3.72 | 3.68 | 3.10 | 3.72 | 3.85 |
TS4 | -1.84 | 4.39 | 4.81 | 3.14 | 4.39 | 4.60 |
CF3CFCN-+CF3 | -6.86 | 117.40 | 122.38 | 133.13 | 120.29 | 120.12 |
CN-+C3F7 | -6.32 | 120.79 | 114.06 | 126.48 | 114.35 | 115.48 |
Table 2 ZPE corrections(ΔZPE) and relative energies for the species involved in the decomposition of C4- anion calculated at various levels of theory with respect to trans-C4- conformation*
Species | ΔZPE/(kJ·mol-1) | Relative energy/(kJ·mol-1) | ||||
---|---|---|---|---|---|---|
M06?2X/AVTZ | RCCSD(T)/CBS | ROCBS?Q | RCCSD(T)?F12A/ VDZ?F12 | RCCSD(T)?F12A/ VTZ?F12 | ||
TS1 | -3.43 | 11.25 | 13.72(12.51) | 11.59(9.92) | 12.68(11.76) | 12.76(11.92) |
IM1 | 0.21 | -75.94 | -75.69(-76.57) | -80.83(-81.38) | -77.86(-78.66) | -77.66(-78.58) |
F+(CF3)2CCN- | -5.10 | 92.59 | 91.76 | 98.11 | 91.21 | 92.01 |
TS2 | -2.59 | 1.55 | -11.30 | -11.38 | -13.26 | -13.01 |
IM2 | 0.88 | -59.79 | -53.39 | -52.51 | -54.10 | -53.72 |
FCN+C(CF3)2- | -8.49 | 185.14 | 187.82 | 196.94 | 185.64 | 186.15 |
TS3 | -0.84 | 15.02 | 15.82 | 15.69 | 15.65 | 15.77 |
C4-, cis | -0.75 | 3.72 | 3.68 | 3.10 | 3.72 | 3.85 |
TS4 | -1.84 | 4.39 | 4.81 | 3.14 | 4.39 | 4.60 |
CF3CFCN-+CF3 | -6.86 | 117.40 | 122.38 | 133.13 | 120.29 | 120.12 |
CN-+C3F7 | -6.32 | 120.79 | 114.06 | 126.48 | 114.35 | 115.48 |
Group | Mulliken charge/e | |||
---|---|---|---|---|
C4- | IM1c | IM3c | IM4c | |
CN | -0.987 | -0.463 | -0.072 | -0.646 |
F | -0.409 | -0.682 | -0.451 | -0.408 |
CF3 | -0.179 | -0.289 | -0.182 | -0.108 |
CO2 | 0 | -0.033 | -0.781 | -0.721 |
Table 3 Mulliken charges for various functional groups involved in C4- anion and intermediates calculated at the M06?2X/AVTZ level
Group | Mulliken charge/e | |||
---|---|---|---|---|
C4- | IM1c | IM3c | IM4c | |
CN | -0.987 | -0.463 | -0.072 | -0.646 |
F | -0.409 | -0.682 | -0.451 | -0.408 |
CF3 | -0.179 | -0.289 | -0.182 | -0.108 |
CO2 | 0 | -0.033 | -0.781 | -0.721 |
1 | Rabie M., Fracnck C. M., Environ. Sci. Technol., 2018, 52(2), 369—380 |
2 | Wang B. S., Yu X. J., Hou H., Zhou W. J., Luo Y. B., Trans. China Electrotech. Soc., 2020, 35(1), 21—33 |
王宝山, 余小娟, 侯华, 周文俊, 罗运柏. 电工技术学报, 2020, 35(1), 21—33 | |
3 | Coetello M. G., Flynn R. M., Bulinski M., Fluorinated Nitriles As Dielectric Gases, US 20150083979, 2015⁃03⁃26 |
4 | Nechmi H. E., Beroual A., Girodet A., Vinson P., IEEE Trans. Dielectr. Electr. Insul., 2016, 23(5), 2587—2593 |
5 | Kieffel Y., Irwin T., Ponchon P., Owens J., IEEE Power Energy Mag., 2016, 14(2), 36—39 |
6 | Zhang X., Chen Q., Zhang J., Li Y., Song X., Ran Z., Tang J., IEEE Access, 2019, 7(2), 19100-19108 |
7 | Hu S., Zhou W., Yu J., Qiu R., Li H., IEEE Access, 2019, 7(1), 50159—50167 |
8 | Li Z., Ding W., Liu Y., IEEE Trans. Dielectr. Electr. Insul., 2019, 26(4), 1065—1072 |
9 | Wu Y., Wang C., Sun H., Murphy A. B., Rong M., Yang F., Chen Z., Niu C., Wang X., J. Phys. D., Appl. Phys., 2018, 51(15), 155206 |
10 | Yu X., Hou H., Wang B., J. Phys. Chem. A, 2018, 122(38), 7704—7715 |
11 | Gao K. L., Yan X. L., Liu Y., Wang B. S., Hu S. Z., Li Z. C., Trans. China Electrotech. Soc., 2020, 35(1), 3—20 |
高克利, 颜湘莲, 刘炎, 王宝山, 胡世卓, 李志闯. 电工技术学报, 2020, 35(1), 3—20 | |
12 | Suess L., Liu Y., Parthasarathy R., Dunning F. B., J. Chem. Phys., 2003, 119(24), 12890—12894 |
13 | Chen L., Zhang B., Li X., Yang T., J. Appl. Phys., 2020, 128(14), 143303 |
14 | Rankovic M., Chalabala J., Zawadzki M., Kocisek J., Slavicek P., Fedor J., Phys. Chem. Chem. Phys., 2019, 21(30), 16451 |
15 | Rankovic M., Kumar R., Nag P., Kocisek J., Fedor J., J. Chem. Phys., 2020, 152(24), 244304 |
16 | Zhao Y., Truhlar D. G., Theor. Chem. Acc., 2008, 120(1), 215—241 |
17 | Dunning T. H., J. Chem. Phys., 1989, 90(2), 1007—1023 |
18 | Scuseria G. E., Janssen C. L., Schaefer H. F., J. Chem. Phys., 1988, 89(12), 7382—7387 |
19 | Wood G. P. F., Radom L., Petersson G. A., Barnes E. C., Frisch M. J., Montgomery J. A., J. Chem. Phys., 2006, 125(9), 094106 |
20 | Mackie I. D., Dilabio G. A., J. Chem. Phys., 2011, 135(13), 134318 |
21 | Knizia G., Adler T. B., Werner H. J., J. Chem. Phys., 2009, 130(5), 054104 |
22 | Anderson L. N., Oviedo M. B., Wong B. M., J. Chem. Theory Comput., 2017, 13(4), 1656—1666 |
23 | Rienstar J. C., Tschumper G. S., Schaefer H. F, Nandi S., Ellison G. B., Chem. Rev., 2002, 102(1), 231—282 |
24 | Gauss J., Tajti A., Kallay M., Stanton J. F., Szalay P. G., J. Chem. Phys., 2006, 125(14), 144111 |
25 | Reiher M., Wolf A., J. Chem. Phys., 2004, 121(1), 2037—2047 |
26 | DeYonker N. J., Cundari T. R., Wilson A. K., J. Chem. Phys., 2006, 124(11), 114104 |
27 | Arbelo⁃Gonzalez W., Crespo⁃Otero R., Barbatti M., J. Chem. Theory Comput., 2016, 12(10), 5037—5049 |
28 | Bauernschmitt R., Ahlrichs R., Chem. Phys. Lett., 1996, 256(4), 454—464 |
29 | Klippebstein S. J., Yang Y., Ryzhov V., Dunbar R. C., J. Chem. Phys., 1996, 104(12), 4502—4516 |
30 | Troe J., Miller T. M., Viggiano A. A., J. Chem. Phys., 2012, 136(12), 121102 |
31 | Hou H., Yu X. J., Zhou W. J., Luo Y. B., Wang B. S., Chem. J. Chinese Universities, 2018, 39(11), 2477—2484 |
侯华, 余小娟, 周文俊, 罗运柏, 王宝山. 高等学校化学学报, 2018, 39(11), 2477—2484 | |
32 | Hou H., Wang B. S., Chem. J. Chinese Universities, 2021, 42(12), 3709—3715 |
侯华, 王宝山. 高等学校化学学报, 2021, 42(12), 3709—3715 | |
33 | Yu X., Hou H., Wang B., J. Comput. Chem., 2017, 38(10), 721—729 |
34 | Zhang B., Uzelac N., Cao Y., IEEE Trans. Dielectr. Electr. Insul., 2018, 25(4), 1340—1350 |
35 | Bopp J. C., Roscioli J. R., Johnson M. A., Miller T. M., Viggiano A. A., Villano S. M., Wren S. W., Lineberger W. C., J. Phys. Chem. A, 2007, 111(7), 1214—1221 |
36 | Nechmi H. E., Beroual A., Girodet A., Vinson P., IEEE Trans. Dielectr. Electr. Insul., 2017, 24(2), 886—892 |
37 | Chachereau A., Hosl A., Franck C. M., J. Phys. D: Appl. Phys., 2018, 51(49), 495201 |
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