-
基于ReaxFF, 采用NVT系综和Berendsen方法对0–7 GPa时和2500 K时固相硝基甲烷的 分解过程进行分子动力学计算, 通过分析硝基甲烷发生分解反应生成的碎片数量随时间的变化, 对不同压强下硝基甲烷的分解机理进行研究. 计算结果表明在0–3 GPa时, 初始分解路径为C–N键断裂和硝基甲烷的异构化; 在4–7 GPa 时, 初始分解路径为分子间质子转移和C–N, N–O键的断裂; 在硝基甲烷的第二阶段反应中存在H2O, NO, NO2, HONO, 硝基甲烷分子自身的催化反应. 硝基甲烷在高温高压下发生热分解反应生成碳团簇, 且团簇中碳原子的数量和碳团簇的空间构型随着压强的变化而变化.
-
关键词:
- ReaxFF 分子动力学 /
- 热分解 /
- 压强效应 /
- 碳团簇
[1] Tappan B C, Brill T B 2003 Propellents, Explosives, Pyrotechnics 28 72
[2] Russell T P, Allen T M, Gupta Y M 1977 Chem. Phys. Lett. 267 351
[3] Yang Y Q, Wang S F, Sun Z Y, Dlott D D 2004 J. Appl. Phys. 95 3667
[4] Kassoy D R, Kapila A K, Stewart D S 1989 Comb. Sci. Tech. 63 33
[5] Furutani H, Fukumura H, Masuhara H, Kambara S, Kitaguchi T, Tsukada H, Ozawa T 1998 J. Phys. Chem. B 102 3395
[6] Prasad M, Conforti P F, Garrison B J 2007 J. Appl. Phys. 101 103113
[7] Von deer Linde D, Sokolowski-Tinten K 2000 Appl. Surf Sci. 154 1
[8] Peng Y J, Liu YQ, Wang Y H, Zhang S P, Yang Y Q 2009 Acta Phys. Sin. 58 655 (in Chinese) [彭亚晶, 刘玉强, 王英惠, 张淑平, 杨延强 2009 物理学报 58 655]
[9] Piermarini G J, Block S, Miller P J 1989 J. Phys. Chem. 93 462
[10] Shaw R, Decarli, P S, Ross D S, Lee E L Stromberg H D 1979 Combust. Flame 35 237
[11] Xu J, Zhao J J 2009 Acta Phys. Sin. 58 4144 (in Chinese) [徐京城, 赵纪军 2009 物理学报 58 4144]
[12] Wei D Q, Zhang F, Woo T K 2002 AIP Conf. Proc. 620 407
[13] Reed E J, Manaa M R, Laurence L E, Glaesemann K R, Joannopoulos J D 2008 Nature Phys. 4 72
[14] Chang J, Lian P, Wei D Q, Chen X R, Zhang Q M, Gong Z Z 2010 Phys. Rev. Lett. 105 188302
[15] Liu L M, Car R, Selloni A, Dabbs D M, Aksay I A, Yetter R A 2012 J. Am. Chem. Soc. 134 19011
[16] Chen Q F, Cang L C, Chen D Q, Jing F Q 2005 Chin. Phys. 14 2077
[17] van Duin A C, Dasgupta S, Lorant F, Goddard III W A 2001 J. Phys. Chem. A 105 9396
[18] Han S P, van Duin A C, Goddard III W A, Strachan A 2011 J. Phys. Chem. B 115 6534
[19] Guo F, Cheng X, Zhang H 2012 J. Phys. Chem. A 116 3514
[20] Rom N, Zybin S V, van Duin A C, Goddard III W A, Zeiri Y, Katz G, Kosloff R 2011 J. Phys. Chem. A 115 10181
[21] Grimme S 2006 J. Comput. Chem. 27 1787
[22] Trevino S F, Prince E, Hubbard C R 1980 J. Chem. Phys. 73 2996
[23] Wu C J, Fried L E 1997 J. Phys. Chem. A 101 8675
[24] Chakraborty D, Muller R P, Dasgupta S, Goddard III W A 2000 J. Phys. Chem. A 104 2261
[25] Lewis J P, Glaesemann K R, VanOpdorp K, Voth G A 2000 J. Phys. Chem. A 104 11384
[26] Chakraborty D, Muller R P, Goddard III W A 2001 J. Phys. Chem. A 105 1302
[27] Okovytyy S, Kholod Y, Qasim M, Fredrickson H, Leszczynski J 2005 J. Phys. Chem. A 109 2964
[28] Manaa M R, Fried L E, Melius C F, Elstner M, Frauenheim T 2002 J. Phys. Chem. A 106 9024
[29] Xu J J, Zhao J J, Sun L 2008 Mol. Simulat. 34 961
[30] Zheng Z, Xu J J, Zhao J J 2010 High Pressure Res. 30 301
[31] Ge L N, Wei Y, Ji G F, Chen X R, Zhao F, Wei D Q 2012 J. Phys. Chem. B 116 13696
[32] Zhu W H, Huang H, Huang H J, Xiao H M 2012 J. Chem. Phys. 136 044516
[33] Wu J C, Fried L E, Yang L H, Goldman N, Baste S 2009 Nature Chem. 1 57
[34] Zhang L, Chen L, Wang C, Wu J Y 2013 Acta Phys. Chim. Sin. 29 1145 (in Chinese) [张力, 陈朗, 王晨, 伍俊英 2013 物理化学学报 29 1145]
[35] Strachan A, van Duin A C, Chakraborty D, Dasgupta S, Goddard III W A 2003 Phys. Rev. Lett. 91 98301
[36] Strachan A, Kober E M, van Duin A C, Oxgaard J, Goddard III W A 2005 J. Chem. Phys. 122 054502
[37] Zhou T T, Shi Y D, Huang F L 2012 Acta Phys. Chim. Sin. 28 2605 (in Chinese) [周婷婷, 石一丁, 黄风雷 2012 物理化学学报 28 2605]
[38] Isayev O, Gorb L, Qasim M, Leszczynski J 2008 J. Phys. Chem. B 112 11005
[39] Zhang L Z, Zybin S V, van Duin A C, Dasgupta S, Goddard III W A, Kober E M 2009 J. Phys. Chem. A 13 10619
[40] Wang Y, Li P, Ning X J 2005 Acta Phys. Sin. 54 2847 (in Chinese) [王音, 李鹏, 宁西京 2005 物理学报 54 2847]
[41] Ornellas D L1968 J. Phys. Chem. 72 2390
-
[1] Tappan B C, Brill T B 2003 Propellents, Explosives, Pyrotechnics 28 72
[2] Russell T P, Allen T M, Gupta Y M 1977 Chem. Phys. Lett. 267 351
[3] Yang Y Q, Wang S F, Sun Z Y, Dlott D D 2004 J. Appl. Phys. 95 3667
[4] Kassoy D R, Kapila A K, Stewart D S 1989 Comb. Sci. Tech. 63 33
[5] Furutani H, Fukumura H, Masuhara H, Kambara S, Kitaguchi T, Tsukada H, Ozawa T 1998 J. Phys. Chem. B 102 3395
[6] Prasad M, Conforti P F, Garrison B J 2007 J. Appl. Phys. 101 103113
[7] Von deer Linde D, Sokolowski-Tinten K 2000 Appl. Surf Sci. 154 1
[8] Peng Y J, Liu YQ, Wang Y H, Zhang S P, Yang Y Q 2009 Acta Phys. Sin. 58 655 (in Chinese) [彭亚晶, 刘玉强, 王英惠, 张淑平, 杨延强 2009 物理学报 58 655]
[9] Piermarini G J, Block S, Miller P J 1989 J. Phys. Chem. 93 462
[10] Shaw R, Decarli, P S, Ross D S, Lee E L Stromberg H D 1979 Combust. Flame 35 237
[11] Xu J, Zhao J J 2009 Acta Phys. Sin. 58 4144 (in Chinese) [徐京城, 赵纪军 2009 物理学报 58 4144]
[12] Wei D Q, Zhang F, Woo T K 2002 AIP Conf. Proc. 620 407
[13] Reed E J, Manaa M R, Laurence L E, Glaesemann K R, Joannopoulos J D 2008 Nature Phys. 4 72
[14] Chang J, Lian P, Wei D Q, Chen X R, Zhang Q M, Gong Z Z 2010 Phys. Rev. Lett. 105 188302
[15] Liu L M, Car R, Selloni A, Dabbs D M, Aksay I A, Yetter R A 2012 J. Am. Chem. Soc. 134 19011
[16] Chen Q F, Cang L C, Chen D Q, Jing F Q 2005 Chin. Phys. 14 2077
[17] van Duin A C, Dasgupta S, Lorant F, Goddard III W A 2001 J. Phys. Chem. A 105 9396
[18] Han S P, van Duin A C, Goddard III W A, Strachan A 2011 J. Phys. Chem. B 115 6534
[19] Guo F, Cheng X, Zhang H 2012 J. Phys. Chem. A 116 3514
[20] Rom N, Zybin S V, van Duin A C, Goddard III W A, Zeiri Y, Katz G, Kosloff R 2011 J. Phys. Chem. A 115 10181
[21] Grimme S 2006 J. Comput. Chem. 27 1787
[22] Trevino S F, Prince E, Hubbard C R 1980 J. Chem. Phys. 73 2996
[23] Wu C J, Fried L E 1997 J. Phys. Chem. A 101 8675
[24] Chakraborty D, Muller R P, Dasgupta S, Goddard III W A 2000 J. Phys. Chem. A 104 2261
[25] Lewis J P, Glaesemann K R, VanOpdorp K, Voth G A 2000 J. Phys. Chem. A 104 11384
[26] Chakraborty D, Muller R P, Goddard III W A 2001 J. Phys. Chem. A 105 1302
[27] Okovytyy S, Kholod Y, Qasim M, Fredrickson H, Leszczynski J 2005 J. Phys. Chem. A 109 2964
[28] Manaa M R, Fried L E, Melius C F, Elstner M, Frauenheim T 2002 J. Phys. Chem. A 106 9024
[29] Xu J J, Zhao J J, Sun L 2008 Mol. Simulat. 34 961
[30] Zheng Z, Xu J J, Zhao J J 2010 High Pressure Res. 30 301
[31] Ge L N, Wei Y, Ji G F, Chen X R, Zhao F, Wei D Q 2012 J. Phys. Chem. B 116 13696
[32] Zhu W H, Huang H, Huang H J, Xiao H M 2012 J. Chem. Phys. 136 044516
[33] Wu J C, Fried L E, Yang L H, Goldman N, Baste S 2009 Nature Chem. 1 57
[34] Zhang L, Chen L, Wang C, Wu J Y 2013 Acta Phys. Chim. Sin. 29 1145 (in Chinese) [张力, 陈朗, 王晨, 伍俊英 2013 物理化学学报 29 1145]
[35] Strachan A, van Duin A C, Chakraborty D, Dasgupta S, Goddard III W A 2003 Phys. Rev. Lett. 91 98301
[36] Strachan A, Kober E M, van Duin A C, Oxgaard J, Goddard III W A 2005 J. Chem. Phys. 122 054502
[37] Zhou T T, Shi Y D, Huang F L 2012 Acta Phys. Chim. Sin. 28 2605 (in Chinese) [周婷婷, 石一丁, 黄风雷 2012 物理化学学报 28 2605]
[38] Isayev O, Gorb L, Qasim M, Leszczynski J 2008 J. Phys. Chem. B 112 11005
[39] Zhang L Z, Zybin S V, van Duin A C, Dasgupta S, Goddard III W A, Kober E M 2009 J. Phys. Chem. A 13 10619
[40] Wang Y, Li P, Ning X J 2005 Acta Phys. Sin. 54 2847 (in Chinese) [王音, 李鹏, 宁西京 2005 物理学报 54 2847]
[41] Ornellas D L1968 J. Phys. Chem. 72 2390
| 引用本文: |
|
| Citation: |
|
计量
- 文章访问数: 1816
- PDF下载量: 1185
- 被引次数: 0
下载:
