(H_2O)_n(n=1—3)对HN(NO_2)_2→HONONNO_2氢迁移反应的影响
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摘要
采用CBS-QB3方法对HN(NO_2)2→HONONNO_2氢迁移机理和速率常数进行理论研究,并在此基础上考虑了水簇(H_2O)_n(n=1—3)对该反应机理及速率常数的影响。结果表明,HN(NO_2)_2→HONONNO_2氢迁移过程需克服33.8 kcal/mol的能垒。水簇(H_2O)_n(n=1—3)的加入不仅使得氢转移方式从原有反应中的直接抽氢转变为双、三、四氢原子协同转移,而且使得反应能垒降低了15.2~22.8 kcal/mol。其中,(H_2O)_3的参与使能垒降低22.8 kcal/mol,而(H_2O)_2和H_2O使其分别降低22.5 kcal/mol和15.2 kcal/mol。此外,在200~1 000 K温度范围内(H_2O)_3参与使通道的速率常数k3比相同温度下无水参与通道的速率常数k0大了4.2×10~3~6.9×10~(24)倍,说明在200~1 000 K温度范围内(H_2O)_3对HN(NO_2)_2→HONONNO_2氢迁移反应所起的正催化作用最大。
The effect of( H_2O)_n(n = 1—3) on the hydrogen abstraction reaction of HN(NO_2)_2→HONONNO_2has been investigated by employing CBS-QB3 method and conventional transition state theory with wigner tunneling correction. The reaction without catalysts overcomes the barrier height of 33. 8 kcal / mol to form HONONNO_2.( H_2O)_n(n = 1—3) does not change the product of the reaction,but the direct hydrogen abstraction mechanism changes to double,three,and four hydrogen transfer mechanism. Compared with the naked reaction,the barrier height of the hydrogen abstraction reaction with( H_2O)_n(n = 1—3) is lower by15. 2 ~ 22. 8 kcal / mol. Moreover,the barrier height of( H_2O)_3assisted reaction is the lowest. Besides,the rate constants without and with catalyst show that the rate constant of( H_2O)_3-assisted channel is predicted to be faster by 4. 2 × 103~ 6. 9 × 1024 times than that of the naked hydrogen transfer reaction at 200 ~1 000 K,showing that,in temperature range 200 ~ 1 000 K,the( H_2O)_3plays a positive catalytic role for the reaction of HN( NO_2)_2→HONONNO_2.
The effect of( H_2O)_n(n = 1—3) on the hydrogen abstraction reaction of HN(NO_2)_2→HONONNO_2has been investigated by employing CBS-QB3 method and conventional transition state theory with wigner tunneling correction. The reaction without catalysts overcomes the barrier height of 33. 8 kcal / mol to form HONONNO_2.( H_2O)_n(n = 1—3) does not change the product of the reaction,but the direct hydrogen abstraction mechanism changes to double,three,and four hydrogen transfer mechanism. Compared with the naked reaction,the barrier height of the hydrogen abstraction reaction with( H_2O)_n(n = 1—3) is lower by15. 2 ~ 22. 8 kcal / mol. Moreover,the barrier height of( H_2O)_3assisted reaction is the lowest. Besides,the rate constants without and with catalyst show that the rate constant of( H_2O)_3-assisted channel is predicted to be faster by 4. 2 × 103~ 6. 9 × 1024 times than that of the naked hydrogen transfer reaction at 200 ~1 000 K,showing that,in temperature range 200 ~ 1 000 K,the( H_2O)_3plays a positive catalytic role for the reaction of HN( NO_2)_2→HONONNO_2.
引文
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[2]VENKATACHALAM S,SANTHOSH G,NINAN K N.An overview on the synthetic routes and properties of ammonium dinitramide(ADN)and other dinitramide Salts[J].Propellants Explosives Pyrotechnics,2004,29(3):178-187.
[3]YANG R,THAKRE P,YANG V.Thermal decomposition and combustion of ammonium dinitramide(Review)[J].Combustion Explosion and Shock Waves,2005,41(6):657-679.
[4]BADGUJAR D M,TALAWAR M B,ASTHANA S N,et al.Advances in science and technology of modern energetic materials:an overview[J].Journal of Hazardous Materials,2008,151(2):289-305.
[5]TALAWAR M B,SIVABALAN R,ANNIYAPPAN M,et al.Emerging trends in advanced high energy materials[J].Combustion Explosion and Shock Waves,2007,43(1):62-72.
[6]BORMAN S.Alzheimers-disease-free-radical reactions may play key role[J].Chemical Engineering News,1994,72(16):4-5.
[7]ALAVI M,LEIDNER D E.Review:knowledge management and knowledge management systems:conceptual foundations and research issues[J].MIS quarterly,2001,25(1):107-136.
[8]VENKATACHALAM S,SANTHOSH G,NINAN K N.An Overview on the Synthetic Routes and Properties of Ammonium Dinitramide(ADN)and other Dinitramide Salts[J].Propellants Explosives Pyrotechnics,2004,29(3):178-187.
[9]SINGH R P,VERMA R D,MESHRI D T,et al.Energetic nitrogen rich salts and ionic liquids[J].Angewandte Chemie International Edition,2006,45(22):3584-3601.
[10]TANBUG R,KIRSCHBAUM K,PINKERTON A A.Energetic materials:The preparation and structural characterization of melaminium dinitramide and melaminium nitrate[J].Journal of Chemical Crystallography,1999,29(1):45-55.
[11]RUSSELL T P,PIERMARINI G J,BLOCK S,et al.Pressure,temperature reaction phase diagram for ammonium dinitramide[J].The Journal of Physical Chemistry,1996,100(8):3248-3251.
[12]OXLEY J C,SMITH J L,ZHENG W,et al.Thermal decomposition studies on ammonium dinitramide(ADN)and 15N and 2H Isotopomers[J].The Journal of Physical Chemistry A,1997,101(31):5646-5652.
[13]POLITZER P,SEMINARIO J M,CONCHA M C,et al.Density functional study of the structure and some decomposition reactions of the dinitramide anion N(NO2)2[J].Journal of Molecular Structure,1993,287(106):235-240.
[14]DOYLE R J.Sputtered ammonium dinitramide:tandem mass spectrometry of a new ionic nitramine[J].Organic Mass Spectrometry,1993,28(2):83-91.
[15]MEBEL A M,LIN M C,MOROKUMA K,et al.Theoretical study of the gas-phase structure,thermochemistry,and decomposition mechanisms of NH4NO2and NH4N(NO2)2[J].The Journal of Physical Chemistry,1995,99(18):6842-6848.
[16]KAZAKOV A I,RUBTSOV Y I,MANELIS G B,et al.Kinetics of the thermal decomposition of dinitramide.2.kinetics of the reactions of dinitramide with decomposition products and other components of a solution[J].Russian Chemical Bulletin,1998,47(1):39-45.
[17]KAZAKOV A I,RUBTSOV Y I,MANELIS G B,et al.Kinetics of thermal decomposition of dinitramide[J].Russian Chemical Bulletin,1997,46(12):2015-2020.
[18]RAHM M.BRINCK T.Dinitraminic acid(HDN)isomerization and self-decomposition revisited[J].Chemical Physics,2008,348(1-3):53-60.
[19]王志银,许琼,张田雷,等.二硝酰胺铵热分解机理的理论研究进展[J].含能材料,2015,23(9):831-841.
[20]FRISCH M J,TRUCKS G W,POPLE J A,et al.Gaussian 09,revision A.01[CP].Gaussian inc:pittsburgh,pa,2009.
[21]MONTGOMERY J A,FRISCH M J,OCHTERSKI J W,et al.A complete basis set model chemistry.VI.use of density functional geometries and frequencies[J].The Journal of Chemical Physics,1999,110(6):2822-2827.
[22]MONTGOMERY J A,OCHTERSK J W,PETERSSON G A.A complete basis set model chemistry.IV.an improved atomic pair natural orbital method[J].Journal of Chemical Physics,1994,101(7):5900-5909.
[23]LYNCH B J,ZHAO Y,TRUHLAR D G.Effectiveness of diffuse basis functions for calculating relative energies by density functional theory[J].The Journal of Physical Chemistry,2003,107(9):1384-1388.
[24]PETERSSON G A,TENSFELDT T G,MONTGOMERY J A.A complete basis set model chemistry.III.The complete basis set quadratic configuration interaction family of methods[J].The Journal of Chemical Physics,1991,94(9):6091-6101.
[25]ZHANG S,TRUONG T N.VKLab version 1.0[CP].Salt Lake City:University of Utah,2001.
[26]朱艳艳,魏东辉,张文静,等.几种常见氢迁移反应的理论新见解[J].大学化学,2014,29(4):52-57.