• <tr id="yyy80"></tr>
  • <sup id="yyy80"></sup>
  • <tfoot id="yyy80"><noscript id="yyy80"></noscript></tfoot>
  • 99热精品在线国产_美女午夜性视频免费_国产精品国产高清国产av_av欧美777_自拍偷自拍亚洲精品老妇_亚洲熟女精品中文字幕_www日本黄色视频网_国产精品野战在线观看 ?

    BTATz-Pb復(fù)合物對(duì)雙基和RDX-改性雙基推進(jìn)劑的熱行為、非等溫動(dòng)力學(xué)及燃燒性能的影響

    2013-10-18 05:27:10任瑩輝趙鳳起張鮮波馬海霞徐抗震王伯周儀建華宋紀(jì)蓉胡榮祖
    物理化學(xué)學(xué)報(bào) 2013年1期

    李 文 任瑩輝,,* 趙鳳起 張鮮波 馬海霞 徐抗震 王伯周 儀建華 宋紀(jì)蓉,3 胡榮祖

    (1西北大學(xué)化工學(xué)院,陜西省物理無(wú)機(jī)化學(xué)重點(diǎn)實(shí)驗(yàn)室,西安 710069;2西安近代化學(xué)研究所,燃燒與爆炸技術(shù)重點(diǎn)實(shí)驗(yàn)室,西安 710065;3故宮博物院文??萍疾?北京 100009)

    1 Introduction

    3,6-Bis(1H-1,2,3,4-tetrazol-5-yl-amino)-1,2,4,5-tetrazine(BTATz),a novel energetic material,was synthesized firstly by Hiskey et al.1at Los Alamos National Laboratory.It was one of the high-nitrogen energetic compounds with an excellent performance,such as high nitrogen content of 79.02%,density of 1.76 g·cm-3,enthalpy of formation of 883 kJ·mol-1,and moderate mechanical and thermal sensitivity.2-7Our research group has been involved in a systematic experimental study about the synthesis and purification,6the burning rate measurement,8the quantum chemistry study,5thermal behavior and kinetic investigation of the thermal decomposition processes,7even as a substitute of hexogen(RDX)in the composite modified double base(CMDB)propellant formulation.9Many researches focusing on the BTATz showed that it had a prospect function as a primary component in the high burning rate propellant for the booster rocket motor and the kinetic energy ammunition,and it also could be used in the minimum signature propellant for the smokeless ammunition.8,10-11

    Lead salts,12-15oxides16or nano-oxides17were usually added to the solid propellant as the combustion catalyst.Although the lead compounds could bring about the heavy metal pollution to the surrounding and human health,it was well known that they could improve the solid propellant ballistic properties,i.e.,they could increase burning rate and decrease the pressure exponent of the burning rate.So they are extensively used as one of the key ballistic modifiers in solid propellant formulations.18Therefore,the study on them had not any significance unless the excellent substitute was developed.In this work,the lead complex of BTATz(LCBTATz)was synthesized and its structure was also characterized.The thermal behaviors,nonisothermal decomposition reaction kinetics,thermal safety,and combustion properties of double-base(DB)propellant containing LCBTATz or composite modified double-base(CMDB)propellant containing catalyst were investigated.

    2 Experimental

    Caution!Although none of the compounds described herein have exploded or detonated in the course of this research,these materials should be handled with extreme care using the best safety practices.

    2.1 Equipment and conditions

    The thermogravimetry-derivative thermogravimetry(TGDTG)and differential scanning calorimetry(DSC)curves under the condition of flowing nitrogen gas(purity,99.999%;atmospheric pressure)were obtained by using a TA2950 thermal analyzer(TACo.,USA)and a 204HP differential scanning calorimeter(Netzsch Co.,Germany).The conditions of TG-DTG were:sample mass,about 1 mg;N2flowing rate,40 cm3·min-1;heating rate(β),10 K·min-1.The conditions of DSC analyses were:sample mass,about 1 mg;N2flowing rate,50 cm3·min-1;heating rate,5,10,15,and 20 K·min-1;furnace pressures,0.1 MPa;reference sample,α-Al2O3;type of crucible,aluminum pan with apierced lid.The specific heat capacity(Cp,J·g-1·K-1)was determined with continuous Cpmode on a Micro-DSC III mircocalorimeter(Setaram Co.,France).Heating rate,0.15 K·min-1;sample mass,about 100 mg;atmosphere,N2;reference sample,calcined α-Al2O3.The burning rates of the samples were measured in a strand burner filled with nitrogen at different pressures,and the samples prepared were the Φ 5 mm×100 mm cylinder strand coated with polyvinyl formal.19

    2.2 Materials

    The lead complex of BTATz used in the propellant was carried out as follows:BTATz(provided by Xi′an Modern Chemistry Research Institute,purity,99.9%,measured by high performance liquid chromatography)5and Pb(CH3COO)2·3H2O(AR grade)with mole ratio of 1:2 were dissolved into DMSO and deionized water,respectively.The mixture was stirred for 1.5 h at 70°C.After that,a precipitate was filtered,washed with water repeatedly and dried at 80°C.Finally,the orange powder was obtained.Anal.Calc.for C12H16N28O5Pb(%):C 17.20,H 1.81,N 47.32,Pb 23.63.Found:C 17.2,H 1.9,N 46.7,Pb 24.7.IR(KBr,v/cm-1):3017,2863,1624,1506,1438,1323,1042,780,674.

    Scheme 1 Structure of the title complex

    The chemical structure of the title complex is shown in Scheme 1.

    The sample of DB001 used in the experiment was a DB propellant containing LCBTATz composed of 59%(mass fraction)nitrocellulose(NC),30%nitroglycerin(NG),8.5%diethyl phthalate(DEP),and other additives,etc.The strand sample composed of 500 g ingredients and 12.5 g LCBTATz,LCBTATz as ballistic modifier was prepared by a solventless DB propellant extrusion technique,including slurry mixing,rolling,and extruding.The control DB propellant without ballistic modifier(No.DB002)was also prepared for the comparison with the sample DB001.

    The RDX-CMDB propellant sample of CMDB100 used in the experiment was composite modified double base propellant containing LCBTATz,composed of 38%(mass fraction)nitrocellulose(NC),28%nitroglycerin(NG),2.5%LCBTATz,26%hexogen(RDX),5%N-nitro-dihydroxyethylamine-dinitrate(DINA)and other auxiliary.The strand sample composed of 500 g ingredients and 12.5 g LCBTATz,LCBTATz as ballistic modifier was prepared by a solventless CMDB propellant extrusion technique,including slurry mixing,rolling,and extruding.The control CMDB propellant without ballistic modifier(No.CMDB101)was also prepared for the comparison with the sample CMDB100.20-23

    3 Results and discussion

    3.1 Thermal behaviors

    The TG-DTG curves of DB001 and CMDB100 propellants at the heat rate of 10 K·min-1are shown in Figs.1 and 2,and the DSC curves at the heating rate of 5,10,15,20 K·min-1are shown in Figs.3 and 4,respectively.

    Fig.1 TG-DTG curves for propellant DB001

    Fig.2 TG-DTG curve for propellant CMDB100

    Fig.3 DSC curves for propellant DB001

    From Fig.1,it can be found that there is only one mass-loss stage in TG curve,corresponding to one invisible exothermic peak in DSC curve.For TG curve,there is a mass loss of about 77%between 380 and 540 K,which is close to the mass(80%)of NG and NC,and it likely attributes to the volatilization and decomposition of NC and decomposition of NG.24

    There are two mass loss stages in Fig.2,corresponding to the two continuous exothermic peaks in the DSC curve.The first begins at 390 K and stops at 495 K,witnessing about 61%mass loss,which is close to the total mass(54%)of the nitroglycerine and nitrocellulose mixture in the RDX-CMDB propellant.It can be attributed to the volatilization and decomposition of the NG/NC mixture,corresponding to the invisible peak in the DSC curve(main exothermic stage,Fig.4).The second follows the decomposition of NG/NC process,and stops at 540 K,with 20%mass loss,which belongs to the RDX decom-position in the RDX-CMDB propellant.Because the decomposition of RDX occurs in succession,the decomposition heats of the two processes overlap each other part.

    Fig.4 DSC curves for propellant CMDB001

    3.2 Calculation of nonisothermal reaction kinetics

    To explore the reaction mechanisms of the main exothermic decomposition processes of the propellants DB001 and CMDB100 and obtain the corresponding kinetic parameters[apparent activation energy(Ea/(kJ·mol-1)),pre-exponential constant(A/s-1)and the most probable kinetic model functions],the DSC curves at the heating rate of 5,10,15,and 20 K·min-1were dealt with mathematic means,and the basic data and temperature data corresponding to the conversion degrees(α)were found and shown in Tables 1 and 2,respectively.

    Five integral methods(General integral,MacCallum-Tanner,?atava-?esták,Agrawal,Flynn-Wall-Ozawa)and one differential method(Kissinger)were employed.25-27While the values of Eaobtained by Ozawa′s method from the isoconversional DSC curves at the heating rate of 5,10,15,and 20 K·min-1,the Ea-α curves were shown in Fig.5.It shows that the activation energy changed slightly in the section of 0.20-0.84(α)for DB001 and 0.22-0.80(α)for CMDB100,which were properly selected to calculate the nonisothermal reaction kinetics.

    Forty-one types of kinetic model functions and the basic data(Table 2)for the propellant were put into the integral and dif-ferential equations for calculation.The values of Ea,lg A,and the linear correlation coefficient(r)were calculated on computer with the linear least-squares method,and the most probable mechanism function was selected by the better value of r.25-27The results of satisfying the conditions at the same time were the final results as listed in Table 3,and the relevant functions were the reaction mechanism function of the decomposition process.

    Table 1 Basic data for the main exothermic decomposition processes of the propellants DB001 and CMDB100

    Table 2 Temperature data for the main exothermic decomposition processes of the propellants DB001 and CMDB100

    Fig.5 E a- α curves for the propellants of DB001 and CMBD100 E ais the apparent activation energy of kinetic model functions.

    Table 3 Kinetic parameters for the main exothermic decomposition process of the propellants DB001 and CMDB100

    From Table 3,one can see that the values of Eaand lg A obtained from thenonisothermal DSC curves are approximately in agreement with the values calculated by Kissinger′s method and Ozawa′s method,and the mechanism function number is determinated.The decomposition reaction mechanism functions of two propellants are listed in Table 4.The substituting f(α)expression,and the values of Eaand A into Eq.(1),the corresponding kinetic equations[Eqs.(2)and(3)]of the decomposition reaction of the propellants are obtained and shown in Table 4.

    3.3 Thermal safety studies

    3.3.1 Self-accelerating decomposition temperature

    The values(Te0and Tp0)of the onset temperature(Te)and peak temperature(Tp)corresponding to β→0 obtained by Eq.(4),25-27are listed in Table 5.

    where b and c are coefficients,TSADTis the self-accelerating de-composition temperature.

    Table 4 Mechanism functions,apparent activation energies,and kinetic equations for the propellants DB001 and CMDB100

    3.3.2 Thermal ignition temperature(TTITT)and critical temperatures of thermal explosion(Tb)

    The corresponding critical temperatures of thermal explosion(Tbeand Tbp)obtained from Eq.(6),28are also listed in Table 5.The high values of Tbfor DB001 and CMDB100 propellants show that the transition from thermal decomposition to thermal explosion is not easy to take place.

    where R is the gas constant,EOis the value of Eaby Ozawa′s method.

    3.3.3 Adiabatic time-to-explosion

    The adiabatic time-to-explosion(tTIad)of energetic materials is the time of decomposition transiting to explosion under the adiabatic conditions and is an important parameter for assessing their thermal stability and safety.

    Substituting the following data into Smith equations[Eqs.(7)-(9)],29,30the values of tTIadfor the propellants are acquired and also listed in Table 5.

    For the propellant DB001:Cp=-20.95+0.195 T-5.69×10-4T2+5.61×10-7T3(J·g-1·K-1),Q=-ΔHd=1703.5 J·g-1,A=AK=1018.20s-1,E=EK=182500 J·mol-1,R=8.314 J·mol-1·K-1,mechanism f(α)=α-1/2,the integral lower limit T1=Teo=444.5 K,the upper limit T2=Tb=471.8 K.EKand AKare calculated by Kissinger method.

    Table 5 Derivative parameters for DB001 and CMDB100

    Table 6 Burning rates(u)of DB001,DB002,CMDB100,and CMDB101 at different pressures

    For the propellant CMDB100:the specific heat capacity,Cp=2.60-1.16×10-2T+2.49×10-5T2(J·g-1·K-1),Q=-ΔHd=1072.5 J·g-1,A=AK=1017.14s-1,E=EK=173130 J·mol-1,R=8.314 J·mol-1·K-1,mechanism f(α)=2(1-α)3/2,the integral lower limit T1=Teo=442.4 K,the upper limit T2=Tb=464.1 K.

    3.3.4 Thermodynamic parameters of activation reaction

    The entropy of activation(ΔS≠),enthalpy of activation(ΔH≠),and free energy of activation(ΔG≠)of the decomposition reaction,corresponding to T=Tp0,Ea=EK,and A=AK,are obtained from Eqs.(10)-(12),25,26respectively,and also listed in Table 5.The positive values of ΔG≠indicate that the exothermic decomposition reaction of the propellants must proceed under the heat condition.

    where kBis the Boltzmann constant,and h is the Plank constant.

    From Table 5,the calculated values of TSADT,TTITT,and Tbfor the propellant DB001 and CMDB100 show that they have the high thermal safety from adiabatic decomposition to explosion.

    3.4 Combustion property

    For the sake of the possible application of LCBTATz in DB propellant and RDX-CMDB propellant,the burning rates[u/(mm·s-1)]of DB002(mass fractions of NC/NG/DEP/auxiliary:59%/30%/8.5%/2.5%)and DB001 were measured under different pressures(p).

    Fig.6 Burning rate curves of DB001

    Also,the CMDB101(mass fractions of NC/NG/RDX/auxiliary:38%/28%/26%/8%)and CMDB100 were measured under different pressures,respectively.The data are listed in Table 6 and the curves of burning rates are shown in Figs.6 and 7.It can be seen that with the help of the catalysis of LCBTATz,the burning rate of the DB propellant and RDX-CMDB propellant are improved observably.The burning rate of the DB propellant can be improved by 208.4%at 2 MPa and“super burning effect”is occurred at 2-8 MPa,and burning rate of the CMDB propellant can be improved by 159.2%at 2 MPa and the burning rate is increased remarkably at 2-8 MPa.

    In order to evaluate the effects of the ballistic modifier on the combustion property of the propellants,the pressure exponent(n)of the burning rate was calculated,and the mean value of the catalysis efficiency(Zˉ)was compared before and after LCBTATz was added into the propellant formulation.The values of n and Zˉwere obtained by Eqs.(13)and(14),31,32and the relationship between Z and test pressure were shown in Figs.8 and 9.

    where,I:without catalysis DB propellant,II:2.5%LCBTATz DB propellant,III:without catalysis RDX-CMDB propellant,IV:2.5%LCBTATZ RDX-CMDB propellant

    For DB001:

    Fig.7 Burning rate curves of CMDB100

    Fig.8 Relationship of catalytic efficiency and text pressure at 2-8 MPa in DB001

    Fig.9 Relationship of catalytic efficiency and text pressure at 2-8 MPa in CMDB100

    Fig.8 shows that the value of Z is higher than 2 at 2-8 MPa,and that the pressure exponent of DB100 propellant is reduced by 64%from 0.805 to 0.289 at 2-8 MPa.It is reduced to-0.065 at 8-12 MPa,which is in the range of“mesa effect”.From Fig.9,it can be seen that the value of Z is higher than 1.7 and the pressure exponent of CMDB propellant is reduced to 0.178 at 2-8 MPa,within the range of which“plateau combustion”occurs.

    As one can see,LCBTATz as an auxiliary ballistic energetic modifier can be effective to increase the burning rate and reduce the pressure exponent of propellants.Especially,super burning effect occurs at low pressure and the“mesa effect”occurs at 8-12 MPa in the DB propellant.The pressure exponent of CMDB100 is reduced to 0.178,and“plateau combustion”occurs at 4-12 MPa.

    4 Conclusions

    The lead complex based BTATz(LCBTATz)was prepared,characterized,and investigated.It was used as a catalyst for DB001 and CMDB100.The reaction kinetic equations of the main exothermal decomposition processes of DB001 and CMDB100 are dα/d t=1016.91×(α-1/2)×exp(-1.76×105/RT)and dα/d t=1017.77×2(1-α)3/2×exp(-1.78×105/RT),respectively.The The results of evaluating the thermal safety for the propellants were obtained as:(1)for DB001,TSADT=444.50 K,TTITT=453.96 K,Tb=471.84 K;when EK=182500 J·mol-1,and AK=1018.20s-1,tTlad=39.36 s,ΔS=99.87 J·mol-1·K-1;ΔH=178.66 kJ·mol-1,ΔG=132.56 kJ·mol-1;(2)For CMDB100,TSADT=442.38 K,TTITT=452.89 K,Tb=464.13 K;when EK=162100 J·mol-1,and AK=1015.9s-1,tTlad=21.3 s,ΔS=79.72 J·mol-1·K-1,ΔH=169.36 kJ·mol-1,ΔG=133.18 kJ·mol-1.With the help of the ballistic modifier in the DB propellant formulation,the burning rate can be improved by 208.4%at 2 MPa and 126.5%at 4 MPa,and the pressure exponent can be reduced to-0.06 at 8-12 MPa.Also,in the CMDB propellant formulation,the burning rate can be improved by 159.2%at 2 MPa,the pressure exponent can be reduced to 0.18 at 4-12 MPa.The results show that LCBTATz has obvious catalysis in increasing the rate and excellent ability to reduce pressure index in the combustion of double-base propellants.Compared with other general lead compounds,or nanocompounds,LCBTATz can either enhance the burning rate or lower pressure index in DB propellants,which is a kind of high efficient combustion catalyst at the rang of medium and low pressure.33-38

    (1)Chavez,D.;Hiskey,M.;Darrenl,D.N.Propellants,Explosives Pyrotech nics 2004,29,209.

    (2)Hickey,M.A.;Chavez,D.E.;Naud,D.Preparation of 3,3′-Azobis(6-amino-1,2,4,5-tetrazine).US Patent,6342589,2002.

    (3)Hickey,M.A.;Chavez,D.E.;Naud,D.3,6-bis(1 H-1,2,3,4-tetrazol-5-ylamino)-1,2,4,5-tetrazine or Salt Thereof.US Patent,6657059,2003.

    (4)Yue,S.T.;Yang,S.Q.Chin.J.Energy Mater.2004,12,155.[岳守體,陽(yáng)世清.含能材料,2004,12,155.]

    (5)Wang,B.Z.;Lai,W.P.;Liu,Q.;Lian,P.;Xue,Y.Q.Chin.J.Org.Ch em.2008,28,422.[王伯周,來(lái)蔚鵬,劉 愆,廉 鵬,薛永強(qiáng).有機(jī)化學(xué),2008,28,422.]

    (6)Saikia,A.;Sivabalan,R.;Polke,B.G.;Gore,G.M.;Singh,A.;Rao,A.S.;Sikder,A.K.J.Hazard.Mater.2009,170,306.doi:10.1016/j.jhazmat.2009.04.095

    (7)Zhang,X.G.;Zhu,H.;Yang,S.Q.;Zhang,W.;Zhao,F.Q.;Liu,Z.R.;Pan,Q.Ch in.J.P rop.Technol.2007,8,322.[張興高,朱 慧,陽(yáng)世清,張 煒,趙鳳起,劉子如,潘 清.推進(jìn)技術(shù),2007,8,322.]

    (8)Son,S.F.;Berghout,H.L.;Bolme,C.A.;Chavez,D.E.;Naud,D.;Hiskey,M.A.Proceedings of the Combustion Institute 2000,28,919.doi:10.1016/S0082-0784(00)80298-2

    (9)Yi,J.H.;Zhao,F.Q.;Wang,B.Z.;Liu,Q.;Zhou,C.;Hu,R.Z.;Ren,Y.H.;Xu,S.Y.;Xu,K.Z.;Ren,X.N.J.Hazard.Mater.2010,181,432.doi:10.1016/j.jhazmat.2010.05.029

    (10)Hickey,M.A.;Chavez,D.E.;Naud,D.Low-Smoke Pyrotechnic Compositions.US Patent,6312537,2001.

    (11)Li,S.W.;Zhao,F.Q.;Yuan,C.;Luo,Y.;Gao,Y.Chin.J.Solid R ocket Tech.2002,25,36. [李上文,趙鳳起,袁 潮,羅 陽(yáng),高 茵.固體火箭技術(shù),2002,25,36.]

    (12)Fan,X.Z.;Li,J.Z.;Zhang,L.Y.;Wang,B.Z.;Liu,X.G.Chin.J.Energ.Mater.2007,15,316.[樊學(xué)忠,李吉禎,張臘瑩,王伯周,劉小剛.含能材料,2007,15,316.]

    (13)Zhao,F.Q.;Chen,P.;Li,S.W.;Wang,B.C.;Du,H.;Deng,M.Z.Acta A rmamentarii.2004,25,30.[趙鳳起,陳 沛,李上文,王百成,杜 恒,鄧敏智.兵工學(xué)報(bào),2004,25,30.]

    (14)Deng,M.Z.;Du,H.;Zhao,F.Q.;Luo,Y.;Yuan,C.J.Solid Rocket.Tech nol.2003,26,53.[鄧敏智,杜 恒,趙鳳起,羅陽(yáng),袁 潮.固體火箭技術(shù),2003,26,53.]

    (15)Singh,G.;Felix,P.J.Hazard.Mater.2002,A90,1.

    (16)Denisyuk,A.P.;Demidova,L.A.Comb ustion,E xplosion,and S hock Waves 2004,40,311.doi:10.1023/B:CESW.0000028944.73795.0e

    (17)Zhu,C.G.;Wang,F.W.;Chu,D.B.Chin.J.Inorg.Chem.2007,23,335.[朱傳高,王鳳武,褚道葆.無(wú)機(jī)化學(xué)學(xué)報(bào),2007,23,335.]

    (18)Dong,X.F.;Li,Y.;Xiong,X.F.;Cao,R.L.Chin.J.Expl.Prop.2011,34,69.[董秀芳,李 煜,熊賢峰,曹瑞林.火炸藥學(xué)報(bào),2011,34,69.]

    (19)Zhao,F.Q.;Gao,H.X.;Luo,Y.;Hu,R.Z.;Pei,C.;Gao,S.L.;Yang,X.W.;Shi,Q.Z.J.Therm.Anal.Cal.2006,85,791.doi:10.1007/s10973-005-7455-4

    (20)Yi,J.H.;Zhao,F.Q.;Xu,S.Y.;Gao,H.X.;Hu,R.Z.Chem.Res.Chin.Univ.2008,24,1.doi:10.1016/S1005-9040(08)60001-X

    (21)Yi,J.H.;Zhao,F.Q.;Xu,S.Y.;Hang,L.Y.;Gao,H.X.;Hu,R.Z.J.Hazard.Mater.2009,165,853.doi:10.1016/j.jhazmat.2008.10.107

    (22)Yi,J.H.;Zhao,F.Q.;Xu,S.Y.;Gao,H.X.;Hu,R.Z.;Hao,H.X.;Pei,Q.;Gao,Y.Acta Phys.-Chim.Sin.2007,23,1316.[儀建華,趙鳳起,徐司雨,高紅旭,胡榮祖,郝海霞,裴 慶,高 茵.物理化學(xué)學(xué)報(bào),2007,23,1316.]doi:10.1016/S1872-1508(07)60065-5

    (23)Yi,J.H.;Zhao,F.Q.;Xu,S.Y.;Zhang,L.Y.;Ren,X.N.;Gao,H.X.;Hu,R.Z.J.Therm.Anal.Cal.2009,95,381.doi:10.1007/s10973-008-9241-6

    (24)Yi,J.H.;Zhao,F.Q.;Ren,Y.H.;Wang,B.Z.;Zhou,C.;Ren,X.N.;Xu,S.Y.;Hao,H.X.;Hu,R.Z.J.Therm.Anal.Cal.2011,104,1029.doi:10.1007/s10973-010-1258-y

    (25)Hu,R.Z.;Gao,S.L.;Zhao,F.Q.;Shi,Q.Z.;Zhang,T.L.;Zhang,J.J.Th ermal Analysis Kinetics,2nd ed.;Science Press:Beijing,2008;pp 322-334.[胡榮祖,高勝利,趙鳳起,史啟楨,張同來(lái),張建軍.熱分析動(dòng)力學(xué).北京:科學(xué)出版社,2008:322-334.]

    (26)Zhao,F.Q.;Hu,R.Z.;Gao,H.X.;Ma,H.X.T hermochemical P roperties,Nonisothermal Decomposition R eaction Kinetics and Quantum Chemical Investigation of 2,6-Diamino-3,5-dinitropyrazine-1-oxide(LLM-105),New Developments in Hazardous Materials Research;Nova Science Publishers Inc.:New York,2006;Chapter 4.

    (27)Ma,H.X.;Song,J.R.;Zhao,F.Q.;Hu,R.Z.;Xiao,H.M.J.Phys.Chem.A 2007,111,8642.doi:10.1021/jp073092o

    (28)Zhang,T.L.;Hu,R.Z.;Xie,Y.;Li,F.P.Thermochim.Acta 1994,244,171.doi:10.1016/0040-6031(94)80216-5

    (30)Hu,R.Z.;Zhang,H.;Xia,Z.M.;Guo,P.J.;Gao,S.L.;Shi,Q.Z.;Lu,G.E.;Jiang,J.Y.Chin.J.Energ.Mater.2003,11,130.[胡榮祖,張 海,夏志明,郭鵬江,高勝利,史啟禎,路桂娥,江勁勇.含能材料,2003,11,130.]

    (31)Chen,P.;Zhao,F.Q.;Luo,Y.;Hu,R.Z.;Gao,S.L.;Zheng,Y.M.;Deng,M.Z.;Gao,Y.Chinese Journal of Ch emistry 2004,22,1056.

    (32)Yi,J.H.;Zhao,F.Q.;Hong,W.L.;Xu,S.Y.;Hu,R.Z.;Chen,Z.Q.;Zhang,L.Y.J.Hazard.Mater.2009,11,021.

    (33)Li,Z.L.;Ma,Z.L.;Xiao,Z.L.;Zhang,X.Z.Ch in.J.E nerg.Mater.2006,14,95.[李志良,馬忠亮,肖忠良,張續(xù)柱.含能材料,2006,14,95.]

    (34)Wang,H.;Zhao,F.Q.;Gao,H.X.;Li,S.W.;Hao,H.X.Chin.J.Energ.Mater.2006,14,45.[王 晗,趙鳳起,高紅旭,李上文,郝海霞.含能材料,2006,14,45.]

    (35)Hong,W.L.;Liu,J.H.;Zhao,F.Q.;Li,Y.M.;Luo,Z.K.Acta Chim.S in.2005,63,249.[洪偉良,劉劍洪,趙鳳起,李玉梅,羅仲寬.化學(xué)學(xué)報(bào),2005,63,249.]

    (36)Hong,L.W.;Li,L.L.;Zhao,F.Q.;Tian,D.Y.;Liu,J.H.;Zhang,P.X.J.Solid Rocket.Technol.2007,30,135. [洪良偉,李琳琳,趙鳳起,田德余,劉劍洪,張陪新.固體火箭,2007,30,135.]

    (37)Hong,L.W.;Zhao,F.Q.;Liu,J.H.;Tian,D.Y.;Luo,Z.K.;Chen,P.;Luo,Y.Chin.J.Inorg.Ch em.2004,20,996.[洪良偉,趙鳳起,劉劍洪,田德余,羅仲寬,陳 沛,羅 陽(yáng).無(wú)機(jī)化學(xué)學(xué)報(bào),2004,20,996.]

    (38)Yi,J.H.;Zhao,F.Q.;Gao,H.X.;Xu,S.Y.;Wang,M.C.;Hu,R.Z.J.Hazard.Mater.2008,153,261.doi:10.1016/j.jhazmat.2007.08.064

    麻豆久久精品国产亚洲av| 久久国产精品人妻蜜桃| 超碰av人人做人人爽久久| a级毛片a级免费在线| 啪啪无遮挡十八禁网站| 国产精品永久免费网站| 网址你懂的国产日韩在线| 国产三级在线视频| 麻豆国产97在线/欧美| 中国美女看黄片| 99热这里只有是精品在线观看| 日韩一区二区视频免费看| 成年女人看的毛片在线观看| 亚洲自偷自拍三级| 春色校园在线视频观看| 人妻丰满熟妇av一区二区三区| 国产精品98久久久久久宅男小说| 成人国产麻豆网| а√天堂www在线а√下载| 日本黄色片子视频| 亚洲性久久影院| 人人妻,人人澡人人爽秒播| 哪里可以看免费的av片| 亚洲欧美清纯卡通| 真实男女啪啪啪动态图| 中文亚洲av片在线观看爽| 九九久久精品国产亚洲av麻豆| 亚洲av熟女| 又爽又黄无遮挡网站| 免费av观看视频| 久久热精品热| 精品久久久久久成人av| 日本成人三级电影网站| 国内揄拍国产精品人妻在线| 午夜老司机福利剧场| 国产久久久一区二区三区| 欧美日韩瑟瑟在线播放| 99久久精品热视频| 成人无遮挡网站| 亚洲avbb在线观看| 一级黄色大片毛片| 热99在线观看视频| 禁无遮挡网站| 国产在线男女| 成人国产一区最新在线观看| 亚洲av一区综合| 国产亚洲欧美98| 在线观看舔阴道视频| 午夜福利在线在线| 校园人妻丝袜中文字幕| 干丝袜人妻中文字幕| 色5月婷婷丁香| av中文乱码字幕在线| 久久久精品欧美日韩精品| 午夜激情福利司机影院| 国产精品亚洲美女久久久| 亚洲美女黄片视频| 99久久无色码亚洲精品果冻| 亚洲av成人精品一区久久| 亚洲一区二区三区色噜噜| 日本精品一区二区三区蜜桃| 51国产日韩欧美| 波多野结衣巨乳人妻| 91午夜精品亚洲一区二区三区 | 日本一本二区三区精品| 国产爱豆传媒在线观看| 有码 亚洲区| 乱系列少妇在线播放| 国产在线男女| 亚洲自拍偷在线| 一夜夜www| 精品日产1卡2卡| 亚洲国产精品合色在线| 他把我摸到了高潮在线观看| 99在线视频只有这里精品首页| 观看免费一级毛片| 嫩草影视91久久| 亚洲精品国产成人久久av| 亚洲人成伊人成综合网2020| 欧美激情久久久久久爽电影| 国产精品国产三级国产av玫瑰| 日本一二三区视频观看| 小蜜桃在线观看免费完整版高清| 婷婷精品国产亚洲av在线| 亚洲最大成人av| 成年免费大片在线观看| 网址你懂的国产日韩在线| www.色视频.com| 性色avwww在线观看| 真实男女啪啪啪动态图| av在线观看视频网站免费| 我要搜黄色片| 精品人妻一区二区三区麻豆 | 大型黄色视频在线免费观看| 中文字幕熟女人妻在线| 蜜桃久久精品国产亚洲av| 欧美区成人在线视频| 99热只有精品国产| 亚洲人成伊人成综合网2020| 特级一级黄色大片| 精品一区二区免费观看| 俺也久久电影网| 联通29元200g的流量卡| 一级a爱片免费观看的视频| а√天堂www在线а√下载| 亚洲久久久久久中文字幕| 亚洲专区国产一区二区| 精品久久久久久久久av| 99久国产av精品| 精品福利观看| 亚洲av美国av| 夜夜夜夜夜久久久久| 免费看光身美女| 热99在线观看视频| 国产欧美日韩一区二区精品| 久久久久久久久久成人| 精品乱码久久久久久99久播| 免费在线观看成人毛片| 国语自产精品视频在线第100页| avwww免费| 亚洲精品粉嫩美女一区| 欧美日韩黄片免| 国产一区二区三区av在线 | 精品久久久噜噜| 欧美精品啪啪一区二区三区| 不卡一级毛片| 热99在线观看视频| 亚洲国产欧美人成| www.www免费av| 免费看av在线观看网站| 99热精品在线国产| 九九在线视频观看精品| 国产一区二区在线观看日韩| 噜噜噜噜噜久久久久久91| 久久午夜亚洲精品久久| 久久精品国产亚洲av天美| 亚洲性久久影院| 中文字幕av成人在线电影| 免费不卡的大黄色大毛片视频在线观看 | 成人国产麻豆网| 成人国产麻豆网| 久久久久久国产a免费观看| 午夜福利在线观看吧| 啦啦啦啦在线视频资源| 免费观看精品视频网站| 欧美日韩综合久久久久久 | 亚洲无线在线观看| 国产真实乱freesex| 精品久久久久久久久久久久久| 欧美激情久久久久久爽电影| 亚洲精品在线观看二区| 亚洲国产色片| 国产大屁股一区二区在线视频| 人妻夜夜爽99麻豆av| 美女xxoo啪啪120秒动态图| 干丝袜人妻中文字幕| 国产精品国产高清国产av| 亚州av有码| 亚洲成人久久爱视频| 欧美日韩国产亚洲二区| 国产精品一区二区三区四区久久| 精品午夜福利视频在线观看一区| 日本黄色视频三级网站网址| 日韩强制内射视频| 最近最新中文字幕大全电影3| 日韩精品青青久久久久久| 日本爱情动作片www.在线观看 | 在线观看免费视频日本深夜| 美女xxoo啪啪120秒动态图| 直男gayav资源| 日本黄大片高清| 偷拍熟女少妇极品色| 亚洲不卡免费看| 身体一侧抽搐| 免费搜索国产男女视频| 午夜日韩欧美国产| 国产精品,欧美在线| 日韩 亚洲 欧美在线| 欧美日韩瑟瑟在线播放| 成人特级av手机在线观看| 免费看日本二区| 一区二区三区激情视频| 极品教师在线免费播放| 日韩大尺度精品在线看网址| 久久亚洲精品不卡| 亚洲欧美激情综合另类| 亚洲电影在线观看av| 极品教师在线免费播放| 九色国产91popny在线| 久久久午夜欧美精品| 亚洲国产精品成人综合色| 国产成人a区在线观看| 国产精品福利在线免费观看| 精品一区二区三区视频在线| .国产精品久久| 色哟哟·www| 成人亚洲精品av一区二区| 又紧又爽又黄一区二区| 国国产精品蜜臀av免费| 亚洲天堂国产精品一区在线| 成人三级黄色视频| 成年人黄色毛片网站| 成人永久免费在线观看视频| 五月玫瑰六月丁香| 亚洲图色成人| 深夜a级毛片| 男人的好看免费观看在线视频| 在线播放无遮挡| 91麻豆精品激情在线观看国产| 久久精品国产亚洲网站| 两个人的视频大全免费| 成人无遮挡网站| 欧美日本视频| 亚洲内射少妇av| 老司机福利观看| 成人毛片a级毛片在线播放| 国产黄色小视频在线观看| 久久人妻av系列| 亚洲精品在线观看二区| 午夜精品久久久久久毛片777| 亚洲,欧美,日韩| 亚洲精品色激情综合| 欧美中文日本在线观看视频| 成人毛片a级毛片在线播放| 亚洲国产精品成人综合色| a级一级毛片免费在线观看| 日韩精品有码人妻一区| 欧美3d第一页| 大型黄色视频在线免费观看| 久久午夜亚洲精品久久| 成人国产综合亚洲| 欧美日韩中文字幕国产精品一区二区三区| 老师上课跳d突然被开到最大视频| 免费看a级黄色片| 99久久精品国产国产毛片| 国产精品99久久久久久久久| 色综合站精品国产| 亚洲在线观看片| 一a级毛片在线观看| 精品人妻熟女av久视频| 欧美区成人在线视频| 我要搜黄色片| 免费av观看视频| 精品乱码久久久久久99久播| 亚洲图色成人| 国产不卡一卡二| 日韩 亚洲 欧美在线| 麻豆成人av在线观看| 最近视频中文字幕2019在线8| 国产在视频线在精品| 2021天堂中文幕一二区在线观| 国产亚洲精品久久久com| 国内精品一区二区在线观看| 18禁在线播放成人免费| 国产精品野战在线观看| 国产高清视频在线观看网站| 观看免费一级毛片| 免费av毛片视频| 干丝袜人妻中文字幕| 成人av一区二区三区在线看| 在线观看午夜福利视频| 亚洲色图av天堂| 听说在线观看完整版免费高清| 亚洲在线观看片| 成人国产麻豆网| 两人在一起打扑克的视频| 亚洲中文字幕一区二区三区有码在线看| 男女之事视频高清在线观看| av在线亚洲专区| 变态另类丝袜制服| 国产精品一区二区免费欧美| 久久婷婷人人爽人人干人人爱| 亚洲成a人片在线一区二区| 色哟哟哟哟哟哟| 免费搜索国产男女视频| 亚洲欧美日韩东京热| 精品久久国产蜜桃| 国内精品久久久久精免费| 亚洲欧美日韩无卡精品| 免费人成视频x8x8入口观看| 欧美国产日韩亚洲一区| av福利片在线观看| 国产一区二区在线观看日韩| 在线观看美女被高潮喷水网站| 成年女人毛片免费观看观看9| 亚洲av二区三区四区| 亚洲av.av天堂| 熟女人妻精品中文字幕| 国产伦一二天堂av在线观看| 男女下面进入的视频免费午夜| 男人的好看免费观看在线视频| 欧美潮喷喷水| 村上凉子中文字幕在线| 日韩av在线大香蕉| 久久国产精品人妻蜜桃| 男人舔奶头视频| 午夜亚洲福利在线播放| 亚洲图色成人| 欧美又色又爽又黄视频| 在线免费十八禁| 国产精品久久久久久久电影| 亚洲精品久久国产高清桃花| 成人高潮视频无遮挡免费网站| 国产精品日韩av在线免费观看| 国产又黄又爽又无遮挡在线| 91麻豆精品激情在线观看国产| 欧美日韩亚洲国产一区二区在线观看| 最好的美女福利视频网| 两人在一起打扑克的视频| 久久热精品热| 国产美女午夜福利| 午夜福利高清视频| 国产美女午夜福利| 两个人的视频大全免费| 久9热在线精品视频| 99视频精品全部免费 在线| 免费人成视频x8x8入口观看| 白带黄色成豆腐渣| 免费搜索国产男女视频| 一个人看的www免费观看视频| 国产伦人伦偷精品视频| 成人永久免费在线观看视频| 日韩一区二区视频免费看| 亚州av有码| 中文字幕人妻熟人妻熟丝袜美| 少妇丰满av| 久久草成人影院| 国产精品福利在线免费观看| 干丝袜人妻中文字幕| 人人妻,人人澡人人爽秒播| 国产精品美女特级片免费视频播放器| 欧美一区二区精品小视频在线| 国产亚洲精品久久久com| 在线观看免费视频日本深夜| 久久久久九九精品影院| 精品一区二区三区视频在线观看免费| 日本一二三区视频观看| 国内精品美女久久久久久| 俺也久久电影网| 日本成人三级电影网站| 亚洲黑人精品在线| 黄色日韩在线| 性色avwww在线观看| av天堂中文字幕网| 99riav亚洲国产免费| 日本成人三级电影网站| 桃红色精品国产亚洲av| 麻豆成人av在线观看| 男女视频在线观看网站免费| 三级男女做爰猛烈吃奶摸视频| 亚洲国产精品成人综合色| 黄色配什么色好看| 99久久无色码亚洲精品果冻| 国产高清不卡午夜福利| 男插女下体视频免费在线播放| 在线a可以看的网站| 最近最新免费中文字幕在线| 麻豆成人av在线观看| 一区二区三区免费毛片| 小说图片视频综合网站| 久久国内精品自在自线图片| 亚洲中文字幕一区二区三区有码在线看| 桃红色精品国产亚洲av| 色哟哟哟哟哟哟| 国产精品嫩草影院av在线观看 | 69av精品久久久久久| 欧美精品啪啪一区二区三区| 男女视频在线观看网站免费| 国产视频一区二区在线看| videossex国产| 国产黄片美女视频| 18禁裸乳无遮挡免费网站照片| 女同久久另类99精品国产91| 男人和女人高潮做爰伦理| 亚洲电影在线观看av| 99久久精品国产国产毛片| 国产午夜福利久久久久久| 亚洲最大成人手机在线| 国内少妇人妻偷人精品xxx网站| 可以在线观看的亚洲视频| 午夜福利高清视频| 97超级碰碰碰精品色视频在线观看| 欧美又色又爽又黄视频| 干丝袜人妻中文字幕| 久久国产乱子免费精品| 欧美极品一区二区三区四区| 99久久精品热视频| 亚洲av成人精品一区久久| 国产男人的电影天堂91| 少妇的逼水好多| 我要看日韩黄色一级片| 少妇熟女aⅴ在线视频| 亚洲七黄色美女视频| 亚洲va日本ⅴa欧美va伊人久久| 精品免费久久久久久久清纯| 欧美不卡视频在线免费观看| 中国美女看黄片| 全区人妻精品视频| 麻豆成人午夜福利视频| 久久精品人妻少妇| 国产69精品久久久久777片| 亚洲乱码一区二区免费版| 色视频www国产| 午夜福利18| 男人狂女人下面高潮的视频| 草草在线视频免费看| 高清在线国产一区| 亚洲国产欧洲综合997久久,| 真人做人爱边吃奶动态| 少妇裸体淫交视频免费看高清| 欧美激情国产日韩精品一区| 免费搜索国产男女视频| av.在线天堂| 亚洲欧美日韩高清专用| 午夜福利在线在线| 女的被弄到高潮叫床怎么办 | 人妻丰满熟妇av一区二区三区| 麻豆国产97在线/欧美| 国产精品人妻久久久久久| 一级毛片久久久久久久久女| 伦理电影大哥的女人| 亚洲精品久久国产高清桃花| 12—13女人毛片做爰片一| 三级毛片av免费| 久久人人精品亚洲av| 午夜福利成人在线免费观看| 丰满人妻一区二区三区视频av| 午夜精品一区二区三区免费看| 哪里可以看免费的av片| 色5月婷婷丁香| 欧美zozozo另类| 女同久久另类99精品国产91| 简卡轻食公司| 深夜a级毛片| 亚洲人成网站在线播| 亚洲综合色惰| 成人一区二区视频在线观看| 18禁在线播放成人免费| 国产精品98久久久久久宅男小说| 在现免费观看毛片| 人人妻人人澡欧美一区二区| 精品久久久久久成人av| 88av欧美| 在线播放无遮挡| 亚洲欧美日韩卡通动漫| 免费观看在线日韩| 很黄的视频免费| 91av网一区二区| 久久精品国产亚洲av天美| 美女高潮喷水抽搐中文字幕| 人人妻人人看人人澡| 最近中文字幕高清免费大全6 | а√天堂www在线а√下载| 波野结衣二区三区在线| 久久久国产成人免费| av中文乱码字幕在线| 校园春色视频在线观看| 九九久久精品国产亚洲av麻豆| 成人美女网站在线观看视频| 国产精品自产拍在线观看55亚洲| 久久国内精品自在自线图片| 日本黄大片高清| 非洲黑人性xxxx精品又粗又长| 搡老岳熟女国产| 欧美高清性xxxxhd video| 美女黄网站色视频| 久久久精品大字幕| 美女高潮喷水抽搐中文字幕| 天堂影院成人在线观看| 精品久久久久久,| 午夜激情福利司机影院| 欧美日韩黄片免| 嫩草影院入口| 91在线观看av| 国产精品三级大全| 日韩大尺度精品在线看网址| 精品乱码久久久久久99久播| 国产久久久一区二区三区| 亚洲国产精品sss在线观看| xxxwww97欧美| 婷婷精品国产亚洲av在线| 日韩 亚洲 欧美在线| 老熟妇仑乱视频hdxx| 1024手机看黄色片| 麻豆久久精品国产亚洲av| 男人和女人高潮做爰伦理| av.在线天堂| 午夜福利视频1000在线观看| 在线天堂最新版资源| 在线观看午夜福利视频| 亚洲专区国产一区二区| 欧美黑人巨大hd| 亚洲色图av天堂| 欧美成人a在线观看| 色综合色国产| 亚洲aⅴ乱码一区二区在线播放| 欧美三级亚洲精品| 美女 人体艺术 gogo| 3wmmmm亚洲av在线观看| 中文字幕免费在线视频6| 欧美日韩精品成人综合77777| 嫩草影院新地址| 欧美极品一区二区三区四区| 久久国产乱子免费精品| 99热这里只有是精品在线观看| 成人国产一区最新在线观看| 男人和女人高潮做爰伦理| av.在线天堂| 一边摸一边抽搐一进一小说| 人妻制服诱惑在线中文字幕| 少妇的逼好多水| 午夜视频国产福利| 精品久久久久久久久av| 久久99热6这里只有精品| 久久欧美精品欧美久久欧美| 午夜爱爱视频在线播放| 免费高清视频大片| 国内久久婷婷六月综合欲色啪| av国产免费在线观看| 国产亚洲欧美98| 日韩人妻高清精品专区| 日韩 亚洲 欧美在线| 大型黄色视频在线免费观看| 免费人成视频x8x8入口观看| 搞女人的毛片| 欧美性感艳星| 欧美高清成人免费视频www| 亚洲性夜色夜夜综合| 国产午夜精品论理片| 嫩草影院精品99| 国产精品99久久久久久久久| 日日干狠狠操夜夜爽| 成人国产综合亚洲| 亚洲av熟女| 婷婷亚洲欧美| 丝袜美腿在线中文| 国产精品乱码一区二三区的特点| 日日干狠狠操夜夜爽| 色综合色国产| 99国产精品一区二区蜜桃av| 黄色一级大片看看| 一区二区三区四区激情视频 | 亚洲美女视频黄频| 久久精品国产鲁丝片午夜精品 | 亚洲男人的天堂狠狠| 成人三级黄色视频| 日本三级黄在线观看| 我的女老师完整版在线观看| 精品久久久久久久久久免费视频| 国产成年人精品一区二区| 午夜精品一区二区三区免费看| 亚洲熟妇熟女久久| 日日摸夜夜添夜夜添小说| 欧美性猛交╳xxx乱大交人| 日韩国内少妇激情av| 亚洲欧美日韩卡通动漫| 国产精品乱码一区二三区的特点| 国产高清有码在线观看视频| 两性午夜刺激爽爽歪歪视频在线观看| 久久亚洲真实| 亚洲人成网站在线播放欧美日韩| 91av网一区二区| 国产亚洲精品久久久久久毛片| 草草在线视频免费看| 在线免费十八禁| 国产乱人伦免费视频| 亚洲国产欧洲综合997久久,| 亚洲在线自拍视频| 亚洲国产精品sss在线观看| 一边摸一边抽搐一进一小说| 欧美+日韩+精品| 99久久中文字幕三级久久日本| 可以在线观看的亚洲视频| 夜夜看夜夜爽夜夜摸| 亚洲av一区综合| 在线播放无遮挡| 亚洲国产欧洲综合997久久,| 九色国产91popny在线| 少妇人妻一区二区三区视频| 午夜精品久久久久久毛片777| 女同久久另类99精品国产91| 免费搜索国产男女视频| 成人国产综合亚洲| 色精品久久人妻99蜜桃| 国产亚洲精品久久久久久毛片| 亚洲欧美清纯卡通| 欧美最新免费一区二区三区| 精品免费久久久久久久清纯| 在线观看舔阴道视频| a级毛片免费高清观看在线播放| 国产 一区 欧美 日韩| 久久精品国产亚洲av香蕉五月| 午夜福利成人在线免费观看| 美女大奶头视频| 欧美中文日本在线观看视频| 免费看a级黄色片| 麻豆精品久久久久久蜜桃| 午夜福利高清视频| 麻豆国产av国片精品| 不卡一级毛片| 国产精品嫩草影院av在线观看 | 全区人妻精品视频| 久久午夜亚洲精品久久| 亚洲专区中文字幕在线| 欧美中文日本在线观看视频| 久久精品国产亚洲av香蕉五月| 人妻丰满熟妇av一区二区三区| 亚洲av日韩精品久久久久久密| 国产精品野战在线观看| 噜噜噜噜噜久久久久久91| 中文字幕高清在线视频| 日韩强制内射视频| 伦精品一区二区三区| 欧美成人a在线观看| 久久香蕉精品热|