N-脒基脲二硝酰胺放热分解反应的动力学行为

物理化学学报(Wuli Huaxue Xuebao )Acta Phys.⁃Chim.Sin .,2008,24(3)：453-458Received:August 14,2007;Revised:December 11,2007;Published on Web:January 23,2008.∗Corresponding author.Email:npecc@;Tel:+8629⁃88291663ⒸEditorial office of Acta Physico ⁃Chimica Sinica[Article]March N ⁃脒基脲二硝酰胺放热分解反应的动力学行为高红旭1张海2赵凤起1,∗胡荣祖1马海霞3徐抗震3仪建华1徐司雨1高茵1(1西安近代化学研究所,西安710065;2西北大学数学系,西安710069;3西北大学化工学院,西安710069)摘要：用DSC 和微热量仪研究了N ⁃脒基脲二硝酰胺(GUDN)的放热分解反应动力学行为和比热容,计算得到程序升温下GUDN 主放热分解反应的动力学参数(活化能E a 和指前因子A )、自加速分解温度(T SADT )、绝热条件下达到最大分解反应速率的时间(t TM Rad )和至爆时间(t TIad ).结果表明,在非等温DSC 条件下,GUDN 的热分解过程可用经验级数自催化动力学方程d α/d t =1018.49exp(-195500/RT )(1-α)0.81+1018.00exp(-177000/RT )α1.29(1-α)0.71描述.热分解转热爆炸的临界温升速率为0.1236K ·h -1.所得的T SADT 、t TMRad 和t TIad 值分别为473.95K 、2.24s 和3.51s.关键词：N ⁃脒基脲二硝酰胺;自催化分解;动力学参数;临界温升速率;热爆炸;非等温DSC中图分类号：O642;O643Kinetic Behaviour of the Exothermic Decomposition Reaction ofN ⁃Guanylurea DinitramideGAO Hong ⁃Xu 1ZHANG Hai 2ZHAO Feng ⁃Qi 1,∗HU Rong ⁃Zu 1MA Hai ⁃Xia 3XU Kang ⁃Zhen 3YI Jian ⁃Hua 1XU Si ⁃Yu 1GAO Yin 1(1Xi ′an Modern Chemistry Research Institute,Xi ′an 710065,P.R.China ;2Department of Mathematics,Northwest University,Xi ′an 710069,P.R.China;3College of Chemical Engineering,Northwest University,Xi ′an 710069,P.R.China )Abstract ：The kinetic behaviour of the exothermic decomposition reaction and the specific heat capacity of N ⁃guanylurea dinitramide (GUDN)were determined by DSC and mircocalorimeter.Its kinetic parameters of the major exothermic decomposition reaction in a temperature ⁃programmed mode [the apparent activation energy (E a )and pre ⁃exponential factor (A )],self ⁃accelerating decomposition temperature (T SADT ),time to maximum rate (t TM rad ),and time ⁃to ⁃ignition (t TIad )under adiabatic conditions were calculated.The results showed that under non ⁃isothermal DSC conditions,the thermal decomposition of GUDN could be described by the empiric ⁃order autocatalytic equation:d α/d t =1018.49×exp(-195500/RT )(1-α)0.81+1018.00exp (-177000/RT )α1.29(1-α)0.71,and the value of the critical rate of temperature rise in GUDN was 0.1236K ·h -1when the decomposition reaction converted into thermal explosion.The values of T SADT ,t TMRad ,and t TIad were 473.95K,2.24s,and 3.51s,respectively.Key Words ：GUDN;Autocatalytic decomposition;Kinetic parameters;Critical rate of temperature rise;Thermal explosion;Non ⁃isothermal DSCN ⁃Guanylurea dinitramide (GUDN)is a new energetic oxidiz-er with higher energy and lower sensitivities.Its crystal density is 1.755g ·cm -3,detonation velocity is about 8210m ·s -1,specific impulse and pressure exponent are 213.1s and 0.73[1],respec-tively.Therefore,it has the potential for possible use as an ener-gy ingredient of propellants and explosives from the point ofview of the above ⁃mentioned high performances.A number of papers have reported on its preparation [2,3]and properties [4-13],however,its kinetic parameters and critical rate of temperature rise of thermal explosion for the autocatalytic decomposing re-action have not been described unequivocally.The aim of the present work is to obtain more detailed information on the auto-453Acta Phys.⁃Chim.Sin.,2008Vol.24catalytic decomposition of GUDN to fit kinetic models of the re-action and to estimate kinetic parameters,self⁃accelerating de-composition temperature(T SADT),time to maximum rate(t TM Rad) and time⁃to⁃ignition(or explosion)(t Tlad)under adiabatic condi-tions and the critical rate of temperature rise of thermal explo-sion.This is quite useful in the evaluation of its thermal stability under non⁃isothermal condition and in the study of its thermal changes at high temperature.1Theoretical and method1.1Basic theory of decomposition reactionThe enthalpy(q1)of thermal decomposition reaction per unit time for energetic materials(EMs)can be expressed by the e-quation:q1=QVd M dαd t(1) where Q is the enthalpy of the thermal decomposition reaction in J·mol-1,V the volume of EMs loaded in cm3,d the loading den-sity in g·cm-3,M the mole mass of EMs in g·mol-1and dα/d t the reaction rate in s-1.The thermal decomposition,as an autocatalytic reaction,can be described by the following equations:k1A➝B(2) k2A+B➝2B(3) where A represents the initial reactant and B the thermal decom-position product.The rate expression that corresponds to this scheme isdαd t=k1(1-α)m+k2αn(1-α)p(4) whereαstands for the conversion degree,for DSC curve,α=H/H o,H o is the total exothermicity of the EMs(corresponding to the global area under the DSC curve)and H is the reaction heat in a certain time(corresponding to the partial area under the DSC curve);k1=A1exp(-E a1/RT),k2=A2exp(-E a2/RT),where A1and A2are the pre⁃exponential factors,E a1and E a2the activa-tion energies for the autocatalytic reaction,R is the gas constant, T the temperature,t the time;m,n and p are the apparent reac-tion orders.Substituting Eq.(4)into Eq.(1)givesq1=QVd M[A1exp-E a1RT()(1-α)m+A2exp-E a2RT()αn(1-α)p](5)At the same time,the amount of heat(q2)transferred by the wall of the reactor to surrounding medium in unit time isq2=k′(T-T c)S(6) where k′is an overall heat transfer coefficient in J·cm-2·K-1·s-1; T c the temperature of the reaction wall and surroundings accord-ing to the linear relationship T c=T o+βt,whereβis the heating rate K·min-1,T o the initial temperature at which the DSC curve devi-ates from the baseline in K;S the external surface of the loaded sample in cm2.1.2Transition from decomposition to thermal explosion With the boundary conditions of thermal explosion,Eq.(5)be-comesq1|Tb=QVd M[k1b(1-αb)m+k2bαn b(1-αb)p](7) whereαb is the value ofαcorresponding to T b,k1b=A1exp(-E a1/ RT b),k2b=A2exp(-E a2/RT b),where T b is the critical temperature of thermal explosion of EMs in K and Eq.(6)becomesq2|Tb=k′(T b-T e0)S(8) where T e0is the onset temperature in the DSC curve under linear temperature increase condition whenβtends to zero. According to the q1-T and q2-T relations,the sufficient and es-sential conditions from thermal decomposition to thermal explo-sion can be expressed asq1|Tb=q2|T b(9)d q1d T Tb=d q2d T Tb(10)⎧⎩⏐⏐⏐⏐⏐⎨⏐⏐⏐⏐⏐Differentiation of Eq.(5)with respect to t givesd q1d T T=Tb,α=αb=QVd(d T/d t)TbRT b[(k1b E a1(1-αb)m+k2b E a2αn b(1-αb)p)+ (k1b(1-αb)m+k2bαn b(1-αb)p)(k2b n(1-αb)pαn-1b-k2b p(1-αb)p-1αn b-k1b m(1-αb)m-1)]/M(d T/d t)T b(11)where(d T/d t)Tbis the increasing rate of temperature in EMs when thermal decomposition converts into thermal explosion. This is difficult to solve directly from conventional experiments. Differentiation of Eq.(6)with respect to t givesd q2d T T=Tb=k′S(d T/d t)Tbd Td t()T b-β[](12)Combining Eqs.(7)-(9),yieldsQVdM[k1b(1-αb)m+k2bαn b(1-αb)p]=k′S(T b-T e0)(13) Combining Eqs.(10)-(12),yieldsQVd(d T/d t)T bRT2b[(k1b E a1(1-αb)m+k2b E a2αn b(1-αb)p)+(k1b(1-αb)m+k2bαn b(1-αb)p)(k2b n(1-αb)pαn-1b-k2b p(1-αb)p-1αn b-k1b m(1-αb)m-1)]/M(d T/d t)T b=k′S(d T/d t)T b d T d t()T b-β[](14)As the thermal explosion starts,(d T/d t)T b>>β,and Eq.(14)may be simplified to the following form:QVd(d T/d t)T bRT2b[(k1b E a1(1-αb)m+k2b E a2αn b(1-αb)p)+(k1b(1-αb)m+k2bαn b(1-αb)p)(k2b n(1-αb)pαn-1b-k2b p(1-αb)p-1αn b-k1b m(1-αb)m-1)]/M(d T/d t)T b=k′S(15) Combining Eqs.(13)and(15),we getd Td t()T b={(T b-T e0)(k1b(1-αb)m+k2bαn b(1-αb)p)(k2b n(1-αb)pαn-1b-k2b p(1-αb)p-1αn b-k1b m(1-αb)m-1)}/{(k1b(1-αb)m+k2bαn b(1-αb)p-(T b-T e0)(k1b E a1RT2b(1-αb)m+k2b E a2RT2bαn b(1-αb)p}(16) Equation(16)is the relation formula for estimating the critical rate of temperature rise in EMs when the apparent empiric⁃order autocatalytic decomposition converts into thermal explosion. Once the values of E a1,E a2,A1,A2,T e0,T b,αb,m,n,and p have been calculated from an analysis of the DSC curves under the454No.3GAO Hong ⁃Xu et al .：Kinetic Behaviour of the Exothermic Decomposition Reaction of N ⁃Guanylurea Dinitramidesame experimental conditions,the corresponding value of (d T /d t )T bcan then be obtained from Eq.(16).1.3Method of computing kinetic parametersIn order to obtain the values of A 1,A 2,E a1,E a2,αb ,m ,n,and p needed for solving Eq.(16)obtained from Eq.(4),combing Eq.(4)and α=H /H 0,we obtaind H d t=H 0A 1e -E a1/RT (1-α)m +H 0A 2e -E a2/RT αn (1-α)p(17)Where d T d t,T ,α()is a three ⁃dimension data vector,(A 1,A 2,E a1,E a2,m ,n ,p )is a seve n ⁃dimension vector about parameters which would be estimated.Setting ζ=(T ,α)(18)andθ=(A 1,A 2,E a1,E a2,m ,n ,p )=(θ1,θ2,θ3,θ4,θ5,θ6,θ7)(19)the Eq.(17)may be denoted asd H d t=f (T ,α,A 1,A 2,E a1,E a2,m ,n ,p )=f (ζ,θ)(20)Substituting the original data d Td t ()i ,T i ,αi[]i =1,2,…,L into Eq.(20)givesd H d t=f (T i ,αi ,A 1,A 2,E a1,E a2,m ,n ,p )=f (T i ,αi,θ)i =1,2,…,L (21)In order to analyze the non ⁃linear function f (T i ,α,θ)about θ=(A 1,A 2,E a1,E a2,m ,n ,p ),the Taylor expansion of Eq.(21)at theinitial point θ(0)=(A (0)1,A (0)2,E (0)a1,E (0)a2,m (0),n (0),p (0))and reserving the first item and the second item is usedd H d t=f (ζ,θ(0))+əf (ζ,θ)əA 1θ=θ(0)(A 1-A (0)1)+əf (ζ,θ)əA 2θ=θ(0)(A 2-A (0)2)+əf (ζ,θ)əE a1θ=θ(0)(E a1-E (0)a1)+əf (ζ,θ)əE a2θ=θ(0)(E a2-E (0)a2)+əf (ζ,θ)əm θ=θ(0)(m -m (0))+əf (ζ,θ)ənθ=θ(0)(n -n (0))+əf (ζ,θ)əpθ=θ(0)(p -p (0))(22)where d H d t is a linear function as (A 1-A (0)1),(A 2-A (0)2),(E a1-E (0)a1),(E a2-E (0)a2),(m -m (0)),(n -n (0))and (p -p (0)).Setting θ(l +1)=θ(l )+γ(l )(l =0,1,2,…)and substituting the origins data d Hd t ()i ,T i ,αi []into Eq.(22)gived H d t ()=f (T i ,αi ,θ(l ))+7j =1∑əf (T i ,αi ,θ)əθj θ=θ(l )(θ(l +1)j -θ(l )j )(23)Then the mean ⁃square procedure is applied by taking minimalvalues of evaluation function SS (θ)=Li =1∑d H d t ()i-f (T i,αi,θ(l ))-7j =1∑əf (T i,αi,θ)əθjθ=θ(l )(θj -θ(l )j )[]2=note Li =1∑d H d t()i-f (T i,αi,θ(l ))-7j =1∑X (l )ijγ(l )j[]2(24)LettingY (l )=d H d t ()1-f (T 1,α1,θ(l ))d H d t ()2-f (T 2,α2,θ(l ))…d H d t ()L-f (T L ,αL ,θ(l ))⎡⎣⎢⎢⎢⎢⎢⎢⎢⎢⎢⎢⎢⎢⎢⎢⎢⎢⎢⎢⎢⎤⎦⎥⎥⎥⎥⎥⎥⎥⎥⎥⎥⎥⎥⎥⎥⎥⎥⎥⎥⎥X (l )=X (l )11…X (l )17X (l )21…X (l )27…X (l )L 1…X (l )L 7⎡⎣⎢⎢⎢⎢⎢⎢⎢⎢⎢⎢⎢⎤⎦⎥⎥⎥⎥⎥⎥⎥⎥⎥⎥⎥γ(l )=γ(l )1γ(l )2γ(l )7⎡⎣⎢⎢⎢⎢⎢⎢⎢⎢⎢⎢⎢⎤⎦⎥⎥⎥⎥⎥⎥⎥⎥⎥⎥⎥=θ1-θ(l )1θ2-θ(l )2θ7-θ(l )7⎡⎣⎢⎢⎢⎢⎢⎢⎢⎢⎢⎢⎢⎤⎦⎥⎥⎥⎥⎥⎥⎥⎥⎥⎥⎥where γ(l )j =θj -θ(l )j ,X (l )ij =əf (T i ,αi ,θ)əθjθ=θ(l )Under the condition of the existence of (X (l )′X (l )),we have(X (l )′ij X (l ))γ(l )=X (l )Y (l )l =0,1,2, (25)Letting A (0)1,A (0)2,E (0)a1,E (0)a2,m (0),n (0),and p (0)as an initial values and using these values,the value of θ(1)=θ(0)+γ(0)may be calculat-ed.This modified value of θ(1)is used as an initial value for the next calculation which yields another modified value of θ(2)=θ(1)+γ(1).Thus after satisfying the condition of Eq.(26)seven consis-tent estimation values in Eq.(27)will be obtained.θ(l +1)j -θ(l )j <δ(j =1,2,…7)(26)δ[14].θ^=θ(l +1)=(A (l +1)1,A (l +1)2,E (l +1)a1,E (l +1)a2,m (l +1),n (l +1),p (l +1))(27)1.4Estimation of adiabatic time ⁃to ⁃explosionIf E a1≈E a2,A 1≈A 2and m ≈p ≈1in Eq.(4),and the catalyst concentration achieves a stationary state:αcat ≈const.(28)Eq.(4)becomesd αd t=(k 1+k 2α)(1-α)≡k (1-α)(29)Under the adiabatic condition,the differential equation [15,16]de-scribing the time ⁃temperature relation of this one ⁃order exother-mal decomposition with an Arrhenius temperature dependence isC p d T d t=Q (1-α)A exp(-E /RT )(30)where C p ,Q ,A and E are the specific heat capacity,heat of reac-tion,pre ⁃exponential constant and activation energy,respective-ly,R is the gas constant,T is the absolute temperature,t is the time,αis the fraction of substance decomposed and can be ex-pressed as a function of temperatureα=TT 0∫C p Q d T =TT 0∫a+bT Qd T (31)where C p =a +bT ,on rearranging and integrating Eq.(30),we ob-taint =1QA T T 0∫a+bT 1-αe E /RT d T =1QA T T 0∫(a+bT )e E /RT1-TT 0∫(a+bT )Qd T []d T =1QAT T 0∫(a+bT )e E /RT1-1QT p 0T 00or e0∫(a+bT )d T[]d T455Acta Phys.鄄Chim.Sin.,2008Vol.24=1QATT 0∫(a+bT )e E /RT1-1Qa (T p0-T 00or e0)+b 2(T 2p0-T 200or e0)[]{}d T (32)Once the values of a ,b ,Q ,A ,E ,T e0,and T p0,have been calculated from an analysis of the DSC curves,the correspondent value of t can then be obtained from Eq.(32).2Experimental2.1MaterialsGUDN was prepared according to the method reported in the literature [1].It is a pale yellow crystal.m.p.=214℃(decompo-sition).For GUDN(C 2H 7O 5N 7)M r =209.15,w i (calculated):11.48%C,3.34%H,46.89%N;w i (found):11.14%C,3.34%H,46.99%N.IR spectrum(KBr)ν/cm -1:1743(—C(NH)—),1688(—C(O)—),1523,1444(—NO 2—).UV ⁃Vis spectrum(H 2O),λmax :282.5,212.0nm.The analytical results show that it has the composition of C 2H 7O 5N 7.2.2Instruments and conditionsIn the present experiments,the initial data needed for calculating all the kinetic parameters were obtained using a differentialscanningcalorimeter(TA,USA)with an aluminum cell.The conditions of the DSC analyses were:sample mass,about 1mg;heating rates,2.5,5,10and 15K ·mi n -1;atmosphere,N 2gas;reference sample,α⁃Al 2O 3.DSC curves obtained under the same conditions overlap with each other,indicating that the reproducibility of tests is satisfactory.Specific heat capacity of GUDN was determined by a mircocalorimeter Micro ⁃DSC III (SETARAM,France).The mircocalorimeter was calibrated by Joule effect before each experiment.The solution enthalpy of KCl in deionized water was determined at 298.15K with the value of (17.266±0.074)kJ ·mol -1,close to the literature value of (17.241±0.018)kJ ·mol -1[17],indicating that the calorimetric system was reliable.The specific heat capacity of standard sample α⁃Al 2O 3,m =320.60mg,was determined at 298.15K with the value of 79.44kJ ·mol -1,close to the literature of 79.02kJ ·mol -1[18],indicating that the calorimetric system was accurate.The conditions of the mircocalorimeter analyses were:atmosphere,N 2gas;sample mass,608.46mg;the range of temperature,283-353K ,heating rates,0.15K ·min -1.3Results and discussion3.1Decomposition kinetics of GUDNThe typical DSC curve of GUDN is shown in Fig.1.The DSC curve shows that only one exothermic peak before 250℃.A major exothermic peak at 219.17℃is due to the decomposition of GUDN in molten state.The original data (T i ,αi ,i =1,2,…,13)taken from the DSC curve at a heating rate of 10K ·mi n -1are shown in Table 1.The measured values of βi and T e i (i =1,2,…,4),the calculated value of E oe and E op by the Ozawa ′s method [19],the values of E Kp and A K by the Kissinger ′s method [20],the value (T e0)of T e ,which is self ⁃accelerating decomposition temperature (T SADT ),corresponding toβ→0obtained by Eq.(33)taken from literature [21],the value (T p0)of corresponding to β→0,the value of T b obtained by Eq.(34)taken from literature [21],and the value of αb corresponding to T b are shown in Table 2.T e i =T e0+b βi +c β2i ,i =1,2,…4(33)T b =E oe -E 2oe -4E oe RT e0√2R(34)The calculated v alues of E a1,E a2,A 1,A 2,m ,n,and p by the above ⁃mentioned method are given in Table 3.By substituting the values of T e0,T b ,and αb in Table 2,and E a1,E a2,A 1,A 2,m ,n,and p in Table 3into Eq.(16),the value of (d T /d t )T b listed inTable 3is obtained.The results in Tables 2and 3show that:(1)under our non ⁃isothermal DSC conditions,the thermal decomposition of GUDN can be described by the empiric ⁃order autocatalytic equation:d αd t=1018.49exp -195500RT ()(1-α)0.81+1018.00exp -177000RT()α1.29(1-α)0.71(35)(2)The value of the critical rate of temperature rise in GUDN is 0.1236K ·h -1when the decomposition reaction converts into thermal explosion;(3)Because (d T /d t )T b >>β,we conclude thatinFig.1DSC curve for GUDN at a heating rate of 10K ·min -1Table1Basic data of the major exothermic decompositionof GUDN determined by DSC aao o -1Datrum pointT i /K αi (d H i /d t )i /(mJ ·s -1)103(d α/d T )i /(K -1)1467.150.000010.07240.44572469.150.00010.08670.53413471.150.00040.10880.67044473.150.00100.14170.87305475.150.00210.1902 1.1716477.150.00370.2619 1.6137479.150.00660.3881 2.3908481.150.01170.6584 4.0559483.150.0216 1.2507.69810485.150.0420 2.57115.8411487.150.0837 5.28032.5212489.150.161910.8867.0213491.150.291624.60151.2456No.3GAO Hong ⁃Xu et al .：Kinetic Behaviour of the Exothermic Decomposition Reaction of N ⁃Guanylurea Dinitramidethe derivation process of Eq.(16),the assumption of adopting (d T /d t )T b-β(d T /d t )Tb=1is rational.3.2The value of C p for GUDNThe determination and linear ⁃fit result of the specific heat capacity (C p )of GUDN are shown in Fig.2.The result shows,the equation of specific heat capacity of GUDN with temperature is C p =0.2068579+0.003439981T in the temperature range of 283.3-354.9K.3.3Time ⁃to ⁃maximum rate and time ⁃to ⁃explosionunder adiabatic conditionThe adiabatic time ⁃to ⁃explosion (t TIad )and adiabatic time ⁃to ⁃maximum rate (t TM Rad )are the time of energetic material thermal decomposition achieving to explosion and maximum rate under the adiabatic conditions and are two important parameters of assessing the stability and the security of energetic materials.By substituting the values of C p =0.2068579+0.003439981T ,differential mechanism function f (α)=(1-α),E =E K =237706J ·mol -1,A =A K =1023.43s -1,decomposition heat Q =1629J ·g -1,R =8.314J ·mol -1·K -1,α,conversion degree,α=TT 0∫C p Qd T ,integral upper limit,T =T p0=478.25K for t TMRad ,T =T b =482.32K for t Tlad and integral lower limit,T 0=T e0=473.85K into Eq.(32),the valuesof t TM Rad of 2.24s and t TIad of 3.51s of GUDN are obtained.4Conclusions(1)Under our non ⁃isothermal DSC conditions,the thermaldecomposition of GUDN can be described by the empiric ⁃order autocatalytic equation:d αd t=1018.49exp -195500/RT (1-α)0.81+1018.00exp-177000/RT α1.29(1-α)0.71(2)The value of the critical rate of temperature rise in GUDN is 0.1236K ·h -1when the decomposition reaction converts into thermal explosion.(3)The equation of specific heat capacity of GUDN with temperature is C p =0.2068579+0.003439981T in the temperature range of 283.3-354.9K.The values of T SADT ,t TM Rad ,and t Tlad are 473.95K,2.24s,and 3.51s,respectively.References1Zhao,F.Q.;Chen,P.;Yuan,H.A.;Gao,S.L.;Hu,R.Z.;Shi,Q.Z.Chin.J.Chem.,2004,22(2):1362Venkatachalam,S.;Santhosn,G.;Ninan,K.N.Propellants Explosives Pyrotechnics ,2004,29(3):1783Liu,Q.;Wang,B.Z.;Zhang,Z.Z.;Zhu,C.H.;Lian,P.Chin.J.Explo.Prop.,2006,29(1):29[刘愆,王伯周,张志忠,朱春华,廉鹏.火炸药学报,2006,29(1):29]4Yang,T.H.;He,J.X.;Zhang,H.L.Chin.J.Energ.Mater.,2004,12(1):36[杨通辉,何金选,张海林.含能材料,2004,12(1):36]5Östmark,H.;Bemm,U.;Bergman,H.;Langlet,A.Thermochim.Acta ,2002,384:2536Wang,B.Z.;Liu,Q.;Zhang,Z.Z.;Ji,Y.P.;Zhu,C.H.Chin.J.Energ.Mater.,2004,12(2):38[王伯周,刘愆,张志忠,姬月萍,朱春华.含能材料,2004,12(2):38]7Pang,J.;Wang,J.N.;Zhang,R.E.;Xie,B.Chinese J.Explo.Prop.,2005,28(1):19[庞军,王江宁,张蕊娥,谢波.火炸药学报,2005,28(1):19]8Langlet,A.Guanylurea dinitramide,an 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