Ab initio neural network MD simulation of thermal decomposition of a high energy material CL-20／TNT.docx

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1、PCCPROYA1SOCIETY.OFCHEMISTRYpwoq9gzMoZ滴I/=UOA11SXHINNoNVHSAqPoPP0cM0ZZorrdv81 Uopoqs=qndPAPERViewArtic1eOn1inViewJourndViewIssueRCheckforupdatesCitethis:Phys.Chem.Chem.Phys.,2023,24,11801Abinitioneura1networkMDsimu1ationoftherma1decompositionofahighenergymateria1C1-20TNTfIntroduction1iqunCao,aJinzhe

2、Zeng,JbBoWang,aTongZhu*acandJohn1.H.Zhang*acdefReceived12thFebruary2023,Accepted15thApri12023DOI:10.1039d2cp00710jC1-20(274,6,871012-hexanitro-2,4,6,871012-hexaazaisowurtzitane,a1soknownasHNIW)isoneofthemostpowerfu1energeticmateria1s.However;itshighsensitivitytoenvironmenta1stimu1igreat1yreducesitss

3、afetyandsevere1y1imitsitsapp1ication.Inthiswork,abinitiobasedneura1networkpotentia1(NNP)energysurfacesforbothb-C1-20andC1-20/TNTco-crysta1swereconstructed.Toaccurate1ysimu1atethetherma1decompositionprocessesofthesetwocrysta1systems,reactivemo1ecu1ardynamicssimu1ationsbasedontheNNPswereperformed.Many

4、importantintermediatespeciesandtheirassociatedreactionpathsduringthedecompositionhadbeenidentifiedinthesimu1ationsandthedirectresu1tsondetonationtemperaturesofbothsystemswereprovided.Thesimu1ationsa1soshowedc1ear1ythat2,4,6-trinitroto1uene(TNT)mo1ecu1esintheco-crysta1actasabuffertos1owdownthechainre

5、actionstriggeredbynitrogendioxideandthiseffectismoresignificantat1owertemperatures.Specifica11y,theadditionofTNTmo1ecu1esintheC1-20TNTco-crysta1introducesintermo1ecu1arhydrogenbondsbetweenC1-20andTNTmo1ecu1esinthesystem,therebyincreasingthetherma1stabi1ityoftheco-crysta1.Thecurrentreactivemo1ecu1ard

6、ynamicssimu1ationisperformedbasedontheNNPwhichhe1psinacce1eratingthespeedofabinitiomo1ecu1ardynamics(AIMD)simu1ationbymorethan3ordersofmagnitudewhi1epreservingtheaccuracyofdensityfunctiona1theory(DFT)ca1cu1ations.Thisenab1edustoperform1onger-timesimu1ationsatmorerea1istictemperaturesthattraditiona1A

7、IMDmethodscannotachieve.WiththeadvantageoftheNNPinitspowerfu1fittingabi1ityandtransferabi1ity,theNNP-basedMDsimu1ationcanbewide1yapp1iedtoenergeticmateria1systems.rsc.1i/pccphavesimp1ecompositionsandstructures,andmostofthemcontainamine,nitro,orazidegroups.Current1y,compoundEnergeticmateria1shavebeen

8、wide1yusedinmi1itary,aerospace,andcivi1ianapp1icationsasmi1itaryexp1osives,rocketprope11ants,andfireworks.Theear1ydeve1opedenergeticmateria1spwoq9gzMoZ滴I/=UOA1ISXHINNoNVHSAqPoPP0cM0ZZorrdv81Uopoqs=qndPaperShanghaiEngineeringResearchCenterofMo1ecu1arTherapeutics&NewDrugDeve1opment,Schoo1ofChemistryan

9、dMo1ecu1arEngineering,EastChinaNorma1University,Shanghai,200062,China.E-mai1:tzhu,john.zhangnyu.edubDepartmentofChemistryandChemica1Bio1ogy,InstituteforQuantitativeBiomedicine,Rutgers,theStateUniversityofNewJersey,Piscataway08854-8076,NJ,USACNYU-ECNUCenterforComputationa1ChemistryatNYUShanghai,Shang

10、hai,200062,ChinaaDepartmentofChemistry,NewYorkUniversity,NewYork10003,USAeShenzhenInstituteofSyntheticBio1ogy,ShenzhenInstitutesofAdvancedTechno1ogy,ChineseAcademyofSciences,Shenzhen,Guangdong,Chinaf-Co11aborativeInnovationCenterofExtremeOptics,ShanxiUniversity,Taiyuan,Shanxi,030006,ChinaE1ectronics

11、upp1ementaryinformation(ESI)avai1ab1e.SeeDOI:https:/doi.org/10.1039d2cp00710j2,4,5,8,10,12-hexanitro-2,4,6,8,10,12-hexaazaisowurtzitane(C1-20)1isknownasoneofthemostpowerfu1exp1osives.Ithasbetterperformancethanotherenergeticmateria1sinoxygenba1ance,detonationve1ocity,detonationpressure,andpackingdens

12、ity.However,thehighsensitivitytomechanica1stimu1i1imitstheapp1icationofpureC1-20.Infact,mostoftheenergeticmateria1shavecontradictionsinsensitivityandenergydensity,2andseekingthebestba1ancebetweenthehighenergyoutputandhighsafetyhas1ongbeenanimportantdirectioninthedesignofnove1energeticmateria1s.Recen

13、t1y,co-crysta11izationhasbecomeawide1yusedstrategytoaccessabetterba1ancebetweenthesensitivityandenergyoutputofenergeticmateria1s.3Co-crysta11izationcombinestwoormoretypesofmo1ecu1esinonecrysta11atticethroughnon-cova1entinteractions(hydrogenbonds,ionicbonds,vanderWaa1sinteractions,andp-pstackinginter

14、actions)toimprovethestabi1ityofenergeticmateria1s.Recentexperimenta1studieshaveshownthattheco-crysta11izationofC1-20withotherenergeticmateria1scanimproveeitherimpactstabi1ityortherma1stabi1ity.4-9However,a1thougha1argenumberofC1-20co-crysta1shavebeenproposed,thedetai1edmo1ecu1armechanismsbehinditsbe

15、tterperformanceinstabi1ityoverpureC1-20aresti11unc1ear.Duetotheextremeconditionsandcomp1exreactionsinvo1vedinthetherma1decompositionofenergeticmateria1s,capturingchemica1detai1sattheatomic1eve1inexperimentsisnear1yimpossib1e.Incontrast,computersimu1ationsmakeiteasiertoachievehightempora1andspatia1re

16、so1utions,aswe11asthecontro1ofreactionconditions.Therefore,theoretica1methodssuchasquantumchemistry(QC)ca1cu1ationandmo1ecu1ardynamics(MD)simu1ationhavebecomethemainmethodsinthestudyofenergeticmateria1s.QCca1cu1ation,especia11yabinitioMD(AIMD)simu1ationmethods,isundoubted1ythemostaccurateapproachtostudythebreakingandformationofchemica1bonds.Isayevandcoworkershaveperformedas