

FOLLOWUS
a.Key Laboratory of Science and Technology on High-tech Polymer Materials, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China
b.School of Chemical Sciences, University of Chinese Academy of Sciences, Beijing 100049, China
zhailei@iccas.ac.cn (L.Z.)
fanlin@iccas.ac.cn (L.F.)
Received:01 March 2023,
Revised:2023-3-22,
Accepted:03 April 2023,
Online First:18 May 2023,
Published:01 December 2023
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Gao, M. Y.; Zhai, L.; Mo, S.; Jia, Y.; Liu, Y.; He, M. H.; Fan, L. Thermally conductive polyimide/boron nitride composite films with improved interfacial compatibility based on modified fillers by polyimide brushes. Chinese J. Polym. Sci. 2023, 41, 1921–1936
Meng-Yan Gao, Lei Zhai, Song Mo, et al. Thermally Conductive Polyimide/Boron Nitride Composite Films with Improved Interfacial Compatibility Based on Modified Fillers by Polyimide Brushes[J]. Chinese Journal of Polymer Science, 2023, 41(12): 1921-1936.
Gao, M. Y.; Zhai, L.; Mo, S.; Jia, Y.; Liu, Y.; He, M. H.; Fan, L. Thermally conductive polyimide/boron nitride composite films with improved interfacial compatibility based on modified fillers by polyimide brushes. Chinese J. Polym. Sci. 2023, 41, 1921–1936 DOI: 10.1007/s10118-023-2985-4.
Meng-Yan Gao, Lei Zhai, Song Mo, et al. Thermally Conductive Polyimide/Boron Nitride Composite Films with Improved Interfacial Compatibility Based on Modified Fillers by Polyimide Brushes[J]. Chinese Journal of Polymer Science, 2023, 41(12): 1921-1936. DOI: 10.1007/s10118-023-2985-4.
Boron nitride is chemically modified by polyimide brushes that are grafted on the filler surface. Interfacial compatibility between filler and matrix is greatly improved. Tensile strength of polyimide/boron nitride composite film is up to 80 MPa even at 50 wt% filler content. Both out-of-plane and in-plane thermal conductivity are over 0.8 W/(m·K).
Polyimide-based composite films with high thermal conductivity
good mechanical property and electrical insulating performance are urgently needed in the electronics and microelectronics fields. As one of the key technical challenges to be solved
interfacial compatibility between filler and matrix plays an important role for composite film. Herein
boron nitride was modified by grafting polyimide brushes
via
a two-step method
and a series of thermally conductive polyimide/ boron nitride composite films were prepared. Both characterization and performance results proved that the interfacial interaction and compatibility was greatly enhanced
resulting in a significant reduction in defects and interfacial thermal resistance. The interphase width of transition zone between two phases was also efficiently enlarged due to polyimide brushes grafted on filler surface. As a result
composite films based on polyimide-grafted boron nitride exhibited significantly improved properties compared with those based on pristine filler. Tensile strength can reach up to 80 MPa even if the filler content is as high as 50 wt%. The out-of-plane and in-plane thermal conductivity of composite film increased to 0.841 and 0.850 W·m
−1
·K
−1
respectively. In addition
thermal and dielectric properties of composite films were also enhanced to some extent. The above results indicate that surface modification by chemically grafting polymer brushes is an effective method to improve two-phase interfacial compatibility so as to prepare composite film with enhanced properties.
Bai,L.;Zhai,L.;He,M.H.;Wang,C.O.;Mo,S.;Fan,L.Thermalexpansionbehaviorofpoly(amide-imide)filmswithultrahightensilestrengthandultralowCTE. Chinese J. Polym. Sci. 2020 , 38 ,748−758..
Dong,X.D.;Wan,B.Q.;Qiu,L.;Zheng,M.S.;Gao,J.F.;Zha,J.W.Rigid/flexiblemolecularstructure-inducedpolyimideaerogelswithultralowpermittivityandthermalinsulationproperties. IET Nanodielectr. 2022 ,10.1049/nde2.12041..
Ahn,C.;Kim,T.Y.;Hong,P.H.;Choi,S.;Lee,Y.J.;Kwon,H.;Jeon,H.;Ko,D.W.;Park,I.;Han,H.;Hong,S.W.Highlytransparent,colorlessopticalfilmwithoutstandingmechanicalstrengthandfoldingreliabilityusingmismatchedcharge-transfercomplexintensification. Adv. Funct. Mater. 2022 , 32 ,2111040..
Liu,Y.W.;Tang,L.S.;Qu,L.J.;Liu,S.W.;Chi,Z.G.;Zhang,Y.;Xu,J.R.Synthesisandpropertiesofhighperformancefunctionalpolyimidescontainingrigidnonplanarconjugatedfluorenemoieties. Chinese J. Polym. Sci. 2019 , 37 ,416−427..
Zhuang,Y.B.;Seong,J.G.;Lee,Y.M.Polyimidescontainingaliphatic/alicyclicsegmentsinthemainchains. Prog. Polym. Sci. 2019 , 92 ,35−88..
Zhang,Y.L.;Ruan,K.P.;Zhou,K.;Gu,J.W.ControlleddistributedTi 3 C 2 T x hollowmicrospheresonthermallyconductivepolyimidecompositefilmsforexcellentelectromagneticinterferenceshielding. Adv. Mater. 2023 , 35 ,2211642..
Yu,S.Q.;Huang,M.M.;Hao,R.;He,S.Q.;Liu,H.;Liu,W.T.;Zhu,C.S.Recentadvancesinthermallyconductivepolymercomposites. High Perform. Polym. 2022, 1-21..
Mokoena,T.E.;Magagula,S.I.;Mochane,M.J.;Mokhena,T.C.Mechanicalproperties,thermalconductivity,andmodelingofboronnitride-basedpolymercomposites:areview. Express Polym. Lett. 2021 , 15 ,1148−1173..
Ding,D.L.;Zou,M.H.;Wang,X.;Qin,G.Z.;Zhang,S.Y.;Chan,S.Y.;Meng,Q.Y.;Liu,Z.G.;Zhang,Q.Y.;Chen,Y.H.ThermalconductivityofpolydispersehexagonalBN/polyimidecomposites:IterativeEMTmodelandmachinelearningbasedonfirstprinciplesinvestigation. Chem. Eng. J. 2022 , 437 ,135438..
Gao,M.Y.;Wang,C.O.;Jia,Y.;Zhai,L.;Mo,S.;He,M.H.;Fan,L.Researchprogressinanisotropicthermalconductionbehaviorofpolyimidefilms. Acta Polymerica Sinica (inChinese) 2021 , 52 ,1283−1297..
Haruki,M.Thermalconductivityforpolymercompositematerials:recentadvancesinpolyimidematerials. J. Chem. Eng. Jpn. 2021 , 54 ,186−194..
Shoji,Y.;Ishige,R.;Higashihara,T.;Morikawa,J.;Hashimoto,T.;Takahara,A.;Watanabe,J.;Ueda,M.Cross-linkedliquidcrystallinepolyimideswithsiloxaneunits:theirmorphologyandthermaldiffusivity. Macromolecules 2013 , 46 ,747−755..
Ruan,K.P.;Guo,Y.Q.;Gu,J.W.Liquidcrystallinepolyimidefilmswithhighintrinsicthermalconductivitiesandrobusttoughness. Macromolecules 2021 , 54 ,4934−4944..
Ruan,K.P.;Gu,J.W.Orderedalignmentofliquidcrystallinegraphenefluorideforsignificantlyenhancingthermalconductivitiesofliquidcrystallinepolyimidecompositefilms. Macromolecules 2022 , 55 ,4134−4145..
Chung,S.;Kim,J.T.;Kim,H.;Kim,D.H.;Jeong,S.W.Magneticalignmentofgraphiteplateletsinpolyimidematrixtowardaflexibleelectronicsubstratewithenhancedthermalconductivity. Mater. Today Commun. 2022 , 30 ,103026..
Ruan,K.P.;Guo,Y.Q.;Lu,C.Y.;Shi,X.T.;Ma,T.B.;Zhang,Y.L.;Kong,J.;Gu,J.W.Significantreductionofinterfacialthermalresistanceandphononscatteringingraphene/polyimidethermallyconductivecompositefilmsforthermalmanagement. Research 2021 , 2021 ,8438614..
Haruki,M.;Tada,J.;Funaki,R.;Onishi,H.;Tada,Y.Enhancingthermalconductivitiesofhexagonalboronnitride/fluorinatedpolyimidecompositematerialsusingdirectcurrentelectricalfields. Thermochim. Acta 2020 , 684 ,178491..
Wei,S.Y.;Zheng,Z.B.;Yu,Q.X.;Fan,Z.G.;Liu,S.W.;Chi,Z.G.;Zhang,Y.;Xu,J.R.EnhancedthermalconductivityofPIfilmsbystrengtheningthree-dimensionalrGonetworktemplate. Acta Polymerica Sinica (inChinese) 2019 , 50 ,402−409..
Song,H.;Kim,B.G.;Kim,Y.S.;Bae,Y.S.;Kim,J.;Yoo,Y.Synergisticeffectsofvariousceramicfillersonthermallyconductivepolyimidecompositefilmsandtheirmodelpredictions. Polymers 2019 , 11 ,484..
Han,Y.X.;Ruan,K.P.;Gu,J.W.Multifunctionalthermallyconductivecompositefilmsbasedonfungaltree-likeheterostructuredsilvernanowires@boronnitridenanosheetsandaramidnanofibers. Angew. Chem. Int. Ed. 2023 , 62 ,e202216093..
Han,Y.X.;Ruan,K.P.;Gu,J.W.Janus(BNNS/ANF)-(AgNWs/ANF)thermalconductivitycompositefilmswithsuperiorelectromagneticinterferenceshieldingandjouleheatingperformances. Nano Res. 2022 , 15 ,4747−4755..
Hwang,G.H.;Kwon,Y.S.;Lee,J.S.;Jeong,Y.G.Enhancedmechanicalandanisotropicthermalconductivepropertiesofpolyimidenanocompositefilmsreinforcedwithhexagonalboronnitridenanosheets. J. Appl. Polym. Sci. 2020 , 138 ,50324..
Chen,H.Y.;Ginzburg,V.V.;Yang,J.;Yang,Y.F.;Liu,W.;Huang,Y.;Du,L.B.;Chen,B.Thermalconductivityofpolymer-basedcomposites:fundamentalsandapplications. Prog. Polym. Sci. 2016 , 59 ,41−85..
Ding,D.L.;Wang,H.T.;Wu,Z.Q.;Chen,Y.H.;Zhang,Q.Y.Highlythermallyconductivepolyimidecomposites via constructing3Dnetworks. Macromol. Rapid Commun. 2019, 1800805..
Wu,Y.M.;Ye,K.;Liu,Z.D.;Wang,M.J.;Chee,K.W.A.;Lin,C.;Jiang,N.;Yu,J.H.Effectivethermaltransporthighwayconstructionwithindielectricpolymercomposites via avacuum-assistedinfiltrationmethod. J. Mater. Chem. C 2018 , 6 ,6494−6501..
Zhang,G.D.;Fan,L.;Bai,L.;He,M.H.;Zhai,L.;Mo,S.Mesoscopicsimulationassistantdesignofimmisciblepolyimide/BNblendfilmswithenhancedthermalconductivity. Chinese J. Polym. Sci. 2018 , 36 ,1394−1402..
Lau,K.Y.;Piah,M.A.M.Polymernanocompositesinhighvoltageelectricalinsulationperspective:areview. Malaysian Polym. J. 2011 , 6 ,58−69..
Tanimoto,M.;Ando,S.Preventionofvoidformationinparticulate-filledpolymercomposites:Effectsofthermoplasticmatricesandresidualsolvent. Compos. Sci. Technol. 2016 , 123 ,268−275..
Ma,X.Y.;Liu,L.Z.;Zhang,X.R.;Lv,T.ThermalconductivityenhancementofpolyimidefilmsfilledwithBNandAlNfillers. High Perform. Polym. 2019 , 31 ,959−968..
Zha,J.W.;Yao,S.C.;Qiu,Y.;Zheng,M.S.;Dang,Z.M.Enhanceddielectricpropertiesandenergystorageofthesandwich-structuredpoly(vinylidenefluoride- co -hexafluoro-propylene)compositefilmswithfunctionalBaTiO 3 @Al 2 O 3 nanofibres. IET Nanodielectr. 2019 , 2 ,103−108..
Ding,D.L.;Shang,Z.H.;Zhang,X.;Lei,X.F.;Liu,Z.G.;Zhang,Q.Y.;Chen,Y.H.Greatlyenhancedthermalconductivityofpolyimidecompositesbypolydopaminemodificationandthe2D-alignedstructure. Ceram. Int. 2020 , 46 ,28363−28372..
Duan,G.Y.;Cao,Y.T.;Quan,J.Y.;Hu,Z.M.;Wang,Y.;Yu,J.R.;Zhu,J.BioinspiredconstructionofBN@polydopamine@Al 2 O 3 fillersforpreparationofapolyimidedielectriccompositewithenhancedthermalconductivityandbreakdownstrength. J. Mater. Sci. 2020 , 55 ,8170−8184..
Ou,X.H.;Lu,X.M.;Chen,S.S.;Lu,Q.H.Thermalconductivehybridpolyimidewithultrahighheatresistance,excellentmechanicalpropertiesandlowcoefficientofthermalexpansion. Eur. Polym. J. 2020 , 122 ,109368..
Ma,L.L.;Ma,T.;Wang,B.X.;Fei,X.;Han,R.Y.;Lv,P.;Hao,C.C.;Lei,Q.Q.Effectsofcouplingagentsonpropertiesofpolyimide/h-BNcompositefilms. Insul. Mater. (inChinese) 2017 , 50 ,15−20..
Kizilkaya,C.;Mülazim,Y.;VezirKahraman,M.;KayamanApohan,N.;Güngör,A.Synthesisandcharacterizationofpolyimide/hexagonalboronnitridecomposite. J. Appl. Polym. Sci. 2012 , 124 ,706−712..
Zhang,S.H.;Li,X.Y.;Guan,X.X.;Shi,Y.C.;Wu,K.;Liang,L.Y.;Shi,J.;Lu,M.G.Synthesisofpyridine-containingdiamineandpropertiesofitspolyimidesandpolyimide/hexagonalboronnitridecompositefilms. Compos. Sci. Technol. 2017 , 152 ,165−172..
Yang,N.;Xu,C.;Hou,J.;Yao,Y.M.;Zhang,Q.X.;Grami,M.E.;He,L.Q.;Wang,N.Y.;Qu,X.W.Preparationandpropertiesofthermallyconductivepolyimide/boronnitridecomposites. RSC Adv. 2016 , 6 ,18279−18287..
Liu,L.Z.;Cao,C.H.;Ma,X.Y.;Zhang,X.R.;Lv,T.Thermalconductivityofpolyimide/AlNandpolyimide/(AlN + BN)compositefilmspreparedby in situ polymerization. J. Macromol. Sci. A 2020 , 57 ,398−407..
Guo,Y.Q.;Lyu,Z.Y.;Yang,X.T.;Lu,Y.J.;Ruan,K.P.;Wu,Y.L.;Kong,J.;Gu,J.W.Enhancedthermalconductivitiesanddecreasedthermalresistancesoffunctionalizedboronnitride/polyimidecomposites. Compos. Part B-Eng. 2019 , 164 ,732−739..
Zhang,Y.J.;Wang,J.;Chen,Y.J.Polyhedraloligosilsesquioxane-modifiedboronnitrideenhancesthemechanicalpropertiesofpolyimidenanocomposites. RSC Adv. 2022 , 12 ,7276−7283..
Yang,X.;Wang,C.Y.;Lu,R.;Shen,Y.N.;Zhao,H.B.;Li,J.;Li,R.Y.;Zhang,L.X.;Chen,H.S.;Zhang,T.;Zheng,X.H.Progressinmeasurementofthermoelectricpropertiesofmicro/nanothermoelectricmaterials:acriticalreview. Nano Energy 2022 , 101 ,107553..
Aiyiti,A.;Hu,S.Q.;Wang,C.R.;Xi,Q.;Cheng,Z.F.;Xia,M.G.;Ma,Y.L.;Wu,J.B.;Guo,J.;Wang,Q.L.;Zhou,J.;Chen,J.;Xu,X.F.;Li,B.W.Thermalconductivityofsuspendedfew-layerMoS 2 . Nanoscale 2018 , 10 ,2727−2734..
Wang,H.T.;Ding,D.L.;Liu,Q.;Chen,Y.H.;Zhang,Q.Y.Highlyanisotropicthermallyconductivepolyimidecomposites via thealignmentofboronnitrideplatelets. Compos. Part B-Eng. 2019 , 158 ,311−318..
Houssat,M.;Villeneuve-Faure,C.;LahoudDignat,N.;Locatelli,M.L.;Cambronne,J.P.TemperatureinfluenceonPI/Si 3 N 4 nanocompositedielectricproperties:amultiscaleapproach. Polymers 2021 , 13 ,1936..
Zhang,H.F.;Hao,Q.;Tian,H.C.;Yao,P.J.;Liu,X.Y.;Yu,B.;Ning,N.Y.;Tian,M.;Zhang,L.Q.Polyurethane-polysiloxanecopolymercompatibilizedSiR/TPUTPVwithcomfortablehumantouchtowardwearabledevices. Chinese J. Polym. Sci. 2023 , 41 ,258−266..
Bai,L.;Zhai,L.;He,M.H.;Wang,C.O.;Mo,S.;Fan,L.Preparationofheat-resistantpoly(amide-imide)filmswithultralowcoefficientsofthermalexpansionforoptoelectronicapplication. React. Funct. Polym. 2019 , 141 ,155−164..
Wang,C.O.;Zhai,L.;Mo,S.;Liu,Y.;Gao,M.Y.;Jia,Y.;He,M.H.;Fan,L.Effectofaggregationstructureonthermalexpansionbehaviorofpolyimidefilmswithdifferentthickness. Chinese J. Polym. Sci. 2022 , 40 ,1651−1661..
Bai,L.;Zhai,L.;Wang,C.O.;He,M.H.;Mo,S.;Fan,L.Thermalexpansionbehaviorofamide-containingpolyimidefilmswithultralowthermalexpansioncoefficient. Chem. J. Chinese Univ. (inChinese) 2020 , 41 ,795−802..
Bai,L.;Zhai,L.;He,M.H.;Wang,C.O.;Mo,S.;Fan,L.Effectofhightemperatureannealingonthermalexpansionbehaviorofpoly(amide-imide)filmswithultralowcoefficientofthermalexpansion. Acta Polymerica Sinica (inChinese) 2019 , 50 ,1305−1313..
Liu,L.;Shen,S.Y.;Wang,Y.Y.Enhancedthermalconductivityofflexibleh-BN/polyimidecompositesfilmswithethylcellulose. e-Polymers 2019 , 19 ,305−312..
Ou,X.H.;Chen,S.S.;Lu,X.M.;Lu,Q.H.Enhancementofthermalconductivityanddimensionalstabilityofpolyimide/boronnitridefilmsthroughmechanochemistry. Compos. Commun. 2021 , 23 ,100549..
Tan,W.Y.;Jian,L.F.;Chen,W.P.;Zhang,Y.W.;Lu,X.C.;Huang,W.J.;Zhang,J.S.;Wu,J.W.;Feng,J.L.;Liu,Y.D.;Cui,T.T.;Min,Y.G.Afacilestrategyforintrinsiclow- D k andlow- D f polyimidesenabledbyspirobifluorenegroups. Chinese J. Polym. Sci. 2023 , 41 ,288−296..
Liu,X.J.;Zheng,M.S.;Chen,G.;Dang,Z.M.;Zha,J.W.High-temperaturepolyimidedielectricmaterialsforenergystorage:Theory,design,preparationandproperties. Energ. Environ. Sci. 2022 , 15 ,56−81..
Fan,Z.G.;Liu,S.W.;Chi,Z.G.;Zhang,Y.;Xu,J.R.Constructionandstudyofquantitativestructure-propertyrelationshipmodelforintrinsicpolyimidedielectricconstant. Acta Polymerica Sinica (inChinese) 2021 , 52 ,750−761..
Nan,C.;Liu,G.;Lin,Y.H.;Li,M.Interfaceeffectonthermalconductivityofcarbonnanotubecomposites. Appl. Phys. Lett. 2004 , 85 ,3549−3551..
Ruan,K.P.;Shi,X.T.;Guo,Y.Q.;Gu,J.W.Interfacialthermalresistanceinthermallyconductivepolymercomposites:areview. Compos. Commun. 2020 , 22 ,100518..
Lin,Z.Y.;Liu,Y.;Raghavan,S.;Moon,K.S.;Sitaraman,S.K.;Wong,C.P.Magneticalignmentofhexagonalboronnitrideplateletsinpolymermatrix:towardhighperformanceanisotropicpolymercompositesforelectronicencapsulation. ACS Appl. Mater. Interfaces 2013 , 5 ,7633−7640..
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