一种含腈基的硅烷偶联剂改性石英纤维/含硅芳炔复合材料
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摘要
设计并合成了一种含有二腈基的硅烷偶联剂DCA(Dicyanide-containing Silane Coupling Agent),采用FTIR、1 H-NMR、13 C-NMR表征了其化学结构。将DCA添加到石英纤维/含硅芳炔(QF/PSA)复合材料体系中,DCA含量为QF的2.0wt%时,常温条件下改性后的QF/PSA复合材料层间剪切强度(ILSS)和弯曲强度分别提升了63.3%和28.1%;250℃时ILSS和弯曲强度的保留率分别为83.0%和81.9%;500℃时ILSS和弯曲强度的保留率分别为54.7%和60.0%。偶联剂DCA固化后的热失重5%的温度(Td5)为357.8℃,900℃时残炭率为55.7%。XPS和DSC数据表明,偶联剂DCA在QF/PSA复合材料界面形成化学桥接,其中腈基在229℃固化,炔基在245℃参与PSA的固化,在PSA与QF间形成强界面层。SEM观察表明,经偶联剂DCA改性后QF/PSA复合材料的破坏属于韧性断裂。新型偶联剂DCA可显著改善QF/PSA复合材料界面,提高其高温力学性能。
A novel dicyanide-containing silane coupling agent(DCA)was synthesized and characterized with FTIR,1 H-NMR and 13 C-NMR.After modified by the coupling agent DCA(2.0 wt%),the interlaminar shear strength(ILSS)and flexural strength of the quartz fiber/poly(silicon-containing arylacetylene)(QF/PSA)composites increase by 63.3% and 28.1%at room temperature respectively.The retention of ILSS and flexural strength of QF/PSA are83.0% and 81.9%respectively at 250℃,the retention of ILSS and flexural strength are 54.7%and 60.0%respectively at 500℃.The decomposition temperature of 5%loss(Td5)of the cured DCA is 357.8℃,and its residue rate is up to 55.7% at 900℃.According to DSC analysis,the dicyanide groups cure at about 229℃,and the alkenyl groups copolymerized with PSA at 245℃.The strong interfacial layer form between QF and PSA.XPS analysis shows that DCA could form chemical bonds as the bridges between the matrix and fibers.Confirmed by SEM,the rupture mode of QF/PSA composites modified by DCA on the interface is obviously ductile fracture.DCA can apparently modify the interface of QF/PSA composites and improve its mechanical properties.
A novel dicyanide-containing silane coupling agent(DCA)was synthesized and characterized with FTIR,1 H-NMR and 13 C-NMR.After modified by the coupling agent DCA(2.0 wt%),the interlaminar shear strength(ILSS)and flexural strength of the quartz fiber/poly(silicon-containing arylacetylene)(QF/PSA)composites increase by 63.3% and 28.1%at room temperature respectively.The retention of ILSS and flexural strength of QF/PSA are83.0% and 81.9%respectively at 250℃,the retention of ILSS and flexural strength are 54.7%and 60.0%respectively at 500℃.The decomposition temperature of 5%loss(Td5)of the cured DCA is 357.8℃,and its residue rate is up to 55.7% at 900℃.According to DSC analysis,the dicyanide groups cure at about 229℃,and the alkenyl groups copolymerized with PSA at 245℃.The strong interfacial layer form between QF and PSA.XPS analysis shows that DCA could form chemical bonds as the bridges between the matrix and fibers.Confirmed by SEM,the rupture mode of QF/PSA composites modified by DCA on the interface is obviously ductile fracture.DCA can apparently modify the interface of QF/PSA composites and improve its mechanical properties.
引文
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[25]张芳芳,扈艳红,杜磊,等.含噁嗪环硅烷偶联剂对石英纤维/含硅芳炔复合材料性能的影响[J].功能高分子学报,2017,30(3):347-353.ZHANF F F,HU Y H,DU L,et al.Effects of benzoxazinecontaining silane coupling agent on properties of QF/PSAcomposites[J].Materials Review,2017,30(3):347-353(in Chinese).
[26]李正,张宗波,林先凯,等.邻苯二甲腈的固化机理与改性研究进展[J].材料导报,2013,27(8):82-87.LI Z,ZHANG Z B,LIN X K,et al.Progress on curing mechanism and modification of phthalonitrile resin[J].Materials Review,2013,27(8):82-87(in Chinese).
[27]周恒,刘锋,李小丽,等.邻间对位自催化氰基树脂的制备及相关性能对比研究[C]//第十六届全国复合材料学术年会,2010.ZHOU H,LIU F,LI X L,et al.Preparation and property of ortho,meta and para self-catalyzed resin with cyano group[C]//16th National Annual Conference on Composite Materials,2010(in Chinese).
[28]李智鹏,扈艳红,杜磊,等.国产芳纶上浆剂对聚三唑复合材料力学性能的影响[J].表面技术,2014,43(4):17-23.LI Z P,HU Y H,DU L,et al.Effect of domestic aramid fiber iii sizing agents on mechanical properties of polytriazole composites[J].Surface Technology,2014,43(4):17-23(in Chinese).
[29]杜峰可,袁荞龙,黄发荣.含硅芳炔/苯并噁嗪/氰酸酯三元聚合体系研究[J].高分子学报,2018(3):410-417.DU F K,YUAN Q L,HUANG F R.Studies on the terpolymer of poly(silyleneace-tylene aryleneacetylene)/benzoxazine/cyanate ester[J].Acta Polymerica Sinica,2018(3):410-417(in Chinese).
[30]ZHAO F,HUANG Y D.Improved interfacial properties of carbon fiber/epoxy composites through grafting polyhedral oligomeric silsesquioxane on carbon fiber surface[J].Material Letters,2010,64(24):2742-274.
[2]ITOH M,INOUE K,HIRAYAMA N,et al.Fiber reinforced plastics using a new heat-resistant silicon based polymer[J].Journal of Material Science,2002,37(17):3795-3801.
[3]王沪东,郭康康,周晖,等.聚硼硅氮烷杂化芳炔基树脂制备及抗热氧化性能[J].复合材料学报,2016,33(5):962-969.WANG H D,GUO K K,ZHOU H,et al.Preparation and thermal-oxidation resistance of polyborosilazane hybrid polyarylacetylene resin[J].Acta Materiae Compositae Sinica,2016,33(5):962-969(in Chinese).
[4]高金淼,齐会民,张健,等.新型含硅芳炔树脂及其复合材料性能[J].化工新型材料,2008,36(12):45-47.GAO J M,QI H M,ZHANG J,et al.Properties of new silicon-containing arylacetylene resin and its composite materials[J].New Chemical Materials,2008,36(12):45-47(in Chinese).
[5]徐彬,周权,倪礼忠,等.硅炔杂化树脂及其复合材料的性能[J].功能高分子学报,2012,25(2):148-151XU B,ZHOU Q,NI L Z,et al.Properties of silicone resin modified with silicone-acetylene resin and its composites[J].Journal of Functional Polymers,2012,25(2):148-151(in Chinese).
[6]PIGGOT M,ANDISON D.The carbon fibre-epoxy interface[J].Journal of Reinforced Plastics and Composites,1987,6(3):290-302.
[7]LI J,MA H,HUANG Y.A method for characterizes the interface between carbon fiber and epoxy resin:Three-parameters exponential pattern[J].Material Chemistry and Physics,2005,89(2-3):367-372.
[8]PICKERING K,ABDALLA L.The effect of silane coupling agents on radiata pine fibre for use in thermoplastic matrix composites[J].Composites Part A:Applied Science and Manufacturing,2003,34(10):9115-926.
[9]DWIGHT W,HUFF N.Effects of silane coupling agents on the interphase and performance of glass-fiber reinforced polymer composites[J].Composites Science and Technology,1997(57):975-983.
[10]BUREAU M,DENAUL J.Fatigue resistance of continuous glass fiber/polypropylene composites consolidation dependence[J].Composites Science and Technology,2004,64(12):1785-1794.
[11]WANG L,SHI Y,SA R,et al.Surface modification of aramid fibers by catechol/polyamine codeposition followed by silane grafting for enhanced interfacial adhesion to rubber matrix[J].Industrial&Engineering Chemistry Research,2016,55(49):12547-12556.
[12]CUI H Y,KESSLER M R.Glass fiber reinforced ROMP-based bio-renewable polymers:Enhancement of the interface with silane coupling agents[J].Composites Science and Technology,2012,72(11):1264-1272.
[13]梁秀华,扈艳红,杜磊,等.异氰酸酯基硅烷偶联剂改性石英纤维/含硅芳炔复合材料表面[J].玻璃钢/复合材料,2013(8):44-50.LIANG X H,HU Y H,DU L,et al.Interfacial modification of quartz fiber reinforced silicon-arylacetylene resin composite by coupling agent[J].Fiber Reinforced Plastics/Composites,2013(8):44-50(in Chinese).
[14]王林靖,扈艳红,杜磊,等.乙炔基芳酰胺酸硅烷改进石英纤维/含硅芳炔复合材料高温界面性能[J].复合材料学报,2016,33(2):287-296.WANG L J,HU Y H,DU L,et al.High-temperature interfacial property of quartz fiber/silicon-containing arylacetylene composites with aromatic amic acid-containing alkyne-terminated silane[J].Acta Materiae Compositae Sinica,2016,33(2):287-296(in Chinese).
[15]曾科,杨刚.聚邻苯二甲腈树脂研究进展[J].热固性树脂,2012,27(1):58-63.ZENG K,YANG G.Research progress in phthalonitrile resins[J].Thermosetting Resin,2012,27(1):58-63(in Chinese).
[16]曾科,杨刚.聚邻苯二甲腈树脂研究进展(续)[J].热固性树脂,2012,27(2):60-62.ZENG K,YANG G.Research progress in phthalonitrile resins[J].Thermosetting Resin,2012,27(2):60-62(in Chinese).
[17]曾科,杨刚.聚邻苯二甲腈树脂研究进展(续完)[J].热固性树脂,2012,27(3):58-61.ZENG K,YANG G.Research progress in phthalonitrile resins[J].Thermosetting Resin,2012,27(3):58-61(in Chinese).
[18]KELLER T M.Fluorinated high temperature phthalonitrile[J].Polymer Communications,1987,28(12):337-339.
[19]SASTRI S B,KELLWR T M.Phthalonitrile cure reaction with aromatic diamines[J].Journal of Polymer Science Part A,1998,36(11):1885-1890.
[20]SASRTI S B,ARMISTEAD J P,KELLER T M,Phthalonitrile-carbon fiber composites[J].Polymer Composites,1996,17(6):816-822.
[21]周恒,刘峰,赵彤,等.新型自催化氰基树脂的制备及其初步热性能[J].宇航材料工艺,2010(2):45-48.ZHOU H,LIU F,ZHAO T,et al.Preparation and thermal properties of novel self-catalyst resin with cyano group[J].Aerospace Materials and Technology,2010(2):45-48(in Chinese).
[22]CHENG B,HU Y H,DENG S F.Synthesis and application of a novel dicyanide-containing silane coupling agent[C]//6th Annual International Conference on Material Science and Engineering.Suzhou:IOP Publishing,2018.
[23]中华人民共和国工业和信息化部.纤维增强塑料短梁法测定层间剪切强度:JC/T 773-2010[S].北京:中国标准出版社,2011.Ministry of Industry and Information Technology of the People’s Republic of China.Fiber-reinforced plastics composites:Determination of apparent interlaminar shear strength by short-beam method:JC/T 773-2010[S].Beijing:China Standards Press,2011(in Chinese).
[24]中国国家标准化管理委员会.纤维增强塑料弯曲性能试验方法:GB/T 1449-2005[S].北京:中国标准出版社,2005.Standardization Administration of the People’s Republic of China.Fibre-reinforced plastic composites:Determination of flexural properties:GB/T 1449-2005[S].Beijing:China Standards Press,2005(in Chinese).
[25]张芳芳,扈艳红,杜磊,等.含噁嗪环硅烷偶联剂对石英纤维/含硅芳炔复合材料性能的影响[J].功能高分子学报,2017,30(3):347-353.ZHANF F F,HU Y H,DU L,et al.Effects of benzoxazinecontaining silane coupling agent on properties of QF/PSAcomposites[J].Materials Review,2017,30(3):347-353(in Chinese).
[26]李正,张宗波,林先凯,等.邻苯二甲腈的固化机理与改性研究进展[J].材料导报,2013,27(8):82-87.LI Z,ZHANG Z B,LIN X K,et al.Progress on curing mechanism and modification of phthalonitrile resin[J].Materials Review,2013,27(8):82-87(in Chinese).
[27]周恒,刘锋,李小丽,等.邻间对位自催化氰基树脂的制备及相关性能对比研究[C]//第十六届全国复合材料学术年会,2010.ZHOU H,LIU F,LI X L,et al.Preparation and property of ortho,meta and para self-catalyzed resin with cyano group[C]//16th National Annual Conference on Composite Materials,2010(in Chinese).
[28]李智鹏,扈艳红,杜磊,等.国产芳纶上浆剂对聚三唑复合材料力学性能的影响[J].表面技术,2014,43(4):17-23.LI Z P,HU Y H,DU L,et al.Effect of domestic aramid fiber iii sizing agents on mechanical properties of polytriazole composites[J].Surface Technology,2014,43(4):17-23(in Chinese).
[29]杜峰可,袁荞龙,黄发荣.含硅芳炔/苯并噁嗪/氰酸酯三元聚合体系研究[J].高分子学报,2018(3):410-417.DU F K,YUAN Q L,HUANG F R.Studies on the terpolymer of poly(silyleneace-tylene aryleneacetylene)/benzoxazine/cyanate ester[J].Acta Polymerica Sinica,2018(3):410-417(in Chinese).
[30]ZHAO F,HUANG Y D.Improved interfacial properties of carbon fiber/epoxy composites through grafting polyhedral oligomeric silsesquioxane on carbon fiber surface[J].Material Letters,2010,64(24):2742-274.
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