|
- 2019
SiO2中空微球改性含硅芳炔树脂及其复合材料的结构与性能
|
Abstract:
采用SiO2中空微球对含硅芳炔树脂(PSAC)进行改性,制备了SiO2/PSAC复合材料,以改善PSAC固化后质脆的缺点,提高PSAC基复合材料的力学性能,拓展PSAC在航空航天领域的应用。对SiO2/PSAC复合材料和石英纤维布增强SiO2/PSAC(QF-SiO2/PSAC)复合材料的结构与性能进行了研究,采用SEM分析SiO2/PSAC树脂浇铸体和QF-SiO2/PSAC复合材料断面微观结构,并分析SiO2的增韧机制。采用DMA和TGA分析了SiO2/PSAC复合材料耐热性能和热稳定性,虽然SiO2会导致树脂耐热性能略有下降,但其中空结构使树脂具有优异介电性能。当SiO2的添加量达2wt%时,SiO2/PSAC树脂浇铸体弯曲强度达22.3 MPa,失重5%温度为551℃,1 000℃残留率为86.5%;QF-2SiO2/PSAC复合材料的弯曲强度为298.3 MPa,弯曲模量达31.0 GPa,分别提高了27.5%、59.0%;当SiO2添加量为5wt%时,QF-5SiO2/PSAC复合材料的剪切强度提高了16.0%。 SiO2 hollow microspheres modified Si-containing arylacetylene resin (SiO2/PSAC) casting was prepared to ameliorate the brittleness of cured Si-containing arylacetylene resin and to improve the mechanical properties of the SiO2/PSAC resin casting and to meet the need of the application in the field of aeronautics and astronautics. The structure and properties of the SiO2/PSAC resin casting and quartz fiber reinforced SiO2/PSAC (QF-SiO2/PSAC) composites were investigated. The microstructure of SiO2/PSAC resin castings and QF-SiO2/PSAC composites were observed by SEM, and the toughening mechanism of SiO2 was analyzed. The heat resistance and thermal stability of SiO2/PSAC composites were studied by DMA and TGA. The heat resistance of the resin decreased slightly, but the porous structure made the resin excellent in dielectric properties. Meanwhile, when the content of SiO2 is added to 2wt%, the flexural strength of SiO2/PSAC resin casting is 22.3 MPa. The temperature of decomposition (Td5) is 551℃ and the char yield at 1 000℃ is 86.5%; the flexural strength of QF-2SiO2/PSAC composite is 298.3 MPa, and the modulus reaches 31.0 GPa, which increases by 27.5% and 59.0%, respectively; When the content of SiO2 is 5wt%, the shear strength of QF-5SiO2/PSAC composite increases by 16.0%. 国家自然科学基金(90816021
[1] | BOURY B, CORRIU R J P, MURAMATSU H. Organisation and reactivity of silicon-based hybrid materials with various cross-linking levels[J]. New Journal of Chemistry, 2002, 26(8): 981-988. |
[2] | WANG F, ZHANG J, HUANG J, et al. Synthesis and characterization of poly(dimethylsilyleneet-hynylenephenyleneethynylene) terminated with phenylacetylene[J]. Polymer Bulletin, 2006, 56(1): 19-26. |
[3] | 张玲玲, 高飞, 周围, 等. 含硅氢基团甲基芳炔树脂的合成及表征[J]. 过程工程学报, 2009, 9(3): 574-579.ZHANG L L, GAO F, ZHOU W, et al. Synthesis and characterization of poly(arylacetylene) resins containing methylsilylene groups[J]. The Chinese Journal of Process Engineer 2009, 9(3): 574-579(in Chinese). |
[4] | YIN G, ZHANG J, WANG C, et al. Synthesis and characterization of new disilane-containing arylacetylene resin[J]. Polymers, 2008, 8(1): 771-777. |
[5] | LEVASSORT C, JOUSSE F, DELNAUD L, et al. Poly(ethynylene phenylene ethynylene polysiloxene(silylene)) and methods for preparing same: United States, 6872795[P]. 2005-3-29. |
[6] | 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). |
[7] | 齐会民, 王光后, 张健, 等. 含硅芳炔树脂的改性及其性能研究[C]//第十五届全国复合材料学术会议论文集. 哈尔滨: 中国力学学会, 2009: 335-339.QI H M, WANG G H, ZHANG J, et al. The performance of modified silicon-containing acetylene resin[C]//15th National Conference on Composite Materials. Harbin: Chinese Society of Theoretical and Applied Mechanics, 2008: 335-339(in Chinese). |
[8] | 李晓燕, 任圆, 甘文君. 热固性树脂的增韧进展[J]. 热固性树脂, 2010, 25(5): 41-46.LI X Y, REN Y, GAN W J. Progress in toughening thermosetting resins[J]. Thermosetting Resin, 2010, 25(5): 41-46(in Chinese). |
[9] | 高金淼, 齐会民, 张建, 等. 新型含硅芳炔树脂及其复合材料的性能[J]. 化工新型材料, 2008, 36(12): 45-46.GAO J M, QI H M, ZHANG J, et al. Properties of new siliconaryl-acetylene resin and its composite materials[J]. New Chemical Materials. 2008, 36(12): 45-46(in Chinese). |
[10] | 吴聪, 陈南春, 吴志能, 等. 改性介孔硅-ESO/聚丙烯三元体系复合材料增强增韧机制[J]. 复合材料学报, 2017, 34(4): 723-729.WU C, CHEN N C, WU Z N, et al. Reinforcing and toughening mechanisms of modified diatomite-epoxy soybean oil/polypropylene composites[J]. Acta Materiae Compositae Sinica, 2017, 34(4): 723-729(in Chinese). |
[11] | 曾宏, 张安强. 催化异氰酸酯基与羟基反应选择性的研究进展[J]. 聚氨酯工业, 2017, 32(5): 1-4.ZENG H, ZHANG A Q. The selectivity of catalysts for the reaction of isocyanate and hydroxyl groups[J]. Polyurethane Industry, 2017, 32(5): 1-4(in Chinese). |
[12] | 黄赤, 汪波, 秦岩, 等. 空心玻璃微球含量对环氧复合泡沫塑料性能的影响[J]. 复合材料学报, 2016, 33(8): 1630-1637.HUANG C, WANG B, QIN Y, et al. Effects of hollow glass microsphere content on properties of epoxy syntactic foams[J]. Acta Materiae Compositae Sinica, 2016, 33(8): 1630-1637(in Chinese). |
[13] | 吕婕, 姜丽, 吴金剑, 等. 聚氨酯预聚体改性双酚A型氰酸酯树脂的研究[J]. 材料导报, 2015, 29(24): 36-39.LV J, JIANG L, WU J J, et al. Study of polyurethane prepolymer modified bisphenol A cyanate ester resins[J]. Mterials Review, 2015, 29(24): 36-39(in Chinese). |
[14] | 吴金剑, 谢佳武, 王志娟, 等. F-48环氧树脂改性双酚A型氰酸酯树脂的研究[J]. 材料导报, 2014, 28(14): 91-94.WU J J, XIE J W, WANG Z J, et al. Study of F-48 epoxy resin modified bisphenol A cyanate ester resins[J]. Materials Review, 2014, 28(14): 91-94(in Chinese). |
[15] | 袁慧五, 饶秋华. 无机填料对低粘度高性能环氧树脂性能的影响[J]. 热固性树脂, 2007, 22(6): 33-35.YUAN H W, RAO Q H. The influence of inorganic filler on the performances of high property and low viscosity epoxy resin[J]. Thermosetting Resin, 2007, 22(6): 33-35(in Chinese). |
[16] | 赵彦生, 王华, 党在清, 等. 无机纳米粒子增韧聚丙烯及其机理研究[J]. 现代塑料加工应用, 2006, 18(6): 36-38.ZHAO Y S, WANG H, DANG Z Q, et al. The research of polypropylene toughened by inorganic nanoparticles and toughening mechanisms[J]. Modern Plastics Processing and Applications, 2006, 18(6): 36-38(in Chinese). |
[17] | 高峰, 矫桂琼, 宁荣昌, 等. 层间颗粒增韧复合材料层压板的损伤阻抗特性[J]. 复合材料学报, 2005, 22(2): 116-120.GAO F, JIAO G Q, NING R C, et al. Damage resistance of the composite laminates with interlayer thermoplastic particles[J]. Acta Materiae Compositae Sinica, 2005, 22(2): 116-120(in Chinese). |
[18] | MASAYOSHI I, KOHJI I, KENJI I, et al. New highly heat-resistant polymers containing silicon: Poly(silyleneethynylenephenyleneethynylene)s[J]. Macromolecules, 1997, 30(4): 694-701. |
[19] | AND S K, OKITA K, KAKIGANO T, et al. Thermosetting mechanism study of poly[(phenylsilylene)ethynylene-1,3-phenylenee-thynylene] by solid-state NMR spectroscopy and computational chemistry[J]. Macromolecules, 1998, 31(9): 2804-2808. |
[20] | ZHANG J, HUANG J, ZHOU W, et al. Fiber reinforced silicon-containing arylacetylene resin composites[J]. eXPRESS Polymer Letters, 2007, 1(12): 831-836. |
[21] | OGASAWARA T, ISHIKAWA T, ITOH M, et al. Carbon fiber reinforced composites with newly developed silicon containing polymer MSP[J]. Advanced Composite Materials, 2001, 10(4): 319-327. |
[22] | GUO K K, LI P, ZHU Y P, et al. Thermal curing and degradation behaviour of silicon-containing arylacetylene resins[J]. Polymer Degradation and Stability, 2016, 131: 98-105. |
[23] | 汤乐旻, 周燕, 田鑫, 等. 改性含硅芳炔树脂及其复合材料性能研究[J]. 玻璃钢/复合材料, 2012(6): 41-46.TANG L Y, ZHOU Y, TIAN X, et al. Properties of siliconarylacetylene resin and its composite materials[J]. Fiber Reinforced Plastics/Composites, 2012(6): 41-46(in Chinese). |
[24] | 武光顺. 碳纤维表面纳米结构修饰及其MPSR复合材料性能研究[D]. 哈尔滨: 哈尔滨工业大学, 2016.WU G S. Study on the nanostructure based on the surface of carbon fiber and the properties of CF/MPSR composites[D]. Harbin: Harbin Institute of Technology, 2016(in Chinese). |
[25] | 韩梦娜, 郭康康, 王帆, 等. 乙炔基封端液晶-含硅芳炔共聚树脂的固化机理[J]. 功能高分子学报, 2017, 30(3): 279-289.HAN M N, GUO K K, WANG F, et al. Curing mechanism of acetylene terminated liquid crystal and silicon-containing arylacetylene copolymer resin[J]. Journal of Functional Polymers, 2017, 30(3): 279-289(in Chinese). |
[26] | 李孟宇, 马雅婷, 赵蕾, 等. 纳米SiO2改性环氧树脂复合材料的热稳定性及使用寿命[J]. 复合材料学报, 2017, 34(11): 2421-2427.LI M Y, MA Y T, ZHAO L, et al. Thermal stability and service life of nano-SiO2 modified epoxy composites[J]. Acta Materiae Compositae Sinica, 2017, 34(11): 2421-2427(in Chinese). |
[27] | 郑艳红, 蔡楚江, 沈志刚, 等. 微纳米SiO2/PP复合材料增强增韧的实验研究[J]. 复合材料学报, 2007, 24(6): 19-25.ZHENG Y H, CAI C J, SHEN Z G, et al. Toughening and strengthening of micro-and nano-SiO2/PP composites[J]. Acta Materiae Compositae Sinica, 2007, 24(6): 19-25(in Chinese). |
[28] | 赵春宝, 张楠楠. 氰酸酯/环氧树脂/苯基三硅羟基倍半硅氧烷复合材料研究[J]. 化工新型材料, 2012, 40(11): 40-42.ZHAO C B, ZHANG N N. Study on cyanate ester/epoxy resin/trisilanolphenyl polyhedral oligomeric silsesquioxane (POSS) composites[J]. New Chemical Materials, 2012, 40(11): 40-42(in Chinese). |