液体天然橡胶对湿法混炼制备NR/白炭黑复合材料的增容机理研究
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摘要
采用液体天然橡胶(liquid natural rubber)为增容剂,基于湿法混炼工艺制备天然橡胶/白炭黑(W(NR/SiO_2))复合材料。利用FT-IR、SEM、万能拉力机分别对复合材料的微观结构、拉伸断裂形貌及力学性能进行分析,通过Mooney-Rivilin方程和界面相互作用方程对橡胶-填料界面相互作用定量计算,并探讨了LNR的增容机理。结果表明,使用LNR增容后,NR与白炭黑两相界面变得模糊,断面表现为韧性断裂;硫化胶力学性能在LNR改性后得到改善,白炭黑用量为60phr时表现最为明显,拉伸强度提高了25.73%;不同方程计算结果表明,白炭黑用量一定情况下,使用LNR增容后复合材料两相界面相互作用增强。LNR具有良好的增容效果,复合材料良好的相容性是LNR与NR和白炭黑两相同时发生作用形成增容界面的结果。
Natural rubber/silica composites(NR/SiO_2) was prepared by wet mixing technology with liquid natural rubber(LNR) as compatibilizer.Micro-Structure,tensile fracture surface,mechanical properties and fillerrubber interaction were studied by scanning electron microscopy,FT-IR spectroscopy and universal tensile machine.The rubber-filler interaction was evaluated by Mooney-Rivilin equation and interfacial interaction equation quantitatively.The compatibilizing mechanism of LNR for W(NR/SiO_2) composites was also investigated.The results showed that the SiO_2 particles are tightly encompassed by NR in the presence of LNR and fracture surfaces appeared toughness fracture;good mechanical properties was observed,the tensile strength increase by25.73% when silica was 60phr;the equations showed that filler-rubber interaction have great enhancements under certain amount of silica.It is reveal that LNR has better compatibility,which is attributed to LNR reaction with both NR and SiO_2 to form compatibilizing interface.
Natural rubber/silica composites(NR/SiO_2) was prepared by wet mixing technology with liquid natural rubber(LNR) as compatibilizer.Micro-Structure,tensile fracture surface,mechanical properties and fillerrubber interaction were studied by scanning electron microscopy,FT-IR spectroscopy and universal tensile machine.The rubber-filler interaction was evaluated by Mooney-Rivilin equation and interfacial interaction equation quantitatively.The compatibilizing mechanism of LNR for W(NR/SiO_2) composites was also investigated.The results showed that the SiO_2 particles are tightly encompassed by NR in the presence of LNR and fracture surfaces appeared toughness fracture;good mechanical properties was observed,the tensile strength increase by25.73% when silica was 60phr;the equations showed that filler-rubber interaction have great enhancements under certain amount of silica.It is reveal that LNR has better compatibility,which is attributed to LNR reaction with both NR and SiO_2 to form compatibilizing interface.
引文
[1]张立群.天然橡胶及生物基弹性体[M].北京:化学工业出版社,2014:42-43.
[2]Peng Zheng,Zhong Jieping,Liao Shuangquan.Development of Modification of Natural Rubber[J].Polymer bulletin,2014,(5):41.彭政,钟杰平,廖双泉.天然橡胶改性研究进展[J].高分子通报,2014,(5):41.
[3]Azira A A,Verasamy D,Abdullah N S,et al.Epoxidised natural rubber/silica organic-inorganic composite for tyre masterbatch[J].Advanced Materials Research,2015,1109:205-209.
[4]Liao Lusheng,Zhang Fuquan,Wang Bingbing,et al.Effect of epoxidized natural rubber on the properties of natural rubber/silica wet masterbatch[J].Chinese Journal of Tropical Crops,2016,37(7):1387.廖禄生,张福全,王兵兵,等.环氧化天然橡胶对天然橡胶/白炭黑湿法母炼胶性能的影响[J].热带作物学报,2016,37(7):1387.
[5]Wang M J,Morris M D,Kutsovsky Y.Effect of fumed silica surface area on silicone rubber reinforcement[J].Kgk Rubberpoint,2008,61(3):107-117.
[6]Kaewsakul W,Sahakaro K,Dierkes W K,et al.Optimization of mixing conditions for silica-reinforced natural rubber tire tread compounds[J].Rubber Chemistry&Technology,2012,85(2):277-294.
[7]Byers J T.Fillers for balancing passenger tire tread properties[J].Rubber Chemistry and Technology,2002,75(3):527-548.
[8]Seekkuarachchi I N,Tanaka K,Kumazawa H,et al.Dispersion mechanism of nano-particulate aggregates using a high pressure wet-type jet mill[J].Chemical Engineering Science,2008,63(9):2341-2366.
[9]Fan Zongqing,Song Lixian,Li Zhanhong,et al.Surface modification and characterization of silica using behenyl alcohol with long alkyl group[J].Journal of Synthetic Crystals,2015,44(1):233.范宗青,宋丽贤,黎展宏,等.白炭黑的长链烷基官能化改性及表征[J].人工晶体学报,2015,44(1):233.
[10]Print Journalist.Development progress of wet mixing for new rubber material technology[J].China Rubber/Plastics Technology and Equipment,2015,41(7):1.本刊记者.湿法混炼橡胶新材料工艺技术的开发进展[J].橡塑技术与装备,2015,41(7):1.
[11]Wang M J,Wang T,Wong Y L,et al.NR/carbon black masterbatch produced with continuous liquid phase mixing[J].Kautschuk Und Gummi Kunststoffe,2002,55(7):388-396.
[12]林艳芬.湿炼法NR/nSiO2和NR/炭黑复合材料的制备、结构与性能的研究[D].广州:华南理工大学,2013.
[13]Prasertsri S,Rattanasom N.Fumed and precipitated silica reinforced natural rubber composites prepared from latex system:Mechanical and dynamic properties[J].Polymer Testing,2012,31(5):593-605.
[14]Prasertsri S,Rattanasom N.Mechanical and damping properties of silica/natural rubber composites prepared from latex system[J].Polymer Testing,2011,30(5):515-526.
[15]Miloskovska E,Hansen M R,Friedrich C,et al.In situ silica nanoparticle formation in a rubber matrix monitored via real-time SAXS and solid-state NMR spectroscopy[J].Macromolecules,2014,47(15):5174-5185.
[16]Zhou Rongjie,Li Chaoqun,Yang Xiaohong,et al.Effect of Liquid Natural Rubber as Softener on the Property of NR/Silica Composit[J].Materials Review:Research,2015,29(4):60.周荣杰,李超群,杨晓红,等.液体天然橡胶作软化剂对NR/白炭黑复合材料性能的影响[J].材料导报:研究篇,2015,29(4):60.
[17]Ibrahim A,Sahrim A,Som S C.Blending of natural rubber with linear low-density polyethylene[J].Journal of Applied Polymer Science,1995,58(58):1125-1133.
[18]Pranee P,Sayan D.Ultraviolet-curable liquid natural rubber[J].Journal of Applied Polymer Science,2000,78(8):1478-1485.
[19]Kargarzadeh H,Ahmad I,Abdullah I,et al.Functionalized liquid natural rubber and liquid epoxidized natural rubber:apromising green toughening agent for polyester[J].Journal of Applied Polymer Science,2015,132(3):1-15.
[20]Li Y,Han B,Wen S,et al.Effect of the temperature on surface modification of silica and properties of modified silica filled rubber composites[J].Composites Part AApplied Science&Manufacturing,2014,62(17):52-59.
[21]张帆.材料性能学[M].上海:上海交通大学出版社,2014:113-117.
[22]Wolff S.Optimization of silane-silica OTR compounds.Part 1:variations of mixing temperature and time during the modification of silica with bis-(3-triethoxisilylpropyl)-tetrasulfide[J].Rubber Chemistry&Technology,1982,55(4):967-989.
[23]吴思武.橡胶/纳米碳素复合材料的分散与界面研究[D].广州:华南理工大学,2014.
[24]Mooney M.A theory of large elastic deformation[J].Nature,1940,11(9):582-592.
[25]Rivlin R S,Saunders D W.Large elastic deformations of isotopic materials.VII:experiments on the deformation of rubber[J].Philosophical Transactions of the Royal Society B Biological Sciences,1951,243(243):251-288.
[26]Joly S,Garnaud G,Ollitrault R,et al.Organically modified layered silicates as reinforcing fillers for natural rubber[J].Chemistry of Materials,2002,14(10):4202-4208.
[27]Bokobza L,Erman B.A theoretical and experimental study of filler effect on stress-deformation-segmental orientation relations for poly(dimethylsiloxane)networks[J].Macromolecules,2000,33(23):8858-8864.
[28]Lei Y D,Tang Z H,Guo B C,et al.Synthesis of novel functional liquid and its application as a modifier in SBR/silica composites[J].Express Polymer Letters,2010,4(11):692-703.
[2]Peng Zheng,Zhong Jieping,Liao Shuangquan.Development of Modification of Natural Rubber[J].Polymer bulletin,2014,(5):41.彭政,钟杰平,廖双泉.天然橡胶改性研究进展[J].高分子通报,2014,(5):41.
[3]Azira A A,Verasamy D,Abdullah N S,et al.Epoxidised natural rubber/silica organic-inorganic composite for tyre masterbatch[J].Advanced Materials Research,2015,1109:205-209.
[4]Liao Lusheng,Zhang Fuquan,Wang Bingbing,et al.Effect of epoxidized natural rubber on the properties of natural rubber/silica wet masterbatch[J].Chinese Journal of Tropical Crops,2016,37(7):1387.廖禄生,张福全,王兵兵,等.环氧化天然橡胶对天然橡胶/白炭黑湿法母炼胶性能的影响[J].热带作物学报,2016,37(7):1387.
[5]Wang M J,Morris M D,Kutsovsky Y.Effect of fumed silica surface area on silicone rubber reinforcement[J].Kgk Rubberpoint,2008,61(3):107-117.
[6]Kaewsakul W,Sahakaro K,Dierkes W K,et al.Optimization of mixing conditions for silica-reinforced natural rubber tire tread compounds[J].Rubber Chemistry&Technology,2012,85(2):277-294.
[7]Byers J T.Fillers for balancing passenger tire tread properties[J].Rubber Chemistry and Technology,2002,75(3):527-548.
[8]Seekkuarachchi I N,Tanaka K,Kumazawa H,et al.Dispersion mechanism of nano-particulate aggregates using a high pressure wet-type jet mill[J].Chemical Engineering Science,2008,63(9):2341-2366.
[9]Fan Zongqing,Song Lixian,Li Zhanhong,et al.Surface modification and characterization of silica using behenyl alcohol with long alkyl group[J].Journal of Synthetic Crystals,2015,44(1):233.范宗青,宋丽贤,黎展宏,等.白炭黑的长链烷基官能化改性及表征[J].人工晶体学报,2015,44(1):233.
[10]Print Journalist.Development progress of wet mixing for new rubber material technology[J].China Rubber/Plastics Technology and Equipment,2015,41(7):1.本刊记者.湿法混炼橡胶新材料工艺技术的开发进展[J].橡塑技术与装备,2015,41(7):1.
[11]Wang M J,Wang T,Wong Y L,et al.NR/carbon black masterbatch produced with continuous liquid phase mixing[J].Kautschuk Und Gummi Kunststoffe,2002,55(7):388-396.
[12]林艳芬.湿炼法NR/nSiO2和NR/炭黑复合材料的制备、结构与性能的研究[D].广州:华南理工大学,2013.
[13]Prasertsri S,Rattanasom N.Fumed and precipitated silica reinforced natural rubber composites prepared from latex system:Mechanical and dynamic properties[J].Polymer Testing,2012,31(5):593-605.
[14]Prasertsri S,Rattanasom N.Mechanical and damping properties of silica/natural rubber composites prepared from latex system[J].Polymer Testing,2011,30(5):515-526.
[15]Miloskovska E,Hansen M R,Friedrich C,et al.In situ silica nanoparticle formation in a rubber matrix monitored via real-time SAXS and solid-state NMR spectroscopy[J].Macromolecules,2014,47(15):5174-5185.
[16]Zhou Rongjie,Li Chaoqun,Yang Xiaohong,et al.Effect of Liquid Natural Rubber as Softener on the Property of NR/Silica Composit[J].Materials Review:Research,2015,29(4):60.周荣杰,李超群,杨晓红,等.液体天然橡胶作软化剂对NR/白炭黑复合材料性能的影响[J].材料导报:研究篇,2015,29(4):60.
[17]Ibrahim A,Sahrim A,Som S C.Blending of natural rubber with linear low-density polyethylene[J].Journal of Applied Polymer Science,1995,58(58):1125-1133.
[18]Pranee P,Sayan D.Ultraviolet-curable liquid natural rubber[J].Journal of Applied Polymer Science,2000,78(8):1478-1485.
[19]Kargarzadeh H,Ahmad I,Abdullah I,et al.Functionalized liquid natural rubber and liquid epoxidized natural rubber:apromising green toughening agent for polyester[J].Journal of Applied Polymer Science,2015,132(3):1-15.
[20]Li Y,Han B,Wen S,et al.Effect of the temperature on surface modification of silica and properties of modified silica filled rubber composites[J].Composites Part AApplied Science&Manufacturing,2014,62(17):52-59.
[21]张帆.材料性能学[M].上海:上海交通大学出版社,2014:113-117.
[22]Wolff S.Optimization of silane-silica OTR compounds.Part 1:variations of mixing temperature and time during the modification of silica with bis-(3-triethoxisilylpropyl)-tetrasulfide[J].Rubber Chemistry&Technology,1982,55(4):967-989.
[23]吴思武.橡胶/纳米碳素复合材料的分散与界面研究[D].广州:华南理工大学,2014.
[24]Mooney M.A theory of large elastic deformation[J].Nature,1940,11(9):582-592.
[25]Rivlin R S,Saunders D W.Large elastic deformations of isotopic materials.VII:experiments on the deformation of rubber[J].Philosophical Transactions of the Royal Society B Biological Sciences,1951,243(243):251-288.
[26]Joly S,Garnaud G,Ollitrault R,et al.Organically modified layered silicates as reinforcing fillers for natural rubber[J].Chemistry of Materials,2002,14(10):4202-4208.
[27]Bokobza L,Erman B.A theoretical and experimental study of filler effect on stress-deformation-segmental orientation relations for poly(dimethylsiloxane)networks[J].Macromolecules,2000,33(23):8858-8864.
[28]Lei Y D,Tang Z H,Guo B C,et al.Synthesis of novel functional liquid and its application as a modifier in SBR/silica composites[J].Express Polymer Letters,2010,4(11):692-703.