硅氧烷-丁二烯嵌段共聚物改性二氧化硅填充丁苯橡胶/顺丁橡胶复合材料

徐妍; 李敏; 崔冬梅

doi:10.11777/j.issn1000-3304.2026.26147

您当前的位置：

首页 >

文章列表页 >

硅氧烷-丁二烯嵌段共聚物改性二氧化硅填充丁苯橡胶/顺丁橡胶复合材料

研究论文 | 更新时间：2026-08-06

- 硅氧烷-丁二烯嵌段共聚物改性二氧化硅填充丁苯橡胶/顺丁橡胶复合材料
- Silicone-Butadiene Block Copolymer Modified Silica-filled SBR/BR Rubber Composite Material
- 高分子学报 2026年页码：1-11
- 作者机构：
  
  1.中国科学院长春应用化学研究所高分子科学与技术全国重点实验室长春 130022
  2.中国科学技术大学应用化学与工程学院合肥 230026
- 作者简介：
  
  E-mail: dmcui@ciac.ac.cn
- 基金信息：
  
  国家自然科学基金(基金号 22331010)
- DOI：10.11777/j.issn1000-3304.2026.26147
  中图分类号：
- CSTR：32057.14.GFZXB.2026.7705
- 收稿：2026-04-29，
  
  录用：2026-07-31，
  
  网络首发：2026-08-06，
- 稿件说明：
移动端阅览
徐妍, 李敏, 崔冬梅. 硅氧烷-丁二烯嵌段共聚物改性二氧化硅填充丁苯橡胶/顺丁橡胶复合材料. 高分子学报, doi: 10.11777/j.issn1000-3304.2026.26147.

Xu, Y.; Li, M.; Cui, D. M. Silicone-butadiene block copolymer modified silica-filled SBR/BR rubber composite material. Acta Polymerica Sinica (in Chinese), doi: 10.11777/j.issn1000-3304.2026.26147.
徐妍, 李敏, 崔冬梅. 硅氧烷-丁二烯嵌段共聚物改性二氧化硅填充丁苯橡胶/顺丁橡胶复合材料. 高分子学报, doi: 10.11777/j.issn1000-3304.2026.26147. DOI： CSTR： 32057.14.GFZXB.2026.7705.

Xu, Y.; Li, M.; Cui, D. M. Silicone-butadiene block copolymer modified silica-filled SBR/BR rubber composite material. Acta Polymerica Sinica (in Chinese), doi: 10.11777/j.issn1000-3304.2026.26147. DOI： CSTR： 32057.14.GFZXB.2026.7705.

摘要

为改善白炭黑在非极性丁苯橡胶/顺丁橡胶(SBR/BR)基体中的分散性并提升复合材料性能，本研究设计合成了三乙氧基硅烷封端的硅氧烷-丁二烯共聚物(TESIPB)，并将其作为界面改性剂用于白炭黑填充SBR/BR复合材料. 通过调控硅氧烷封端、聚硅氧烷主链苯环含量及液体聚丁二烯分子量，系统考察了共聚物改性剂对复合材料的硫化特性、填料分散性、力学性能及动态力学性能的影响. 结果表明，TESIPB能有效抑制白炭黑团聚，促进填料均匀分散，显著提高复合材料的撕裂强度和断裂伸长率. 当TESIPB添加量为2.5 phr时，复合材料拉伸强度达22.7 MPa，断裂伸长率提升至1444%，撕裂强度达75.5 N/mm. 动态力学分析显示，适量TESIPB可降低复合材料在60 ℃的损耗因子(tan

)，同时提高0 ℃附近的tan

值，有助于实现低滚动阻力和良好抗湿滑性能的平衡. 本研究为开发高性能绿色轮胎用橡胶复合材料提供了新思路.

Abstract

To improve silica dispersion in a non-polar SBR/BR matrix and enhance composite performance

a polysiloxane-polybutadiene copolymer (TESIPB) with triethoxysilane end groups was designed and synthesized as an interface modifier for silica-filled SBR/BR composites. The effects of the copolymer on vulcanization

filler dispersion

mechanical and dynamic properties were systematically investigated by adjusting its siloxane end groups

benzene ring content

and liquid butadiene molecular weight. Results showed that TESIPB effectively inhibited silica agglomeration

promoted uniform filler dispersion

and significantly improved tear strength and elongation at break. With 2.5 parts of TESIPB

the composite achieved a tensile strength of 22.73 MPa

elongation at break of 1444%

and tear strength of 75.5 N/mm. Dynamic mechanical analysis indicated that an appropriate amount of TESIPB reduced tan

at 60 ℃ while increasing tan

near 0 ℃

enabling a balance between low rolling resistance and good wet-skid resistance. This work offers a new strategy for high-performance green tire rubber composites.

关键词

Keywords

references

Li M. Y. ; Wang K. Y. ; Xiong Y. Z. Multiple intermolecular interaction to improve the abrasion resistance and wet skid resistance of eucommia ulmoides gum/styrene butadiene rubber composite . Materials , 2021 , 14 ( 18 ), 5246 . doi: 10.3390/ma14185246 http://dx.doi.org/10.3390/ma14185246

Takino H. ; Nakayama R. ; Yamada Y. ; Kohjiya S. ; Matsuo T. Viscoelastic properties of elastomers and tire wet skid resistance . Rubber Chem. Technol. , 1997 , 70 ( 4 ), 584 - 594 . doi: 10.5254/1.3538445 http://dx.doi.org/10.5254/1.3538445

Wu J. ; Zhang C. ; Wang Y. ; Su B. ; Gond B. Investigation on wet skid resistance of tread rubber . Exp. Technol. , 2019 , 43 ( 1 ), 81 - 89 . doi: 10.1007/s40799-018-0272-z http://dx.doi.org/10.1007/s40799-018-0272-z

Wolff S. Chemical aspects of rubber reinforcement by fillers . Rubber Chem. Technol. , 1996 , 69 ( 3 ), 325 - 346 . doi: 10.5254/1.3538376 http://dx.doi.org/10.5254/1.3538376

Barrera C. S. ; Cornish K. High performance waste-derived filler/carbon black reinforced guayule natural rubber composites . Ind. Crops Prod. , 2016 , 86 , 132 - 142 . doi: 10.1016/j.indcrop.2016.03.021 http://dx.doi.org/10.1016/j.indcrop.2016.03.021

Bijina V. ; Jandas P. J. ; Joseph S. ; Gopu J. ; Abhitha K. ; John H. Recent trends in industrial and academic developments of green tyre technology . Polym. Bull. , 2023 , 80 ( 8 ), 8215 - 8244 . doi: 10.1007/s00289-022-04445-2 http://dx.doi.org/10.1007/s00289-022-04445-2

Deng S. ; Chen R. X. ; Duan S. Y. ; Jia Q. X. ; Hao X. M. ; Zhang L. Q. Research progress on sustainability of key tire materials . SusMat , 2023 , 3 ( 5 ), 581 - 608 . doi: 10.1002/sus2.159 http://dx.doi.org/10.1002/sus2.159

Hu S. K. ; He S. Y. ; Wang Y. M. ; Wu Y. W. ; Shou T. ; Yin D. X. ; Mu G. Y. ; Zhao X. Y. ; Gao Y. Y. ; Liu J. ; Li F. Z. ; Guo M. M. ; Zhang L. Q. Self-repairable, recyclable and heat-resistant polyurethane for high-performance automobile tires . Nano Energy , 2022 , 95 , 107012 . doi: 10.1016/j.nanoen.2022.107012 http://dx.doi.org/10.1016/j.nanoen.2022.107012

Li F. Z. ; Liu F. ; Liu J. ; Gao Y. Y. ; Lu Y. L. ; Chen J. F. ; Yang H. B. ; Zhang L. Q. Thermo-mechanical coupling analysis of transient temperature and rolling resistance for solid rubber tire: numerical simulation and experimental verification . Compos. Sci. Technol. , 2018 , 167 , 404 - 410 . doi: 10.1016/j.compscitech.2018.08.034 http://dx.doi.org/10.1016/j.compscitech.2018.08.034

Luginsland H. D. ; Fröhlich J. ; Wehmeier A. Influence of different silanes on the reinforcement of silica-filled rubber compounds . Rubber Chem. Technol. , 2002 , 75 ( 4 ), 563 - 579 . doi: 10.5254/1.3544984 http://dx.doi.org/10.5254/1.3544984

Xu T. W. ; Jia Z. X. ; Li J. L. ; Luo Y. F. ; Jia D. M. ; Peng Z. Study on the dispersion of carbon black/silica in SBR/BR composites and its properties by adding epoxidized natural rubber as a compatilizer . Polym. Compos. , 2018 , 39 ( 2 ), 377 - 385 . doi: 10.1002/pc.23946 http://dx.doi.org/10.1002/pc.23946

Hashim A. S. ; Azahari B. ; Ikeda Y. ; Kohjiya S. The effect of bis(3-triethoxysilylpropyl) tetrasulfide on silica reinforcement of styrene-butadiene rubber . Rubber Chem. Technol. , 1998 , 71 ( 2 ), 289 - 299 . doi: 10.5254/1.3538485 http://dx.doi.org/10.5254/1.3538485

Koureas M. ; Kirgou P. ; Amoutzias G. ; Hadjichristodoulou C. ; Gourgoulianis K. ; Tsakalof A. Target analysis of volatile organic compounds in exhaled breath for lung cancer discrimination from other pulmonary diseases and healthy persons . Metabolites , 2020 , 10 ( 8 ), 317 . doi: 10.3390/metabo10080317 http://dx.doi.org/10.3390/metabo10080317

Li S. Q. ; Zhai X. B. ; Chen Z. ; Han D. L. ; Ye X. ; Zhang L. Q. Balancing the "magic triangle" performance of tire rubber nanocomposites with novel low VOC silane coupling agents . Compos. Commun. , 2024 , 46 , 101836 . doi: 10.1016/j.coco.2024.101836 http://dx.doi.org/10.1016/j.coco.2024.101836

Kong S. X. ; Wu S. W. ; Tang Z. H. ; Guo B. C. Hydrogen bond-containing oligomer as a facile interfacial mediator in rubber/silica composites . Compos. Commun. , 2023 , 37 , 101413 . doi: 10.1016/j.coco.2022.101413 http://dx.doi.org/10.1016/j.coco.2022.101413

Xu Y. H. ; Liu Y. D. ; Qin X. ; Liu J. ; Zhang L. Q. A novel strategy to functionalize styrene butadiene rubber toward enhanced interfacial interaction with silica . J. Appl. Polym. Sci. , 2023 , 140 ( 39 ), e 54476 . doi: 10.1002/app.54476 http://dx.doi.org/10.1002/app.54476

Zhang C. F. ; Tang Z. H. ; Guo B. C. ; Zhang L. Q. Concurrently improved dispersion and interfacial interaction in rubber/nanosilica composites via efficient hydrosilane functionalization . Compos. Sci. Technol. , 2019 , 169 , 217 - 223 . doi: 10.1016/j.compscitech.2018.11.016 http://dx.doi.org/10.1016/j.compscitech.2018.11.016

Ryu C. S. ; Kim K. J. Interfacial adhesion in silica-silane filled NR composites: a short review . Polymers , 2022 , 14 ( 13 ), 2705 . doi: 10.3390/polym14132705 http://dx.doi.org/10.3390/polym14132705

Surya I. ; Ismail H. ; Azura A. R. Alkanolamide as an accelerator, filler-dispersant and a plasticizer in silica-filled natural rubber compounds . Polym. Test. , 2013 , 32 ( 8 ), 1313 - 1321 . doi: 10.1016/j.polymertesting.2013.07.015 http://dx.doi.org/10.1016/j.polymertesting.2013.07.015

Yan H. X. ; Sun K. ; Zhang Y. ; Zhang Y. X. Effect of nitrile rubber on properties of silica-filled natural rubber compounds . Polym. Test. , 2005 , 24 ( 1 ), 32 - 38 . doi: 10.1016/j.polymertesting.2004.07.011 http://dx.doi.org/10.1016/j.polymertesting.2004.07.011

Yan H. X. ; Sun K. ; Zhang Y. ; Zhang Y. X. ; Fan Y. Z. Effects of silane coupling agents on the vulcanization characteristics of natural rubber . J. Appl. Polym. Sci. , 2004 , 94 ( 4 ), 1511 - 1518 . doi: 10.1002/app.21071 http://dx.doi.org/10.1002/app.21071

Yan H. X. ; Tian G. H. ; Sun K. ; Zhang Y. ; Zhang Y. X. Effect of silane coupling agent on the polymer-filler interaction and mechanical properties of silica-filled NR . J. Polym. Sci. Part B Polym. Phys. , 2005 , 43 ( 5 ), 573 - 584 . doi: 10.1002/polb.20343 http://dx.doi.org/10.1002/polb.20343

Cui M. Z. ; Liu L. ; Kim J. Infrared spectroscopy evidence for the hydrosilylation of rubbers and hydrogen-containing polysiloxane via heat processing . J. Appl. Polym. Sci. , 2012 , 125 ( 4 ), 3000 - 3005 . doi: 10.1002/app.35647 http://dx.doi.org/10.1002/app.35647

Redaelli M. ; D'Arienzo M. ; Brus J. ; Di Credico B. ; Geppi M. ; Giannini L. ; Matejka L. ; Martini F. ; Panattoni F. ; Spirkova M. ; Šlouf M. ; Scotti R. ; Morazzoni F. On the key role of SiO 2 @POSS hybrid filler in tailoring networking and interfaces in rubber nanocomposites . Polym. Test. , 2018 , 65 , 429 - 439 . doi: 10.1016/j.polymertesting.2017.12.022 http://dx.doi.org/10.1016/j.polymertesting.2017.12.022

Hosseini S. M. ; Torbati-Fard N. ; Kiyani H. ; Razzaghi-Kashani M. Comparative role of Interface in reinforcing mechanisms of nano silica modified by silanes and liquid rubber in SBR composites . J. Polym. Res. , 2016 , 23 ( 9 ), 203 . doi: 10.1007/s10965-016-1096-0 http://dx.doi.org/10.1007/s10965-016-1096-0

Wang D. ; Chen J. L. ; Tang Z. H. ; Huang R. Y. ; Xiao Y. L. ; Chen J. D. ; Yin P. C. ; Guo B. C. ; Zhang L. Q. Exploring epoxy-functionalized polysulfide as a VOC-free and highly effective interfacial modifier for silica-filled rubber composites . Macromolecules , 2024 , 57 ( 2 ), 470 - 480 . doi: 10.1021/acs.macromol.3c01972 http://dx.doi.org/10.1021/acs.macromol.3c01972

Xu L. ; Li B. G. ; Jie S. Y. ; Li Z. S. ; Bu Z. Y. 110 th Anniversary: the epoxidation of polybutadiene via reaction-controlled phase-transfer catalysis . Ind. Eng. Chem. Res. , 2019 , 58 ( 29 ), 13085 - 13092 . doi: 10.1021/acs.iecr.9b02371 http://dx.doi.org/10.1021/acs.iecr.9b02371

Zhou Q. Z. ; Jie S. Y. ; Li B. G. Facile synthesis of novel HTPBs and EHTPBs with high cis -1,4 content and extremely low glass transition temperature . Polymer , 2015 , 67 , 208 - 215 . doi: 10.1016/j.polymer.2015.04.078 http://dx.doi.org/10.1016/j.polymer.2015.04.078

Zhou Q. Z. ; Wang A. Q. ; Dai L. ; Jie S. Y. ; Li B. G. Cleavable polybutadiene rubber: a versatile precursor to hydroxyl-terminated or multi-hydroxyl polybutadiene and polyethylene . Polymer , 2016 , 107 , 306 - 315 . doi: 10.1016/j.polymer.2016.11.033 http://dx.doi.org/10.1016/j.polymer.2016.11.033

Ai L. Q. ; Chen Y. ; He L. J. ; Luo Y. M. ; Li S. H. ; Xu C. H. Synthesis of structured polysiloxazanes via a Piers-Rubinsztajn reaction . Chem. Commun. , 2019 , 55 ( 93 ), 14019 - 14022 . doi: 10.1039/c9cc07312d http://dx.doi.org/10.1039/c9cc07312d

Grande J. B. ; Thompson D. B. ; Gonzaga F. ; Brook M. A. Testing the functional tolerance of the Piers-Rubinsztajn reaction: a new strategy for functional silicones . Chem. Commun. , 2010 , 46 ( 27 ), 4988 . doi: 10.1039/c0cc00369g http://dx.doi.org/10.1039/c0cc00369g

Parks D. J. ; Blackwell J. M. ; Piers W. E. Studies on the mechanism of B(C 6 F 5 ) 3 -catalyzed hydrosilation of carbonyl functions . J. Org. Chem., 2000, 65 ( 10 ), 3090 - 3098 .

Seo Y. ; Gudz A. ; Lowe J. M. ; Gagné M. R. Selective deoxygenation of gibberellic acid with fluoroarylborane catalysts . Tetrahedron , 2019 , 75 ( 49 ), 130712 . doi: 10.1016/j.tet.2019.130712 http://dx.doi.org/10.1016/j.tet.2019.130712

Kruželák J. ; Mikolajová M. ; Kvasničáková A. ; Džuganová M. ; Chodák I. ; Hronkovič J. ; Preťo J. ; Hudec I. Combined sulfur and peroxide vulcanization of filled and unfilled EPDM-based rubber compounds . Materials , 2023 , 16 ( 16 ), 5596 . doi: 10.3390/ma16165596 http://dx.doi.org/10.3390/ma16165596

Zhang P. ; Zhao F. ; Yuan Y. ; Shi X. Y. ; Zhao S. G. Network evolution based on general-purpose diene rubbers/sulfur/TBBS system during vulcanization (I) . Polymer , 2010 , 51 ( 1 ), 257 - 263 . doi: 10.1016/j.polymer.2009.10.057 http://dx.doi.org/10.1016/j.polymer.2009.10.057

Zhang S. ; Cheng Y. H. ; Galuska L. ; Roy A. ; Lorenz M. ; Chen B. B. ; Luo S. C. ; Li Y. T. ; Hung C. C. ; Qian Z. Y. ; St Onge P. B. J. ; Mason G. T. ; Cowen L. ; Zhou D. S. ; Nazarenko S. I. ; Storey R. F. ; Schroeder B. C. ; Rondeau-Gagné S. ; Chiu Y. C. ; Gu X. D. Tacky elastomers to enable tear-resistant and autonomous self-healing semiconductor composites . Adv. Funct. Mater. , 2020 , 30 ( 27 ), 2000663 . doi: 10.1002/adfm.202000663 http://dx.doi.org/10.1002/adfm.202000663

Martin P. J. ; Brown P. ; Chapman A. V. ; Cook S. Silica-reinforced epoxidized natural rubber tire treads: performance and durability . Rubber Chem. Technol. , 2015 , 88 ( 3 ), 390 - 411 . doi: 10.5254/rct.15.85940 http://dx.doi.org/10.5254/rct.15.85940

Wan S. H. ; Lu X. B. ; Zhao H. G. ; Chen S. B. ; Cai S. W. ; He X. R. ; Zhang R. Effect of graphene oxide modified with organic amine on the aging resistance, rolling loss and wet-skid resistance of solution polymerized styrene-butadiene rubber . Materials , 2020 , 13 ( 5 ), 1025 . doi: 10.3390/ma13051025 http://dx.doi.org/10.3390/ma13051025

浏览量

下载量

CSCD

文章被引用时，请邮件提醒。

提交

工具集

关联资源

硅烷封端液体聚丁二烯对二氧化硅填充丁苯橡胶/顺丁橡胶复合材料性能的影响

基于VOCl3活性中心的还原-氧化(V3+/V2+)高效合成无溶剂液体三元乙丙橡胶

膦化聚硅氧烷质子交换膜的制备及其性能研究

聚合物模板微球表面电性对中空二氧化硅微球形貌的影响

脂环族/直链脂肪族硬段复配对聚氨酯共混材料结构与性能的影响