- Volume 55 Issue 1
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Preparation of Silica-Filled SBR Compounds with Low Rolling Resistance by Wet Masterbatch
- Yang, Jae-Kyoung (Mirae Scientific Instruments Inc.) ;
- Park, Wonhyeong (Mirae Scientific Instruments Inc.) ;
- Ryu, Changseok (Mirae Scientific Instruments Inc.) ;
- Kim, Sun Jung (Mirae Scientific Instruments Inc.) ;
- Kim, Doil (Mirae Scientific Instruments Inc.) ;
- Seo, Gon (Mirae Scientific Instruments Inc.)
- Received : 2019.11.14
- Accepted : 2019.12.20
- Published : 2020.03.31
The physical properties of silica-filled SBR compounds (WSBR) prepared using silica-SBR wet masterbatches (WMB) were systematically investigated to understand the effect of the surface treatment of silica on the reinforcement performance of SBR. Treatment of silica with bis(triethoxysilylpropyl)tetrasulfide (TESPT) in the liquid phase, followed by mixing with an SBR solution and recovery by water stripping, easily produced silica-SBR WMB. However, insufficient surface treatment in terms of the amount and stability of the incorporated TESPT led to considerable silica loss and inevitable TESPT elution. Pretreatment of silica in the gas phase with TESPT and another organic material that enabled the formation of organic networks among the silica particles on the surface provided hydrophobated silica, which could be used to produce silica-SBR WMB, in high yields of above 99%. The amount and type of organic material incorporated into silica greatly influenced the cure characteristics, processability, and tensile and dynamic properties of the WSBR compounds. The TESPT and organic material stably incorporated into silica increased their viscosity, while the organic networks dispersed on the silica surface were highly beneficial for reducing their rolling resistance. Excessive dosing of TESTP induced low viscosity and a high modulus. The presence of connection bonds formed by the reaction of glycidyloxy groups with amine groups on the silica surface resulted in physical entanglement of the rubber chains with the bonds in the WSBR compounds, leading to low rolling resistance without sacrificing the mechanical properties. Mixing of the hydrophobated silica with a rubber solution in the liquid phase improved the silica dispersion of WSBR compounds, as confirmed by their low Payne effect, and preservation of the low modulus enhanced the degree of entanglement.
Supported by : Korea Evaluation Institute of Industrial Technology (KEIT)
- X. Liu, S. Zhao, X. Zhang, X. Li, and Y. Bai, "Preparation, Structure, and Properties of Solution-Polymerized Styrene-Butadiene Ruber with Functionalized End-Groups and its Silica-Filled Composites", Polymer, 55, 1964 (2014). https://doi.org/10.1016/j.polymer.2014.02.067
- M. R. Pourhossaini and Razzaghi-Kashani, "Grafting Hydroxy-Terminated Polybutadiene onto Nanosilica Surface for Styrene Butadiene Rubber Compounds", J. Appl. Polym. Sci., 124, 4721 (2012).
- Y.-C. Tao, B. Dong, L.-Q. Zhang, and Y.-P. Wu, "Reaction of Silica-Silane Rubber and Properties of Silane-Silica/Solution-Polymerized Styrene-Butadiene Rubber Composite", Rubber Chem. Technol., 89, 526 (2016). https://doi.org/10.5254/rct.16.84812
- W. Feng, Z. T ang, P. Weng, and B. Guo, "Correlation of Filler Networking with Reinforcement and Dynamic Properties of SSBR/Carbon Black/Silica Composites", Rubber Chem. Technol., 88, 676 (2015). https://doi.org/10.5254/rct.15.84881
- M.-J. Wang, P. Zhang, and K. Mahmud, "Carbon-Silica Dual Phase Filler, A New Generation Reinforcing Agent for Rubber: Part IX. Application to Truck Tire Tread Compound", Rubber Chem. Technol., 74, 124 (2001). https://doi.org/10.5254/1.3547633
- H. M. Edmondson, "Processing Technology" in "Rubber Technology and Manufacture", ed. by C. M. Blow and C. Hepburn, 2nd Ed. p. 309, Butterworth Scientific, Oxford, 1982.
- Y. Qiu, A. Zhang, and L. Wang, "Carbon Black-Filled Styrene Butadiene Rubber Masterbatch Based on Simple Mixing of Latex and Carbon Black Suspension: Preparation and Mechanical Properties", J. Macromol. Sci. B, 54, 1541 (2015). https://doi.org/10.1080/00222348.2015.1103434
- J. Kounavis, C. Hardiman, and B. Scribner, "Emulsil Silica Masterbatch Technology: Compound Design Considerations for Tire Tread Applications", Rubber World, 251, 24 (2015).
- G. Seo, D. I. Kim, S. J. Kim, C. Ryu, J.-K. Yang, and Y.-G. Kang, "Reinforcement of Rubber Properties by Carbon Black and Silica Fillers: A Review", Elast. Compos., 52, 114 (2017).
- A. Blume, "Kinetics of the Silica-Silane Reaction", KGK, 64, 38 (2011).
- Y. Gui, J. Zheng, X. Ye, D. Han, M. Xi, and L. Zhang, "Preparation and Performance of Silica/SBR Masterbatches with High Silica Loading by Latex Compounding Method", Composites Part B, 85, 130 (2016).
- L. Qu, G. Yu, L. Wang, C. Li, G. Zhao, and J. Li, "Effect of Filler-Elastomer Interactions on the Mechanical and Nonlinear Viscoelastic Behaviors of Chemically Modified Silica-Reinforced Solution-Polymerized Styrene Butadiene Rubber", J. Appl. Polym. Sci., 126, 116 (2016).
- B. Ahn, D. Kim, K. Kim, I. J. Kim, H. J. Kim, C. H. Kang, J. Y. Lee, and W. Kim, "Effect of the Functional Group of Silanes on the Modification of Silica Surface and the Physical Properties of Solution Styrene-Butadiene Rubber/Silica Composites", Compos. Interface., 26, 585 (2019). https://doi.org/10.1080/09276440.2018.1514145
- D. Wang, F. Ren, C. Zhu, J. Feng, Q. Cheng, S. Chen, G. Shen, and F. Wang, "Hybrid Silane Technology in Silica-Reinforced Tread Compound", Rubber Chem. Technol., 92, 310 (2019). https://doi.org/10.5254/rct.18.81563
- J. Bertrand and J. Bauer, "NR-Silica-Masterbatches The Easy Processing Way to High Qualiy Compounds", KGK, 1-2, 38 (2018).
- J. Zheng, D. Han, X. Ye, X. Wu, Y. Wu, Y. Wang, and L. Zhang, "Chemical and Physical Interaction between Silane Coupling Agent with Long Arms and Silica and its Effect on Silica/Natural Rubber Composites", Polymer, 135, 200 (2018). https://doi.org/10.1016/j.polymer.2017.12.010
- T. Fukuda, S. Fujii, Y. Nakamaru, and M. Sasaki, "Mechanical Properties of Silica Particle-Filled Styrene-Butadiene Rubber Composites Containing Polysulfide-Type Silane Coupling Agents: Influence of Loading Method of Silane", J. Appl. Polym. Sci., 130, 322 (2013). https://doi.org/10.1002/app.39175
- J.-K. Yang, W. Park, C. Ryu, S. J. Kim, D. Kim, J.-H. Kim, and G. Seo, "Effect of Coupling and Dispersion Agents on the Properties of Styrene-Butadiene Rubber/Butadiene Rubber Compounds Reinforced with Different Silica Contents", Elast. Compos., 53, 109 (2018).
- G. Seo, S. M. Park, K. Ha, K. T. Choi, C. K. Hong, and S. Y. Kaang, "Effectively Reinforcing Roles of the Networked Silica Prepared Using 3,3'-bis(triethoxysilylpropyl)tetrasulfide in the Physical Properties of SBR compounds", J. Mater. Sci., 45, 1897 (2010). https://doi.org/10.1007/s10853-009-4175-3
- C. Ryu, J.-K. Yang, W. Park, Y. Seo, S. J. Kim, D. Kim, S. Park, and G. Seo, "Reinforcement of Styrene-Butadiene/Polybutadiene Rubber Compounds by Modified Silica with Different Surface and Networked States", J. Appl. Polym. Sci., 134, 44893 (2017).
- D. S. Jeong, C. K. Hong, G. T. Lim, and G. Seo, "Networked Silica with Exceptional Reinforcing Performance for SBR Compounds: Interconnected by Methylene Diphenyl Diisocyanate", J. Elastom. Plast., 41, 353 (2009). https://doi.org/10.1177/0095244309103662
- Y. Hoshikawa, B. An, S. Kashihara, T. Ishii, M. Ando, S. Fujisawa, K. Hayakawa, S. Hamatani, H. Yamada, and T. Kyotani, "Analysis of the Interaction between Rubber Polymer and Carbon Black Surfaces by Efficient Removal of Physisorbed Polymer from Carbon-Rubber Composites", Carbon, 99, 148 (2016). https://doi.org/10.1016/j.carbon.2015.12.003
- S. Ghosh, S. K. Goswami, and L. J, Mathias, "Surface Modification of Nano-Silica with Amides and Imides for Use in Polyester Nanocomposites", J. Mater. Chem. A, 19, 6073 (2013).
- Y. W. Ngeow, A. V. Chapman, J. Y. Y. Heng, D. R. Williams, S. Mathys, and C. D. Hull, "Characterization of Silica Modification Modified with Silanes by Using Thermogravimetric Analysis Combined with Infrared Detection", Rubber Chem. Technol., 92, 237 (2019). https://doi.org/10.5254/rct.18.82626
- M. D. L. Castro and L. E. G. Ayuso, "Soxhlet Extraction" in "Reference Module in Chemistry, Molecular Sciences and Chemical Engineering", ed. J. Reedijk, p. 2701, Elsevier, Amsterdam, 2018.
- A. K. Sircar, "Analysis of Elastomer Vulcanizate Composition by TG-DTG Techniques", Rubber Chem. Technol., 65, 503 (1992). https://doi.org/10.5254/1.3538627
- H. Yan, K. Sun, Y. Zhang, Y. Zang, and Y. Fan, "Effect of Silane Coupling Agents on the Vulcaniation Characteristics of Natural Rubber", J. Appl. Polym. Sci., 94, 1511 (2004). https://doi.org/10.1002/app.21071
- J.-K. Yang, W. Park, C. Ryu, S. J. Kim, D. I. Kim, G. Seo, J.-H. Kim, and C.-B. Chung, "Estimation of Silica Flocculation in SBR/BR Compounds Reinforced with Different Silica Contents from Their Rheocurves", J. Appl. Polym. Sci., (2019) https://doi.org/10.1002/app.48559.
- M. Castellano, L. Conzatti, G. Costa, L. Falqui, A. Turturro, B. Valenti, and F. Negroni, "Surface Modification of Silica: 1. Thermodynamic Aspects and Effect on Elastomer Reinforcement", Polymer, 46, 695 (2005). https://doi.org/10.1016/j.polymer.2004.11.010
- J.-K Yang, W. Park, C. Ryu, S. J. Kim, D. Kim, G. Seo, J.-H. Kim, and C.-B. Chung, "Roles of Sulfur and Accelerators in the Vulcanization of SBR Compounds Deduced Through Simulation", Rubber Chem. Technol., 91, 595 (2018). https://doi.org/10.5254/rct.18.82615
- P. Zhang, M. Morris, and D. Doshi, "Materials Development for Lowering Rolling Resistance of Tires", Rubber Chem. Technol., 89, 79 (2016). https://doi.org/10.5254/rct.16.83805
- M.-J. Wang and Y. Kutsovsky, "Effect of Fillers on Wet Skid Resistance of Tires. Part I.: Water Lubrication vs. Filler-Elastomer Interactions", Rubber Chem. Technol., 81, 552 (2008). https://doi.org/10.5254/1.3548220