Super Strong and Tough Elastomers Enabled by Sacrificial Segregated Network

Yong Zhu; Lai-Yun Wei; Xuan Fu; Jun-Qi Zhang; Ling-Min Kong; Guang-Su Huang; Jin-Rong Wu

doi:10.1007/s10118-020-2484-9

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Super Strong and Tough Elastomers Enabled by Sacrificial Segregated Network

ARTICLE | Updated：2020-09-21

- Super Strong and Tough Elastomers Enabled by Sacrificial Segregated Network
- Chinese Journal of Polymer Science Vol. 39, Issue 3, Pages: 377-386(2021)
- Affiliations：
  
  State Key Laboratory of Polymer Materials Engineering, College of Polymer Science and Engineering, Sichuan University, Chengdu 610065, China
- Author bio：
  
  guangsu-huang@hotmail.com (G.S.H.)
  wujinrong@scu.edu.cn (J.R.W.)
- Funds：
- DOI：10.1007/s10118-020-2484-9
  CLC：
- Received：24 June 2020，
  
  Revised：2020-7-13，
  
  Accepted：23 July 2020，
  
  Online First：21 September 2020，
  
  Published：02 January 2021
- Accepted：
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Zhu, Y.; Wei, L. Y.; Fu, X.; Zhang, J. Q.; Kong, L. M.; Huang, G. S.; Wu, J. R. Super strong and tough elastomers enabled by sacrificial segregated network. Chinese J. Polym. Sci. 2021, 39, 377–386

Yong Zhu, Lai-Yun Wei, Xuan Fu, et al. Super Strong and Tough Elastomers Enabled by Sacrificial Segregated Network[J]. Chinese Journal of Polymer Science, 2021, 39(3): 377-386.
Zhu, Y.; Wei, L. Y.; Fu, X.; Zhang, J. Q.; Kong, L. M.; Huang, G. S.; Wu, J. R. Super strong and tough elastomers enabled by sacrificial segregated network. Chinese J. Polym. Sci. 2021, 39, 377–386 DOI： 10.1007/s10118-020-2484-9.

Yong Zhu, Lai-Yun Wei, Xuan Fu, et al. Super Strong and Tough Elastomers Enabled by Sacrificial Segregated Network[J]. Chinese Journal of Polymer Science, 2021, 39(3): 377-386. DOI： 10.1007/s10118-020-2484-9.

摘要

Abstract

The integration of high strength and toughness concurrently is a vital requirement for elastomers from the perspective of long-term durability and reliability. Unfortunately

these properties are generally conflicting in artificial materials. In the present work

we propose a facile strategy to simultaneously toughen and strengthen elastomers by constructing 3D segregated filler network

via

a simple latex mixing method. The as-fabricated elastomers are featured by a microscopic 3D interconnected segregated network of rigid graphene oxide (GO) nanosheets and a continuous soft matrix of sulfur vulcanized natural rubber (NR). We demonstrate that the interconnected segregated filler network ruptures preferentially upon deformation

and thus is more efficient in energy dissipation than the dispersed filler network. Therefore

the segregated filler network exhibits better reinforcing effects for the rubber matrix. Moreover

the excellent energy dissipating ability also contributes to the outstanding crack growth resistance through the release of concentrated stress at the crack tip. As a result

the strength

toughness and fatigue resistance of the nanocomposites are concurrently enhanced. The methodology in this work is facile and universally applicable

which may provide new insights into the design of elastomers with both extraordinary static and dynamic mechanical performance for practical applications.

关键词

Keywords

references

Singha, N. K.; Bhattacharjee, S.; Sivaram, S. . Hydrogenation of diene elastomers, their properties and applications: a critical review . Rubber Chem. Technol. , 1997 . 70 309 - 367 . DOI: 10.5254/1.3538435 http://doi.org/10.5254/1.3538435 .

Huang, J.; Tang, Z.; Yang, Z.; Guo, B. . Bioinspired interface engineering in elastomer/graphene composites by constructing sacrificial metal-ligand bonds . Macromol. Rapid Commun. , 2016 . 37 1040 - 1045 . DOI: 10.1002/marc.201600226 http://doi.org/10.1002/marc.201600226 .

Molinari, N.; Sutton, A.; Stevens, J.; Mostofi, A. In An atomistic model for cross-linked HNBR elastomers used in seals , APS March Meeting, 2015 .

Lei, W.; Zhou, X.; Russell, T. P.; Hua, K. C.; Yang, X.; Qiao, H.; Wang, W.; Li, F.; Wang, R.; Zhang, L. . High performance bio-based elastomers: energy efficient, sustainable materials for tires . J. Mater. Chem. A , 2016 . 10 1039 .

Gong, J. P. . Materials both tough and soft . Science , 2014 . 344 161 DOI: 10.1126/science.1252389 http://doi.org/10.1126/science.1252389 .

Zhao, X. . Designing toughness and strength for soft materials . Proc. Natl. Acad. Sci. USA , 2017 . 114 8138 - 8140 . DOI: 10.1073/pnas.1710942114 http://doi.org/10.1073/pnas.1710942114 .

Bai, R.; Yang, Q.; Tang, J.; Morelle, X. P.; Vlassak, J.; Suo, Z. . Fatigue fracture of tough hydrogels . Extreme Mech. Lett. , 2017 . 15 91 - 96 . DOI: 10.1016/j.eml.2017.07.002 http://doi.org/10.1016/j.eml.2017.07.002 .

Keten, S.; Xu, Z.; Ihle, B.; Buehler, M. J. . Nanoconfinement controls stiffness, strength and mechanical toughness of β -sheet crystals in silk . Nat. Mater. , 2010 . 9 359 DOI: 10.1038/nmat2704 http://doi.org/10.1038/nmat2704 .

Luo, M. C.; Zeng, J.; Fu, X.; Huang, G.; Wu, J. . Toughening diene elastomers by strong hydrogen bond interactions . Polymer , 2016 . 106 21 - 28 . DOI: 10.1016/j.polymer.2016.10.056 http://doi.org/10.1016/j.polymer.2016.10.056 .

Liu, J.; Tan, C. S. Y.; Yu, Z.; Lan, Y.; Abell, C.; Scherman, O. A. . Biomimetic supramolecular polymer networks exhibiting both toughness and self-recovery . Adv. Mater. , 2017 . 29 1604951 DOI: 10.1002/adma.201604951 http://doi.org/10.1002/adma.201604951 .

Nakahata, M.; Takashima, Y.; Harada, A. . Highly flexible, tough, and self-healing supramolecular polymeric materials using host-guest interaction . Macromol. Rapid Commun. , 2016 . 37 86 - 92 . DOI: 10.1002/marc.201500473 http://doi.org/10.1002/marc.201500473 .

Xu, Z. . Mechanics of metal-catecholate complexes: the roles of coordination state and metal types . Sci. Rep. , 2013 . 3 2914 DOI: 10.1038/srep02914 http://doi.org/10.1038/srep02914 .

Zheng, S. Y.; Ding, H.; Qian, J.; Yin, J.; Wu, Z. L.; Song, Y.; Zheng, Q. . Metal-coordination complexes mediated physical hydrogels with high toughness, stick-slip tearing behavior, and good processability . Macromolecules , 2016 . 49 9637 - 9646 . DOI: 10.1021/acs.macromol.6b02150 http://doi.org/10.1021/acs.macromol.6b02150 .

Filippidi, E.; Cristiani, T. R.; Eisenbach, C. D.; Waite, J. H.; Israelachvili, J. N.; Ahn, B. K.; Valentine, M. T. . Toughening elastomers using mussel-inspired iron-catechol complexes . Science , 2017 . 358 502 DOI: 10.1126/science.aao0350 http://doi.org/10.1126/science.aao0350 .

Liu, J.; Wang, S.; Tang, Z.; Huang, J.; Guo, B.; Huang, G. . Bioinspired engineering of two different types of sacrificial bonds into chemically cross-linked cis -1,4-polyisoprene toward a high-performance elastomer . Macromolecules , 2016 . 49 8593 - 8604 . DOI: 10.1021/acs.macromol.6b01576 http://doi.org/10.1021/acs.macromol.6b01576 .

Zhou, X.; Guo, B.; Zhang, L.; Hu, G. H. . Progress in bio-inspired sacrificial bonds in artificial polymeric materials . Chem. Soc. Rev. , 2017 . 46 6301 - 6329 . DOI: 10.1039/C7CS00276A http://doi.org/10.1039/C7CS00276A .

Haque, M. A.; Kurokawa, T.; Kamita, G.; Gong, J. P. . Lamellar bilayers as reversible sacrificial bonds to toughen hydrogel: hysteresis, self-recovery, fatigue resistance, and crack blunting . Macromolecules , 2011 . 44 8916 - 8924 . DOI: 10.1021/ma201653t http://doi.org/10.1021/ma201653t .

Zhu, B.; Jasinski, N.; Benitez, A.; Noack, M.; Park, D.; Goldmann, A. S.; Barner-Kowollik, C.; Walther, A. . Hierarchical nacre mimetics with synergistic mechanical properties by control of molecular interactions in self-healing polymers . Angew. Chem. Int. Ed. , 2015 . 54 8653 - 8657 . DOI: 10.1002/anie.201502323 http://doi.org/10.1002/anie.201502323 .

Van Meerbeek, I. M.; Mac Murray, B. C.; Kim, J. W.; Robinson, S. S.; Zou, P. X.; Silberstein, M. N.; Shepherd, R. F. . Morphing metal and elastomer bicontinuous foams for reversible stiffness, shape memory, and self-healing soft machines . Adv. Mater. , 2016 . 28 2801 - 2806 . DOI: 10.1002/adma.201505991 http://doi.org/10.1002/adma.201505991 .

Takahashi, R.; Sun, T. L.; Saruwatari, Y.; Kurokawa, T.; King, D. R.; Gong, J. P. . Creating stiff, tough, and functional hydrogel composites with low-melting-point alloys . Adv. Mater. , 2018 . 30 1706885 DOI: 10.1002/adma.201706885 http://doi.org/10.1002/adma.201706885 .

Wu, X.; Han, Y.; Zhang, X.; Lu, C. . Highly sensitive, stretchable, and wash-durable strain sensor based on ultrathin conductive layer@polyurethane yarn for tiny motion monitoring . ACS Appl. Mater. Interfaces , 2016 . 8 9936 - 9945 . DOI: 10.1021/acsami.6b01174 http://doi.org/10.1021/acsami.6b01174 .

Li, C.; Yang, Z.; Tang, Z.; Guo, B.; Tian, M.; Zhang, L. . A scalable strategy for constructing three-dimensional segregated graphene network in polymer via hydrothermal self-assembly . Chem. Eng. J. , 2019 . 363 300 - 308 . DOI: 10.1016/j.cej.2019.01.142 http://doi.org/10.1016/j.cej.2019.01.142 .

Gong, T.; Peng, S. P.; Bao, R. Y.; Yang, W.; Xie, B. H.; Yang, M. B. . Low percolation threshold and balanced electrical and mechanical performances in polypropylene/carbon black composites with a continuous segregated structure . Compos. Part B , 2016 . 99 348 - 357 . DOI: 10.1016/j.compositesb.2016.06.031 http://doi.org/10.1016/j.compositesb.2016.06.031 .

Liu, Y. F.; Feng, L. M.; Chen, Y. F.; Shi, Y. D.; Chen, X. D.; Wang, M. . Segregated polypropylene/cross-linked poly(ethylene- co -1-octene)/multi-walled carbon nanotube nanocomposites with low percolation threshold and dominated negative temperature coefficient effect: towards electromagnetic interference shielding and thermistors . Compos. Sci. Technol. , 2018 . 159 152 - 161 . DOI: 10.1016/j.compscitech.2018.02.041 http://doi.org/10.1016/j.compscitech.2018.02.041 .

Lin, Y.; Dong, X.; Liu, S.; Chen, S.; Wei, Y.; Liu, L. . Graphene-elastomer composites with segregated nanostructured network for liquid and strain sensing application . ACS Appl. Mater. Interfaces , 2016 . 8 24143 - 24151 . DOI: 10.1021/acsami.6b08587 http://doi.org/10.1021/acsami.6b08587 .

Zhao, S.; Lou, D.; Li, G.; Zheng, Y.; Zheng, G.; Dai, K.; Liu, C.; Jiang, Y.; Shen, C. . Bridging the segregated structure in conductive polypropylene composites: an effective strategy to balance the sensitivity and stability of strain sensing performances . Compos. Sci. Technol. , 2018 . 163 18 - 25 . DOI: 10.1016/j.compscitech.2018.05.006 http://doi.org/10.1016/j.compscitech.2018.05.006 .

Cao, J.; Lu, C.; Zhuang, J.; Liu, M.; Zhang, X.; Yu, Y.; Tao, Q. . Multiple hydrogen bonding enables the self-healing of sensors for human–machine interactions . Angew. Chem. Int. Ed. , 2017 . 56 8795 - 8800 . DOI: 10.1002/anie.201704217 http://doi.org/10.1002/anie.201704217 .

Liu, J.; Zhao, F.; Tao, Q.; Cao, J.; Yu, Y.; Zhang, X. Visualized simulation for the nanostructure design of flexible strain sensors: from a numerical model to experimental verification. Mater . Horiz . 2019 , 6 , 1892−1898.

George, N.; C.S, J. C.; Mathiazhagan, A.; Joseph, R. . High performance natural rubber composites with conductive segregated network of multiwalled carbon nanotubes . Compos. Sci. Technol. , 2015 . 116 33 - 40 . DOI: 10.1016/j.compscitech.2015.05.008 http://doi.org/10.1016/j.compscitech.2015.05.008 .

Du, J.; Long, Z.; You, Z.; Zhang, L.; Feng, L.; Liu, P.; Chang, L. . Comparison of electrical properties between multi-walled carbon nanotube and graphene nanosheet/high density polyethylene composites with a segregated network structure . Carbon , 2011 . 49 1094 - 1100 . DOI: 10.1016/j.carbon.2010.11.013 http://doi.org/10.1016/j.carbon.2010.11.013 .

Zhan, Y. H.; Wang, J.; Zhang, K. Y.; Li, Y. C.; Meng, Y. Y.; Yan, N.; Wei, W. K.; Peng, F. B.; Xia, H. S. . Fabrication of a flexible electromagnetic interference shielding Fe 3 O 4 @reduced graphene oxide/natural rubber composite with segregated network . Chem. Eng. J. , 2018 . 344 184 - 193 . DOI: 10.1016/j.cej.2018.03.085 http://doi.org/10.1016/j.cej.2018.03.085 .

Zhan, Y.; Lavorgna, M.; Buonocore, G.; Xia, H. . Enhancing electrical conductivity of rubber composites by constructing interconnected network of self-assembled graphene with latex mixing . J. Mater. Chem. , 2012 . 22 10464 - 10468 . DOI: 10.1039/c2jm31293j http://doi.org/10.1039/c2jm31293j .

Li, H.; Yang, L.; Weng, G.; Xing, W.; Wu, J.; Huang, G. . Toughening rubbers with a hybrid filler network of graphene and carbon nanotubes . J. Mater. Chem. A , 2015 . 3 22385 - 22392 . DOI: 10.1039/C5TA05836H http://doi.org/10.1039/C5TA05836H .

Sliozberg, Y. R.; Hoy, R. S.; Mrozek, R. A.; Lenhart, J. L.; Andzelm, J. W. . Role of entanglements and bond scission in high strain-rate deformation of polymer gels . Polymer , 2014 . 55 2543 - 2551 . DOI: 10.1016/j.polymer.2014.03.051 http://doi.org/10.1016/j.polymer.2014.03.051 .

Creton, C.; Ciccotti, M. . Fracture and adhesion of soft materials: a review . Rep. Prog. Phys. , 2016 . 79 046601 DOI: 10.1088/0034-4885/79/4/046601 http://doi.org/10.1088/0034-4885/79/4/046601 .

Kazem, N.; Bartlett, M. D.; Majidi, C. . Extreme toughening of soft materials with liquid metal . Adv. Mater. , 2018 . 30 1706594 DOI: 10.1002/adma.201706594 http://doi.org/10.1002/adma.201706594 .

Bueche, F.; Harding, S. W. . A new absolute molecular weight method for linear polymers . J. Polym. Sci. , 1958 . 32 177 - 186 . DOI: 10.1002/pol.1958.1203212414 http://doi.org/10.1002/pol.1958.1203212414 .

Zhu, Y.; Shen, Q.; Wei, L.; Fu, X.; Huang, C.; Zhu, Y.; Zhao, L.; Huang, G.; Wu, J. . Ultra-tough, strong, and defect-tolerant elastomers with self-healing and intelligent-responsive abilities . ACS Appl. Mater. Interfaces , 2019 . 11 29373 - 29381 . DOI: 10.1021/acsami.9b11041 http://doi.org/10.1021/acsami.9b11041 .

Gong, J. P. . Why are double network hydrogels so tough? . Soft Matter , 2010 . 6 2583 - 2590 . DOI: 10.1039/b924290b http://doi.org/10.1039/b924290b .

de Gennes, P. G. . Soft adhesives . Langmuir , 1996 . 12 4497 - 4500 . DOI: 10.1021/la950886y http://doi.org/10.1021/la950886y .

Brown, H. R. . Effects of chain pull-out on adhesion of elastomers . Macromolecules , 1993 . 26 1666 - 1670 . DOI: 10.1021/ma00059a027 http://doi.org/10.1021/ma00059a027 .

Sun, J. Y.; Zhao, X.; Illeperuma, W. R. K.; Chaudhuri, O.; Oh, K. H.; Mooney, D. J.; Vlassak, J. J.; Suo, Z. . Highly stretchable and tough hydrogels . Nature , 2012 . 489 133 DOI: 10.1038/nature11409 http://doi.org/10.1038/nature11409 .

Tanaka, Y.; Kuwabara, R.; Na, Y. H.; Kurokawa, T.; Gong, J. P.; Osada, Y. . Determination of fracture energy of high strength double network hydrogels . J. Phys. Chem. B , 2005 . 109 11559 - 11562 . DOI: 10.1021/jp0500790 http://doi.org/10.1021/jp0500790 .

Webber, R. E.; Creton, C.; Brown, H. R.; Gong, J. P. . Large strain hysteresis and mullins effect of tough double-network hydrogels . Macromolecules , 2007 . 40 2919 - 2927 . DOI: 10.1021/ma062924y http://doi.org/10.1021/ma062924y .

Carretero-González, J.; Retsos, H.; Verdejo, R.; Toki, S.; Hsiao, B. S.; Giannelis, E. P.; López-Manchado, M. A. . Effect of nanoclay on natural rubber microstructure . Macromolecules , 2008 . 41 6763 - 6772 . DOI: 10.1021/ma800893x http://doi.org/10.1021/ma800893x .

Tang, M.; Xing, W.; Wu, J.; Huang, G.; Xiang, K.; Guo, L.; Li, G. . Graphene as a prominent antioxidant for diolefin elastomers . J. Mater. Chem. A , 2015 . 3 5942 - 5948 . DOI: 10.1039/C4TA06991A http://doi.org/10.1039/C4TA06991A .

Wu, J.; Huang, G.; Li, H.; Wu, S.; Liu, Y.; Zheng, J. . Enhanced mechanical and gas barrier properties of rubber nanocomposites with surface functionalized graphene oxide at low content . Polymer , 2013 . 54 1930 - 1937 . DOI: 10.1016/j.polymer.2013.01.049 http://doi.org/10.1016/j.polymer.2013.01.049 .

Martin, C. A.; Sandler, J. K. W.; Shaffer, M. S. P.; Schwarz, M. K.; Bauhofer, W.; Schulte, K.; Windle, A. H. . Formation of percolating networks in multi-wall carbon-nanotube-epoxy composites . Compos. Sci. Technol. , 2004 . 64 2309 - 2316 . DOI: 10.1016/j.compscitech.2004.01.025 http://doi.org/10.1016/j.compscitech.2004.01.025 .

Bhattacharyya, S.; Sinturel, C.; Bahloul, O.; Saboungi, M. L.; Thomas, S.; Salvetat, J. P. . Improving reinforcement of natural rubber by networking of activated carbon nanotubes . Carbon , 2008 . 46 1037 - 1045 . DOI: 10.1016/j.carbon.2008.03.011 http://doi.org/10.1016/j.carbon.2008.03.011 .

Lu, Y. L.; Li, Z.; Yu, Z. Z.; Tian, M.; Zhang, L. Q.; Mai, Y. W. . Microstructure and properties of highly filled rubber/clay nanocomposites prepared by melt blending . Compos. Sci. Technol. , 2007 . 67 2903 - 2913 . DOI: 10.1016/j.compscitech.2007.05.018 http://doi.org/10.1016/j.compscitech.2007.05.018 .

Vadukumpully, S.; Paul, J.; Mahanta, N.; Valiyaveettil, S. . Flexible conductive graphene/poly(vinyl chloride) composite thin films with high mechanical strength and thermal stability . Carbon , 2011 . 49 198 - 205 . DOI: 10.1016/j.carbon.2010.09.004 http://doi.org/10.1016/j.carbon.2010.09.004 .

Wu, J.; Cai, L. H.; Weitz, D. A. . Tough self-healing elastomers by molecular enforced integration of covalent and reversible networks . Adv. Mater. , 2017 . 29 1702616 DOI: 10.1002/adma.201702616 http://doi.org/10.1002/adma.201702616 .

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