Evaluation of fracture toughness of epoxy polymer composite incorporating micro/nano silica, rubber and CNTs

Cozza, Ronaldo Câmara; Verma, Vikas

doi:10.1590/0104-1428.05720

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REVIEW ARTICLE • Polímeros 30 (3) • 2020 • https://doi.org/10.1590/0104-1428.05720 copy

Evaluation of fracture toughness of epoxy polymer composite incorporating micro/nano silica, rubber and CNTs

Authorship SCIMAGO INSTITUTIONS RANKINGS

Abstract

In engineering applications, fracture toughness is an essential requirement that determines the life of a material. Epoxy polymers are widely used in fibre-reinforced composite materials. Due to their structural efficiency and durability, the use of adhesive and composite materials based on epoxy polymers is widespread in aerospace and automobile industries. In this paper fracture toughness of hybrid epoxy polymer composite with addition of nano/micro figures of silica, rubber and carbon nano tubes (CNTs) is evaluated. It is observed that silica addition promoted nano toughening effect with plastically deformation capability in epoxies. Rubber and multi walled CNTs increased the toughness with negligible reduction in stiffness in epoxies. Future research emphasis can be laid on crucial understanding of stress transfer mechanisms and interfacial bond strength between nano particles – epoxy system and on nanofillers modified epoxies as matrices or interleafs for carbon or glass fiber composites to increase the interlaminar delamination toughness.

Keywords:
CNT; epoxy; rubber; silica

Type of Epoxy Polymers	Modifier SiO₂ size (nm)	SiO₂ Addition	Fracture toughness (MPa.m^1/2)	Fracture energy (J/m²)	Curing Agent	Ref.
DGEBA	–	0-20 wt.%	1.45 ± 0.12, highest for polyether DGEBA at 0.138 volume fraction silica	616 ± 109, highest for polyether DGEBA at 0.138 volume fraction silica	Accelerated methylhexahy drophthalic acid anhydride	Hsieh et al.^[¹1 Hsieh, T. H., Kinloch, A. J., Masania, K., Taylor, A. C., & Sprenger, S. (2010). The mechanisms and mechanics of the toughening of epoxy polymers modified with silica nanoparticles. Polymer, 51(26), 6284-6294. http://dx.doi.org/10.1016/j.polymer.2010.10.048. http://dx.doi.org/10.1016/j.polymer.2010... ^]
DGEBA/F
Polyether DGEBA
TGMDA
DGEBA	Unmodified	30 vol.%	1.11 ± 0.06	303 ± 14	Piperidine	Dittanet and Pearson^[⁸8 Dittanet, P., & Pearson, R. A. (2012). Effect of silica nanoparticle size on toughening mechanisms of filled epoxy. Polymer, 53(9), 1890-1905. http://dx.doi.org/10.1016/j.polymer.2012.02.052. http://dx.doi.org/10.1016/j.polymer.2012... ^]
	23		2.52 ± 0.11	973 ± 17
	74		2.89 ± 0.11	1264 ± 14
	170		2.65 ± 0.06	1030 ± 08
DGEBA	Neat resin	10 vol.%	1.07 ± 0.1	280 ± 20	5phr piperidine	Dittanet and Pearson^[⁹9 Dittanet, P., & Pearson, R. A. (2013). Effect of bimodal particle size distributions on the toughening mechanisms in silica nanoparticle filled epoxy resin. Polymer, 54(7), 1832-1845. http://dx.doi.org/10.1016/j.polymer.2012.12.059. http://dx.doi.org/10.1016/j.polymer.2012... ^]
	42 μm ⁺		1.96 ± 0.15	760 ±10
	23 nm		1.96 ± 0.15	760 ±10
	42 μm ⁺		1.93 ± 0.12	740 ± 80
	74 nm		1.93 ± 0.12	740 ± 80
	42 μm ⁺		1.94 ± 0.15	750 ± 10
	170 nm		1.94 ± 0.15	750 ± 10
DGEBA	20 nm	13 vol.%	0.59-1.42	100-460	Methylhexahydrophthalic acid anhydride (HE600)	Johnsen et al.^[¹⁰10 Johnsen, B. B., Kinloch, A. J., Mohammed, R. D., Taylor, A. C., & Sprenger, S. (2007). Toughening mechanisms of nanoparticle-modified epoxy polymers. Polymer, 48(2), 530-541. http://dx.doi.org/10.1016/j.polymer.2006.11.038. http://dx.doi.org/10.1016/j.polymer.2006... ^]
DGEBF	90 nm	0-7%	Increase in strain rate	–	Poly(propyleneglycol)-diglycidyl ether (PPGDE)	Guo and Li^[³⁰30 Guo, Y., & Li, Y. (2007). Quasi-static/dynamic response of SiO2-epoxy nanocomposites. Materials Science and Engineering A, 458(1-2), 330-335. http://dx.doi.org/10.1016/j.msea.2007.02.011. http://dx.doi.org/10.1016/j.msea.2007.02... ^]

Type of Epoxy	Modifier rubber	Rubber Addition (phr)	Fracture toughness (MPa.m^1/2)	Curing Agent	Ref.
DGEBA	Amine terminated butadiene acrylonitrile rubber (ATBN)	5-20	0.91 to 1.49	Polyaminoimidazoline	Chikhi et al.^[³¹31 Chikhi, N., Fellahi, S., & Bakar, M. (2002). Modification of epoxy resin using reactive liquid (ATBN) rubber. European Polymer Journal, 38(2), 251-264. http://dx.doi.org/10.1016/S0014-3057(01)00194-X. http://dx.doi.org/10.1016/S0014-3057(01)... ^]
DGEBF	Carboxylic nitrile-butadiene nano	15	48.3% increment at 77K	Diethyl toluene diamine (DETD)	Zhao et al.^[³²32 Zhao, Y., Chen, Z.-K., Liu, Y., Xiao, H.-M., Feng, Q.-P., & Fu, S.-Y. (2013). Simultaneously enhanced cryogenic tensile strength and fracture toughness of epoxy resins by carboxylic nitrile-butadiene nano-rubber. Composites. Part A, Applied Science and Manufacturing, 55, 178-187. http://dx.doi.org/10.1016/j.compositesa.2013.09.005. http://dx.doi.org/10.1016/j.compositesa.... ^]
DGEBA	(M22N, M52N, M52)^* * Poly(methyl methacrylate)-bloc-poly(butylacrylate)-bloc-poly(methyl methacrylate) (PMMA–b-PbuA–b-PMMA) BCPs (M22N, M52 and M52N).	12 wt.%	1.22	Methylhexahydrophthalic acid anhydride	Chen and Taylor^[³³33 Chen, J., & Taylor, A. C. (2012). Epoxy modified with triblock copolymers: morphology, mechanical properties and fracture mechanisms. Journal of Materials Science, 47(11), 4546-4560. http://dx.doi.org/10.1007/s10853-012-6313-6. http://dx.doi.org/10.1007/s10853-012-631... ^]
DGEBA	Epoxy terminated butadiene acrylonitrile (ETBN) & ATBN	0-15	1-1.65	Trimethylene glycol di-p-aminobenzoate (TMAB)	Hwang et al.^[⁴⁷47 Hwang, J.-F., Manson, J. A., Hertzberg, R. W., Miller, G. A., & Sperling, L. H. (1989). Structure-property relationships in rubber-toughened epoxies. Polymer Engineering and Science, 29(20), 1466-1476. http://dx.doi.org/10.1002/pen.760292008. http://dx.doi.org/10.1002/pen.760292008... ^]
DGEBA	Hydroxyl terminated polybutadiene liquid rubber (HTPB)	0-20	1.5	Cyclic anhydride (Hy906)	Thomas et al.^[⁵¹51 Thomas, R., Yumei, D., Yuelong, H., Le, Y., Moldenaers, P., Weimin, Y., Czigany, T., & Thomas, S. (2008). Miscibility, morphology, thermal, and mechanical properties of a DGEBA based epoxy resin toughened with a liquid rubber. Polymer, 49(1), 278-294. http://dx.doi.org/10.1016/j.polymer.2007.11.030. http://dx.doi.org/10.1016/j.polymer.2007... ^]

Type of Epoxy	Name of the modifier element	Size diameter (nm)	Size length (µm)	Addition content (wt.%)	Fracture Toughness (MPa.m^1/2)	Fracture Energy (J/m²)	Curing agent	Ref.
DGEBF	–	–	–	–	1.619 ± 0.14	–	Polyamine HA-11	Ayatollahi et al.^[⁵³53 Ayatollahi, M. R., Shadlou, S., & Shokrieh, M. M. (2011). Fracture toughness of epoxy/multi-walled carbon nanotube nano-composites under bending and shear loading conditions. Materials & Design, 32(4), 2115-2124. http://dx.doi.org/10.1016/j.matdes.2010.11.034. http://dx.doi.org/10.1016/j.matdes.2010.... ^]
	MWCNT	30 & 40	10 & 30	0.1	1.865 ± 0.07
				0.5	2.045 ± 0.1
				1	1.93 ± 0.19
DGEBA	MWCNT	120	140	0.5	0.69 to 0.98	133 to 233	HE 600 anhydride	Hsieh et al.^[⁵⁴54 Hsieh, T. H., Kinloch, A. J., Taylor, A. C., & Kinloch, I. A. (2011). The effect of carbon nanotubes on the fracture toughness and fatigue performance of a thermosetting epoxy polymer. Journal of Materials Science, 46(23), 7525-7535. http://dx.doi.org/10.1007/s10853-011-5724-0. http://dx.doi.org/10.1007/s10853-011-572... ^]
LY 564	MWCNT	10 to 15	> 500 nm	0.5-1	2.5	1200	–	Gkikas et al.^[⁵⁵55 Gkikas, G., Barkoula, N.-M., & Paipetis, A. S. (2012). Effect of dispersion conditions on the thermo-mechanical and toughness properties of multi walled carbon nanotubes-reinforced epoxy. Composites. Part B, Engineering, 43(6), 2697-2705. http://dx.doi.org/10.1016/j.compositesb.2012.01.070. http://dx.doi.org/10.1016/j.compositesb.... ^]
DGEBA	–	–	–	–	0.65 ± 0.062	–	Amine hardener H137i	Gojny et al.^[⁸⁵85 Gojny, F., Wichmann, M., Fiedler, B., & Schulte, K. (2005). Influence of different carbon nanotubes on the mechanical properties of epoxy matrix composites – A comparative study. Composites Science and Technology, 65(15-16), 2300-2313. http://dx.doi.org/10.1016/j.compscitech.2005.04.021. http://dx.doi.org/10.1016/j.compscitech.... ^]
	(SW/DW/MW)CNT	–	–	0.3-0.5	0.72 ± 0.014 –	–
	(SW/DW/MW)CNT	–	–	0.3-0.5	0.79 ± 0.048	–
Epoxy 862	–	–	–	–	0.56 ± 0.03	–	Epicure W	Sun et al.^[⁸⁶86 Sun, L., Warren, G. L., O’Reilly, J. Y., Everett, W. N., Lee, S. M., Davis, D., Lagoudas, D., & Sue, H.-J. (2008). Mechanical properties of surface-functionalized SWCNT/epoxy composites. Carbon, 46(2), 320-328. http://dx.doi.org/10.1016/j.carbon.2007.11.051. http://dx.doi.org/10.1016/j.carbon.2007.... ^]
Epoxy 862	^* * p and f-MWCNTs were used to signify the pristine and ozone-functionalized MWCNTs. f-SWCNT	–	–	1	0.66 ± 0.04	–	Epicure W
DGEBA	–	–	–	–	0.46 ± 0.04	64	4methylhexahydrophtahlic anhydride (MHHPA) HE600	Tang et al.^[⁸⁷87 Tang, L., Zhang, H., Han, J., Wu, X., & Zhang, Z. (2011). Fracture mechanisms of epoxy filled with ozone functionalized multi-wall carbon nanotubes. Composites, 72(1), 7-13. http://dx.doi.org/10.1016/j.compscitech.2011.07.016. http://dx.doi.org/10.1016/j.compscitech.... ^]
	*p-MWCNT	~ 15	1-10	0.5-1	0.59 ± 0.05	110, 108
	*p-MWCNT	~ 15	1-10	0.5-1	0.60 ± 0.08	110, 108
	*f-MWCNT	~ 15	1-10	0.5-1	0.64 ± 0.07	135, 145
	*f-MWCNT	~ 15	1-10	0.5-1	0.70 ± 0.06	135, 145

Type of Fiber	Name of the modifier element	% of content addition (wt.%)	% ofK_IC, MPa.m^1/2increment	% ofG_IC, J/m²increment	Ref.
High silica glass fiber	Woven Satin textile fiber	t = 0.26 mm	7.431 [0°]	–	Gouda et al.^[⁴4 Gouda, P. S. S., Kodancha, K. G., Siddaramaiah & Jawali, D. (2013). Experimental and numerical investigations on fracture behavior of high silica glass/satin textile fiber reinforced hybrid polymer composites. Advanced Materials Letters, 4(11), 827-835. http://dx.doi.org/10.5185/amlett.2013.3450. http://dx.doi.org/10.5185/amlett.2013.34... ^]
High silica glass fiber	Woven Satin textile fiber	t = 0.26 mm	4.199 [90°]	–
^* * Glass fibre reinforced-polymer (GFRP) and carbon-fibre reinforced-polymer (CFRP). GFRP	–	–	–	190	Tsai et al.^[⁸⁸88 Tsai, J.-L., Huang, B.-H., & Cheng, Y.-L. (2009). Enhancing fracture toughness of glass/epoxy composites by using rubber particles together with silica nanoparticles. Journal of Composite Materials, 43(25), 3107-3123. http://dx.doi.org/10.1177/0021998309345299. http://dx.doi.org/10.1177/00219983093452... ^]
	SiO₂-CTBN	10 wt.% each	–	930
	SiO₂-CSR	10 wt.% each	–	1030 (390%)
GFRP	Rubber (µm) – SiO₂ (nm)	9 wt.%, 15 wt.%	–	965	Hsieh et al.^[⁸⁹89 Hsieh, T. H., Kinloch, A. J., Masania, K., Sohn Lee, J., Taylor, A. C., & Sprenger, S. (2010). The toughness of epoxy polymers and fibre composites modified with rubber microparticles and silica nanoparticles. Journal of Materials Science, 45(5), 1193-1210. http://dx.doi.org/10.1007/s10853-009-4064-9. http://dx.doi.org/10.1007/s10853-009-406... ^]
GFRP	Carbon	0/90	34.07 (Across)	–	Gouda et al.^[⁹⁰90 Gouda, P. S. S., Kudari, S. K., Prabhuswamy, S., & Jawali, D. (2011). Fracture toughness of glass-carbon (0/90)s fiber reinforced polymer composite-an experimental and numerical study. Journal of Materials and Materials Characterization & Engineering, 10, 671-682.^]
GFRP	Carbon	0/90	32.84 (Along)	–
*CFRP	MWCNT	0.1	–	200-300	Karapappas et al.^[⁹¹91 Karapappas, P., Vavouliotis, A., Tsotra, P., Kostopoulos, V., & Paipetis, A. (2009). Enhanced fracture properties of carbon reinforced composites by the addition of multi-wall carbon nanotubes. Journal of Composite Materials, 43(9), 977-985. http://dx.doi.org/10.1177/0021998308097735. http://dx.doi.org/10.1177/00219983080977... ^]
		0.5	–	400-500
		1	–	400-600
CFRP	MWCNT	–	–	943 (442%)	Borowski et al.^[⁹³93 Borowski, E., Soliman, E., Kandil, U., & Taha, M. (2015). Interlaminar fracture toughness of CFRP Laminates incorporating multi-walled carbon nanotubes. Polymers, 7(6), 1020-1045. http://dx.doi.org/10.3390/polym7061020. http://dx.doi.org/10.3390/polym7061020... ^]
		0.5	–	1175 (25%)
		1	–	1132 (20%)
		1.5	–	1102 (17%)

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