Carbon nanotube-reinforced elastomeric nanocomposites: a review

Figures & data

Figure 1. Structure of (a) graphite sheet, (b) single-wall (SWCNT), (c) double-wall (DWCNT), and (d) multiwall carbon nanotube (MWCNT) (available from online: http://jnm.snmjournals.org/content/48/7/1039/F1.expansion.html).

Figure 2. Schematic diagram showing how a hexagonal sheet of graphite is ‘rolled’ to form a carbon nanotube. Reprinted from reference [4].

Figure 3. Illustrations of the atomic structure of (a) an armchair and (b) a ziz-zag nanotube. Reprinted from reference [4].

Figure 4. A trend in the research activity of CNTs and CNT-related polymer composites over the years (available at: https://sites.google.com/site/cntcomposites/Home).

Figure 5. A trend of the research activity of CNT-related elastomeric composites over the years.

Figure 6. Various covalent functional modifications possible with carbon nanotubes. Reprinted from reference [52].

Figure 7. A schematic representation of adsorption behavior of surfactants onto the surface of CNTs. Reprinted from reference [59].

Table 1. Modification types of CNTs and their composites with rubber matrices.

Type of modification	Modifier	Rubber–CNT composite
Covalent	Acid treatment	NR/SBR-MWCNT [21], NR-MWCNT [60,61], NR-SWCNT [36,62],TPE-MWCNT [27], IIR-MWCNT [38], NBR/SBR-MWCNT [63], PDMS-MWCNT [47,64], CIIR-MWCNT [44], Soft epoxy [65], EPDM-MWCNT [66], SBR-CNT [67], TPU-MWCNT [68]
	Hydroxyl (-OH)	SBR/BR-MWCNT [69]
	Grafting	TPU-MWCNT [70]
	Amino/silane	NR-MWCNT [33], PDMS-MWCNT [71], BADGE/ATBN-MWCNT [72], TPU-MWCNT [73]
Non-covalent	Ionic surfactant	CR-MWCNT [34,41,74,75,76], PDMS-SWCNT [77,78], NR-MWCNT [79,80], PDMS-MWCNT [81], SBR/BR [82], NR
	Non-ionic	NR/SBR-MWCNT [83], SBR/BR-MWCNT [69]
	Catalyst	SEBS-SWCNT [39]

Table 2. Mechanical properties of elastomeric/CNT nanocomposites.

Composite	Processing	TS increase (%)	EM increase (%)	EB increase (%)	Ref
NR + 3 phr MWCNT	Melt	~1378	~260	~(226)	[100]*
NR + 1 phr MWCNT + 29 phr silica	Melt	~38	~26	~(33)	[101]*
NR + 25 phr SWCNT	Melt	~173	~317	~(−27)	[62]^x
NR + 3 phr MWCNT + 40 phr silica	Melt	~2422	~380	~(264)	[100]*
NR + NBR + 2 phr MWCNT	Melt	~18	~100	~(−5)	[83]^y
EPDM + 3 phr MWCNT	Melt	~161	~90	~(71)	[100]*
EPDM + 3 phr MWCNT + 40 phr CB	Melt	~1587	~260	~(203)	[100]*
SBR + 5 phr MWCNT	Melt	~248	~85	~(38)	[67]^x
SBR + 5 phr MWCNT	Melt	~146	~157	~(10)	[102]*
SBR + 5 phr MWCNT + 20 phr EG	Melt	~296	~530	~(−3)	[102]*
SBR/BR + 5 phr MWCNT	Melt	~246	~150	~(66)	[69]^x
SBR + BR + 3 phr CNT + 40 phr silica	Melt	~839	~320	~(71)	[100]*
TPU + 3 wt% MWCNT-g-PTMEG	Melt	~(−4)	~4	~(−6)	[70]^x
SBR + 15 phr MWCNT	Solid (two-roll)	~293	~262	N/A	[63]^x
PDMS + 5 wt% MWCNT	Solid (two-roll)	~155	N/A	~(−21)	[64]^x
MVQ + 0.75 wt% MWCNT	Solvent	~38	~82	~(−46)	[103]*
MVQ + MWCNT + G (0.75 wt%)	Solvent	~109	~96	~(1)	[103]*
PDMS + 1.6 wt% SWCNT	Solvent	~14	−32	~(33)	[77]*
PDMS + 4 wt% SWCNT	Solvent	~183	~629	~(−7)	[78]^y
TPU + 1 wt% (MWCNT+HNT)	Solvent	~143	~35	~(68)	[68]^x
NR + 25 phr CNT	Solvent	~244	~594	~(−27)	[36]^x
SEBS + 1.5 wt% SWCNT	Solvent	~24	~154	~(−8)	[39]^y
NR + 1 phr MWCNT	Solvent and melt	~26	~26	~(−31)	[60]^x
NR + 1 wt% MWCNT	Latex	~58	~33	~(3)	[61]^x
SBR + 25 phr MWCNT	Latex and melt	~80	~163	~(−18)	[104]*

*untreated CNT, ^xcovalently treated CNT, ^ynon-covalently treated CNT.

Table 3. Percolation threshold of CNT/elastomeric composites and their hybrids compounds.

Polymer	Filler	Processing	Percolation threshold	Ref
SBR	MWCNT	Melt	(5)^b	[104]*
SBR/BR	MWCNT	Melt	(<2)^a	[69]^x
SBR/BR	MWCNT	Melt	(<3)^a	[82]^y
SBR/NBR	MWCNT	Melt	(~0.2 and 1)^a	[86]*
NR/NBR	MWCNT	Melt	(2)^b	[83]^y
CIIR	MWCNT	Melt	(6)^b	[44]^x
IIR	MWCNT	Melt	(6 ~ 8)^b	[38]^x
CR	MWCNT	Melt	(5)^b	[76]^y
NBR	MWCNT	Solid (two-roll)	(10)^b	[63]^x
CR	MWCNT	Solid (two-roll)	(3)^b	[34]^y
NR	MWCNT	Solid (two-roll)	(9 ~ 16)^a	[105]*
SR	MWCNT	Solvent	(<0.1)^a	[106]*
SR	MWCNT	Solvent	(~1.0)^c	[107]*
SR	SWCNT	Solvent	(4)^a	[78]^y
PSF	MWCNT	Solvent	(0.1 ~ 0.3)^a	[20]*
NR	MWCNT	Solvent	(0.5–1)^b	[25]*
TPU	MWCNT	Solvent	(0.5 ~ 10)^c	[85]*
EPDM	MWCNT	Solvent	(4)^b	[87]*
MVQ	MWCNT	Solvent	(1.6)^c	[81]^y
MVQ	MWCNT/TRG	Solvent	(2 and 5)^a	[108]*
SBR	SWCNT	Solvent	(0.27)^a	[109]*
SBR	MWCNT	Solvent	(2 and 3)^b	[110]*
PDMS	MWCNT	Manual	(~0.6)^a	[111]*
SR	MWNCT	High-shear	(5 and 10)^a	[64]^x

^awt%, ^bphr, ^c(vol%), *untreated CNT, ^xcovalently treated CNT, ^ynon-covalently treated CNT.

Figure 8. TEM images of SBR-MWCNT composite (0.75 phr) prepared by (a) a rotation–revolution mixer, (b) Banbury mixer [109]; TEM images of NR composite filled with 1% of (c) unmodified CNT, (d) acid-treated CNT [60]; SEM micrographs of NR composites filled with (e) acid-treated MWCNTs, (f) unmodified MWCNTs [61]; SEM images of CNT-filled rubber composite containing 7 phr CNT: (g) without stretching; (h) at 15% stretching [113].

Figure 9. AFM and EFM images of CNT dispersion in elastomeric matrix: (a) AFM images of composite with 2.8 wt% MWCNT before coagulation, (b) after coagulation of the latex beads at 60°C [24], (c) EFM phase image at 0 V, and (d) EFM phase image at 7 V of NBR-MWCNT composite [116].

Figure 10. Raman spectrum of MWCNT, MWCNT-rubber, and MWCNT-IL-rubber composites. IL represents an ionic liquid of 1-allyl-3methylimidazolium chloride, and the MWCNT loading was 3 phr [82].

Figure 11. (a) Stress–strain curves of NR, NR/CNT, and NR/CB compounds and (b) storage modulus of NR/CNT and NR/CB compounds at different filler loadings as a function of dynamic strain amplitude [114].

Figure 12. An illustration of percolation threshold by network formation of CNTs in a rubber matrix.

Figure 13. Dependence of CNT loading on the volume resistivity of NR, SBR, and EPDM composites [87].

Table 4. TGA results for the SBR and NBR reinforced with multiwall carbon nanotubes under N₂ atmosphere [63].

	SBR		NBR
	First weight loss		First weight loss		Second weight loss
CNT (phr)	Maximum (°C)	Residue (wt%)	Maximum (°C)	Residue (wt%)	Maximum (°C)	Residue (wt%)
0	447.4	5.0	423.9	64.9	445.7	9.2
2	450.0	6.4	424.1	64.1	446.5	12.0
5	451.3	8.8	425.8	61.7	425.8	11.8
10	454.8	12.9			443.5	17.7
15	455.1	16.3			452.7	20.6

Figure 14. TGA thermograms (a) and corresponding DTG curve (b) of pure silicone rubber (SR) and SR/MWCNTs nanocomposites [140].

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