Applications of Wet-Functionalized Graphene in Rubber Composites

doi:10.7536/PC180817

Vulcanized rubber products have been applied in various fields for more than 100 years, due to their high elasticity, good biological compatibility, chemical resistance, long-time use stability, etc. Additives like reinforcing fill er, lubricant, coupling agent, and accelerating agent, are necessary to be mixed with the raw rubber to give the rubber certain properties. Specifically, the rein-forcing filler plays the role of enhancing the mechanical strength, abrasive and thermal resistance, as well as prolonging the service life of the rubber. Compared with the traditional reinforcing fillers like carbon black and fumed silica, the graphene, a newly emerging nanomaterial, can reinforce the rubber properties with very small incorporation amount, due to its superior properties. However, the strong van der Vaals force amongst graphene sheets seriously inhibits its dispersion in the rubber. Meanwhile, the dispersion state of the graphene in silicone rubber matrix directly influences the reinforcing effect of the graphene. In recent years, many researchers focus on the functionalization method of the graphene, physically or chemically, to enhance the dispersion of the graphene in rubber matrix, and the interfacial interactions between graphene and rubber. The recent advances in the wet functionalization approaches conducted to the graphene and the applications of the functional graphene in fabricating rubber composites are discussed.

Key words: graphene, functionalization, rubber composites, mechanical properties, thermal properties, electrical properties

Fig. 1 Schematic illustration of GO and reduced GO formation[44, 45]

Table 1 Mechanical properties of physically functionalized graphene/rubber composites

Rubber Type	Preparation method	Functionalization agent	Tensile strength enhancement	ref
NR	Solution mixing	Surfactant	29%	24
SBR	Mechanical mixing	Ionic liquid	490%	32
SBR	Roll milling	Ionic liquid	45%	33
SR	Solution mixing	Silane	~241%	61
SR	Roll milling	SiO₂	~131%	43
NR	Roll milling	ZnO	12.7%	42
NR	Roll milling	ZnO	133%	62
BroR	Solution mixing	CaF₂	70%	63
NBR	Roll milling	Sodium humate	120%	64
NR	Mechanical mixing	Polymer	646%	40
NR	Roll milling	Polymer	23%	65
NR	Solution Casting	Polymer	2900%	41
NR	Solution mixing	Polymer	58%	66
NR	Roll milling	Polymer	~80%	67

Table 1 Mechanical properties of physically functionalized graphene/rubber composites

Rubber Type	Preparation method	Functionalization agent	Tensile strength enhancement	ref
NR	Solution mixing	Surfactant	29%	24
SBR	Mechanical mixing	Ionic liquid	490%	32
SBR	Roll milling	Ionic liquid	45%	33
SR	Solution mixing	Silane	~241%	61
SR	Roll milling	SiO₂	~131%	43
NR	Roll milling	ZnO	12.7%	42
NR	Roll milling	ZnO	133%	62
BroR	Solution mixing	CaF₂	70%	63
NBR	Roll milling	Sodium humate	120%	64
NR	Mechanical mixing	Polymer	646%	40
NR	Roll milling	Polymer	23%	65
NR	Solution Casting	Polymer	2900%	41
NR	Solution mixing	Polymer	58%	66
NR	Roll milling	Polymer	~80%	67

Fig. 2 The preparation of pristine graphene, ZDMA- graphene and NR/ZDMA-graphene composites [62]

Table 2 Mechanical properties of GO/rubber composites

Rubber Type	Preparation method	Incorporation amount	Tensile strength enhancement	ref
NR	Roll milling	1.0 wt%	135%	47
NR	Solution mixing	4.0 wt%	75%	68
NR	Latex mixing	0.7 wt%	87%	69
NR	Roll milling	0.5 wt%	29%	70
NR	Roll milling	5.0 wt%	~100%	71
SBR	Roll milling	5.0 wt%	747%	72
SBR	Latex mixing	7.0 wt%	992%	50
SBR	Roll milling	3.0 wt%	490%	73
SBR	Latex mixing	3.0 wt%	~300%	74
NBR	Solution blending	~0.4 wt%	51%	48
NBR	Roll milling	~1.0 wt%	369%	75
NBR	Roll milling	~3.0 wt%	110%	76
SR	Solution mixing	2.0 wt%	67%	77
SR	Solution mixing	1.0 wt%	181%	49
SR	Mechanical mixing	0.5 wt%	158%	78

Table 2 Mechanical properties of GO/rubber composites

Rubber Type	Preparation method	Incorporation amount	Tensile strength enhancement	ref
NR	Roll milling	1.0 wt%	135%	47
NR	Solution mixing	4.0 wt%	75%	68
NR	Latex mixing	0.7 wt%	87%	69
NR	Roll milling	0.5 wt%	29%	70
NR	Roll milling	5.0 wt%	~100%	71
SBR	Roll milling	5.0 wt%	747%	72
SBR	Latex mixing	7.0 wt%	992%	50
SBR	Roll milling	3.0 wt%	490%	73
SBR	Latex mixing	3.0 wt%	~300%	74
NBR	Solution blending	~0.4 wt%	51%	48
NBR	Roll milling	~1.0 wt%	369%	75
NBR	Roll milling	~3.0 wt%	110%	76
SR	Solution mixing	2.0 wt%	67%	77
SR	Solution mixing	1.0 wt%	181%	49
SR	Mechanical mixing	0.5 wt%	158%	78

Table 3 Mechanical properties of molecules grafted graphene/rubber composites

Rubber Type	Preparation method	Grafted molecules	Tensile strength enhancement	ref
NR	Solution mixing	Silane	~100%	55
SR	Solution mixing	Silane	>50%	57
NBR	Latex mixing	Silane	~120%	79
SBR	Latex mixing	Amine	330%	53
BroR	Solution mixing	Amine	23%	54
SBR	Roll milling	Amide	650%	59
SBR	Latex mixing	Ortho-quinone	800%	80
SBR	Mechanical mixing	Silane	~775%	81
SBR	Latex mixing	Thiol	~50%	52
SBR	Solution mixing	Thiol	180%	82
NR	Latex mixing	Polymer	22%	83
SBR	Latex mixing	Polymer	540%	84
SBR	Roll milling	Polymer	17%	60
NBR	Solution mixing	Polymer	215%	85
BroR	Solution mixing	Polymer	200%	87

Table 3 Mechanical properties of molecules grafted graphene/rubber composites

Rubber Type	Preparation method	Grafted molecules	Tensile strength enhancement	ref
NR	Solution mixing	Silane	~100%	55
SR	Solution mixing	Silane	>50%	57
NBR	Latex mixing	Silane	~120%	79
SBR	Latex mixing	Amine	330%	53
BroR	Solution mixing	Amine	23%	54
SBR	Roll milling	Amide	650%	59
SBR	Latex mixing	Ortho-quinone	800%	80
SBR	Mechanical mixing	Silane	~775%	81
SBR	Latex mixing	Thiol	~50%	52
SBR	Solution mixing	Thiol	180%	82
NR	Latex mixing	Polymer	22%	83
SBR	Latex mixing	Polymer	540%	84
SBR	Roll milling	Polymer	17%	60
NBR	Solution mixing	Polymer	215%	85
BroR	Solution mixing	Polymer	200%	87

Table 4 Thermal properties of physically functionalized graphene/rubber composites

Rubber Type	Preparation method	Functionalization agent	Enhanced thermal properties	ref
NR	Solution mixing	Surfactant	Thermal stability	89
SBR	Mechanical mixing	Ionic liquid	Thermal stability	34
SBR	Roll milling	Ionic liquid	Thermal stability	33
SBR	Roll milling	Ionic liquid	Thermal conductivity	34
BroR	Roll milling	Ionic liquid	Thermal stability Thermal conductivity	31
SR	Solution mixing	Silane	Thermal conductivity	61
SR	Mechanical mixing	Silane	Thermal conductivity	90
SR	Mechanical mixing	Silane	Thermal conductivity	91
NR	Roll milling	ZnO	Thermal conductivity	62
NR	Roll milling	Polymer	Thermal conductivity	65
NR	Mechanical mixing	Polymer	Thermal conductivity	67
NR	Melt blending	Polymer	Thermal stability	92

Table 4 Thermal properties of physically functionalized graphene/rubber composites

Rubber Type	Preparation method	Functionalization agent	Enhanced thermal properties	ref
NR	Solution mixing	Surfactant	Thermal stability	89
SBR	Mechanical mixing	Ionic liquid	Thermal stability	34
SBR	Roll milling	Ionic liquid	Thermal stability	33
SBR	Roll milling	Ionic liquid	Thermal conductivity	34
BroR	Roll milling	Ionic liquid	Thermal stability Thermal conductivity	31
SR	Solution mixing	Silane	Thermal conductivity	61
SR	Mechanical mixing	Silane	Thermal conductivity	90
SR	Mechanical mixing	Silane	Thermal conductivity	91
NR	Roll milling	ZnO	Thermal conductivity	62
NR	Roll milling	Polymer	Thermal conductivity	65
NR	Mechanical mixing	Polymer	Thermal conductivity	67
NR	Melt blending	Polymer	Thermal stability	92

Fig. 3 Filler-matrix interactions in SBR composite system[34]

Table 5 Thermal properties of covalently functionalized graphene/rubber composites

Rubber Type	Preparation method	Functionalization agent	Enhanced thermal properties	ref
SBR	Roll milling	Amine	Thermal stability	94
BroR	Solution mixing	Amine	Thermal stability	54
SR	Solution mixing	Amide	Thermal conductivity	95
EPR	Mechanical mixing	Silane	Thermal stability	56, 96
SR	Solution mixing	Silane	Thermal stability Thermal conductivity	58, 97
SR	Mechanical mixing	Pentaerythritol	Thermal stability	98
NBR	Solution mixing	Polymer	Thermal conductivity	99
BroR	Solution mixing	Polymer	Thermal stability	86

Table 5 Thermal properties of covalently functionalized graphene/rubber composites

Rubber Type	Preparation method	Functionalization agent	Enhanced thermal properties	ref
SBR	Roll milling	Amine	Thermal stability	94
BroR	Solution mixing	Amine	Thermal stability	54
SR	Solution mixing	Amide	Thermal conductivity	95
EPR	Mechanical mixing	Silane	Thermal stability	56, 96
SR	Solution mixing	Silane	Thermal stability Thermal conductivity	58, 97
SR	Mechanical mixing	Pentaerythritol	Thermal stability	98
NBR	Solution mixing	Polymer	Thermal conductivity	99
BroR	Solution mixing	Polymer	Thermal stability	86

Fig. 4 Scheme of procedure for preparation of TEVS-GO and TEVS-GO/LSR composites[58]

Table 6 Electrical properties of physically functionalized graphene/rubber composites

Rubber Type	Preparation method	Functionalization agent	Threshold	ref
NR	Solution mixing	Surfactant	~3 wt%	102
NR	Solution mixing	Surfactant	3 wt%	103
NR	Solution mixing	Surfactant	~4.28 wt%	29
NR	Mechanical mixing	Surfactant	~5 wt%	37
NR	Mechanical mixing	Polymer	~1 wt%	40
NR	Solution mixing	Polymer	~1 wt%	39
NR	Solution Casting	Polymer	~0.4 wt%	41
NR	Solution mixing	Polymer	-	66
SBR/NR	Mechanical mixing	Polymer	~0.3 wt%	37

Table 6 Electrical properties of physically functionalized graphene/rubber composites

Rubber Type	Preparation method	Functionalization agent	Threshold	ref
NR	Solution mixing	Surfactant	~3 wt%	102
NR	Solution mixing	Surfactant	3 wt%	103
NR	Solution mixing	Surfactant	~4.28 wt%	29
NR	Mechanical mixing	Surfactant	~5 wt%	37
NR	Mechanical mixing	Polymer	~1 wt%	40
NR	Solution mixing	Polymer	~1 wt%	39
NR	Solution Casting	Polymer	~0.4 wt%	41
NR	Solution mixing	Polymer	-	66
SBR/NR	Mechanical mixing	Polymer	~0.3 wt%	37

Fig. 5 Schematic of the one-step method for functionalized graphene/NRL nanocomposites production[41]

Fig. 6 Schematic illustration for the fabrication of functionalized graphene/SBR-NR with a double-interconnected network[37]

Table 7 Electrical properties of in-situ reduced GO/rubber composites

Rubber Type	Preparation method	Functionalization agent	Threshold	ref
NR	Roll milling	Thermal reduction	~0.5 wt%	47
NR	Solution mixing	Hydrazine	~0.6 wt%	104
NR	Solution mixing	NaBH₄	~0.5 wt%	27
NR	Mechanical mixing	Hydrazine	~0.3 wt%	105
NR	Solution mixing	Hydroiodic acid	~0.3 wt%	106
NR	Solution mixing	Hydrazine	~3 wt%	107
SBR	Solution mixing	Hydrazine	~2 wt%	50
NBR	Solution mixing	Hydrazine	~0.25 wt%	108
NBR	Solution mixing	Hydrazine	~0.75 wt%	93
NR/SBR/SR	Solution mixing	Thermal reduction	~0.5 wt%	109

Table 7 Electrical properties of in-situ reduced GO/rubber composites

Rubber Type	Preparation method	Functionalization agent	Threshold	ref
NR	Roll milling	Thermal reduction	~0.5 wt%	47
NR	Solution mixing	Hydrazine	~0.6 wt%	104
NR	Solution mixing	NaBH₄	~0.5 wt%	27
NR	Mechanical mixing	Hydrazine	~0.3 wt%	105
NR	Solution mixing	Hydroiodic acid	~0.3 wt%	106
NR	Solution mixing	Hydrazine	~3 wt%	107
SBR	Solution mixing	Hydrazine	~2 wt%	50
NBR	Solution mixing	Hydrazine	~0.25 wt%	108
NBR	Solution mixing	Hydrazine	~0.75 wt%	93
NR/SBR/SR	Solution mixing	Thermal reduction	~0.5 wt%	109

Fig. 7 The preparation of rGO/rubber composites with a conductive segregated network[104]

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Applications of Wet-Functionalized Graphene in Rubber Composites

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Applications of Wet-Functionalized Graphene in Rubber Composites