IntroductionDue to the rapid development of nanoscience and nanotechnology in the past 20 years, improvement of polymer properties by nanofillers has become a vital topic in the field of material science. [1][2][3] The polymer nanocomposites show enhanced properties by the incorporation of low amount of nanofillers such as carbon black (CB), carbon nanotubes (CNTs), graphene and nanoclay. [4][5][6][7] Due to the high surface to volume ratio and/or high aspect ratio, the nanofillers are more efficient than the traditional fillers in reinforcing polymers. 8,9 Among the nanofillers, graphene is an atomically thick, 2D nanomaterial that is the strongest materials measured so far. it has intensively attracted a great deal of interest in extensively exploring its applications. The superior properties of graphene also reflected in the graphene/polymer nanocomposites. It has been widely reported that the mechanical, thermal, electrical, gas-barrier and flame-retardant properties of polymer can be significantly improved by the addition of graphene. 3,6,[18][19][20][21][22][23][24] Its advantages over other nanofillers have been discussed. 3,19,[25][26][27][28] However, the reinforcing efficiency of graphene highly depends on the dispersion and distribution of graphene sheets in the polymer matrix. 29 An optimized graphene-polymer interface is critical in the property transfer. [30][31][32] Pristine graphene sheets are not compatible with organic polymers and have a great tendency to agglomerate in the matrix. 3,33,34 To resolve this problem, functionalization of graphene is an essential step to achieve a molecular level dispersion.3,35 The functionalized graphene (FG) sheets could form strong interfacial bonding with polymer chains, which is favorable for load transfer, but it also confines the motion of interfacial polymer segments. [36][37][38] Thus, the enhancements in stiffness, tensile strength and hardness of polymer are frequently reported, while the elongation at break and ductility is always decreased. 3,6,39 Toughness of polymer is extremely important in the critical structural applications and highperformance areas such as automotive, aerospace and defence. 9,40 Enhancing the toughness of polymer has been a challenging issue, especially for thermosets that have highly cross-linked structure.
9Traditional fillers, such as rubber particles, can improve the toughness, but they show negative impact on mechanical properties and manufacturability. 38,41 In the past few years, toughening of polymers by graphene has been explored and reported in a few publications. 25,[29][30][31][32]38,[42][43][44][45][46][47][48][49][50][51][52][53][54][55] According to the results, it is believed that the incorporation of FG can toughen polymers including both thermoplastics and thermosets, although the understanding of the mechanism is still insufficient. In this review, the authors try to focus on the recent development on the Toughening of polymers by graphene Wang and Song ICE Publishing: All rights reserved