It is important from a fundamental standpoint and for practical applications to understand how the mechanical properties of graphene are influenced by defects. Here we report that the two-dimensional elastic modulus of graphene is maintained even at a high density of sp 3 -type defects. Moreover, the breaking strength of defective graphene is only B14% smaller than its pristine counterpart in the sp 3 -defect regime. By contrast, we report a significant drop in the mechanical properties of graphene in the vacancy-defect regime. We also provide a mapping between the Raman spectra of defective graphene and its mechanical properties. This provides a simple, yet non-destructive methodology to identify graphene samples that are still mechanically functional. By establishing a relationship between the type and density of defects and the mechanical properties of graphene, this work provides important basic information for the rational design of composites and other systems utilizing the high modulus and strength of graphene.

It is well established that pristine multiwalled carbon nanotubes offer poor structural reinforcement in epoxy-based composites. There are several reasons for this which include reduced interfacial contact area since the outermost nanotube shields the internal tubes from the matrix, poor wetting and interfacial adhesion with the heavily cross-linked epoxy chains, and intertube slip within the concentric nanotube cylinders leading to a sword-in-sheath type failure. Here we demonstrate that unzipping such multiwalled carbon nanotubes into graphene nanoribbons results in a significant improvement in load transfer effectiveness. For example, at ∼0.3% weight fraction of nanofillers, the Young's modulus of the epoxy composite with graphene nanoribbons shows ∼30% increase compared to its multiwalled carbon nanotube counterpart. Similarly the ultimate tensile strength for graphene nanoribbons at ∼0.3% weight fraction showed ∼22% improvement compared to multiwalled carbon nanotubes at the same weight fraction of nanofillers in the composite. These results demonstrate that unzipping multiwalled carbon nanotubes into graphene nanoribbons can enable their utilization as high-performance additives for mechanical properties enhancement in composites that rival the properties of singlewalled carbon nanotube composites yet at an order of magnitude lower cost.

The creep behavior of epoxy-graphene platelet (GPL) nanocomposites with different weight fractions of filler is investigated by macroscopic testing and nanoindentation. No difference is observed at low stress and ambient temperature between neat epoxy and nanocomposites. At elevated stress and temperature the nanocomposite with the optimal weight fraction, 0.1 wt% GPLs, creeps significantly less than the unfilled polymer. This indicates that thermally activated processes controlling the creep rate are in part inhibited by the presence of GPLs. The phenomenon is qualitatively similar at the macroscale and in nanoindentation tests. The results are compared with the creep of epoxy-single-walled (SWNT) and multi-walled carbon nanotube (MWNT) composites and it is observed that creep in both these systems is similar to that in pure epoxy, that is, faster than creep in the epoxy-GPL system considered in this work.

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Various aspects of the mechanical behavior of epoxy-based nanocomposites with graphene platelets (GPL) as additives are discussed in this article. The monotonic loading response indicates that at elevated temperatures, the elastic modulus and the yield stress are significantly improved in the composite as compared to neat epoxy. The activation energy for creep is smaller in neat epoxy, which indicates that the composite creeps less, especially at elevated temperatures and higher stresses. The composites also exhibit larger fracture toughness. When subjected to cyclic loading, fatigue crack growth rate is smaller in the composite relative to neat epoxy. This reduction is important by at least an order of magnitude at all stress intensity factor amplitudes. Optimal property improvements in the monotonic, cyclic, and fracture behaviors are obtained for very low filling fraction of approximately 0.1 wt. %. Similar differences in the mechanical behavior are observed when the composite is probed on the local scale by nanoindentation.

The 2D elastic modulus (E2D) and strength (σ2D) of defective graphene sheets containing vacancies, epoxide, and hydroxyl functional groups are evaluated at 300 K by atomistic simulations. The fraction of vacancies is controlled in the range 0% to 5%, while the density of functional groups corresponds to O:C ratios in the range 0% to 25%. In-plane modulus and strength diagrams as functions of vacancy and functional group densities are generated using models with a single type of defect and with combinations of two types of defects (vacancies and functional groups). It is observed that in models containing only vacancies, the rate at which strength decreases with increasing the concentration of defects is largest, followed by models containing only epoxide groups and those with only hydroxyl groups. The effect on modulus of vacancies and epoxides present alone in the model is similar, and much stronger than that of hydroxyl groups. When the concentration of defects is large, the combined effect of the functional groups and vacancies cannot be obtained as the superposition of individual effects of the two types of defects. The elastic modulus deteriorates faster (slower) than predicted by superposition in systems containing vacancies and hydroxyl groups (vacancies and epoxide groups).

Both one-dimensional carbon nanotubes as well as two-dimensional graphene sheets have been extensively investigated as nanofillers in composites. However there are very few reports on their combined use in composite materials. Here we report the mechanical properties including Young's modulus, tensile strength and fatigue properties of an epoxy polymer reinforced with various combinations of graphene and carbon nanotube fillers- i.e., nanotubes alone, graphene alone and a mixture of graphene and nanotubes. We find that at low nanofillers loadings (< 0.1% weight), the graphene fillers performed better than both singlewalled as well as multiwalled carbon nanotubes. However, interestingly it was the combination of carbon nanotubes with graphene that yielded the greatest improvement in mechanical properties. Optical microscopy of thin micro-tomed slices of the composites indicated that in the presence of the nanotubes the graphene sheets appear to have aggregated into chains forming a network structure. Such long range ordering of the nanofillers is very unusual in a nanocomposite system and is likely responsible for the enhanced mechanical properties.

Creep in graphene platelet–epoxy nanocomposites is significantly slowed down relative to the unfilled epoxy case. This effect is observed primarily at elevated temperatures and when the material is subjected to higher stress. Carbon nanotube–epoxy composites prepared under similar conditions do not exhibit this phenomenon. Fracture surfaces of graphene platelet–epoxy samples, shown here, indicate that graphene flakes also retard the propagation of cracks, while fiber‐like ligaments form during the separation process linking the two crack faces and enhancing the material toughness.