Pristine graphene is the strongest material ever measured. However, large-area graphene films produced by means of chemical vapor deposition (CVD) are polycrystalline and thus contain grain boundaries that can potentially weaken the material. We combined structural characterization by means of transmission electron microscopy with nanoindentation in order to study the mechanical properties of CVD-graphene films with different grain sizes. We show that the elastic stiffness of CVD-graphene is identical to that of pristine graphene if postprocessing steps avoid damage or rippling. Its strength is only slightly reduced despite the existence of grain boundaries. Indentation tests directly on grain boundaries confirm that they are almost as strong as pristine. Graphene films consisting entirely of well-stitched grain boundaries can retain ultrahigh strength, which is critical for a large variety of applications, such as flexible electronics and strengthening components.

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.

Although graphene has been successfully grown in large scale via chemical vapor deposition (CVD), it is still questionable whether the mechanical properties of CVD graphene are equivalent to those of exfoliated graphene. In addition, there has been an issue regarding how the tilt angle of the grain boundary (GB) affects the strength of graphene. We investigate the mechanical properties of CVD graphene with nanoindentation from atomic force microscopy and transmission electron microscopy. Surprisingly, the samples with GB angles of 10° and 26° yielded similar fracture stresses of ~ 80 and ~ 79 GPa, respectively. Even for samples with GB exhibiting a wider range, from 0° to 30°, only a slightly wider fracture stress range (~ 50 to ~ 90 GPa) was measured, regardless of tilt angle. The results are contrary to previous studies that have reported that GBs with a larger tilt angle yield stronger graphene film. Such a lack of angle dependence of GB can be attributed to irregular and well-stitched GB structures.

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