Elsevier

Carbon

Volume 82, February 2015, Pages 143-151
Carbon

Strengthening behavior of few-layered graphene/aluminum composites

https://doi.org/10.1016/j.carbon.2014.10.044Get rights and content

Abstract

Strengthening behavior of composite containing discontinuous reinforcement is strongly related with load transfer at the reinforcement–matrix interface. We selected multi-walled carbon nanotube (MWCNT) and few-layer graphene (FLG) as a reinforcing agent. By varying a volume fraction of the reinforcement, aluminum (Al) matrix composites were produced by a powder metallurgy method. Uniform dispersion and uniaxial alignment of MWCNT and FLG in the Al matrix are evidenced by high-resolution transmission electron microscope analysis. Although the reinforcements have a similar molecular structure, FLG has a 12.8 times larger specific surface area per volume more than MWCNT due to geometric difference. Therefore an increment of a yield stress versus a reinforcement volume fraction for FLG shows 3.5 times higher than that of MWCNT Consequently, for both reinforcements, the composite strength proportionally increases with the specific surface area on the composite, and the composites containing 0.7 vol% FLG exhibit 440 MPa of tensile strength.

Introduction

Graphene has attracted interest as a reinforcing agent for metal matrix composites due to excellent mechanical properties based on the strong sp2 Csingle bondC bonds, which are similar to fullerene and carbon nanotube [1], [2]. Furthermore, it has merits over other carbon-based nano materials, which originate from its inherent two-dimensional (2-D) morphology; the planar structure is more favorable to load transfer as well as to impeding atomic diffusion at high temperatures, as compared to its 0-D and 1-D counterparts. Consequently, it provides superior strength for composites at both room temperature and high temperatures.

In order to transmit the excellent properties of graphene to composites, uniform dispersion of an individually-exfoliated graphene is one key factor. Several processes have been introduced to exfoliate graphite to single-layer or few-layer graphene by mechanical and/or chemical means [3], [4], [5]. Mechanical exfoliation using a tape dispenser [2] or atomic force microscopy (AFM) [6] has exhibited inadequate productivity for large-scale industrial applications. Although large-scale synthesis of graphene by gas phase techniques (e.g., thermal chemical vapor deposition) [7], [8], [9] is actively ongoing, this process is still costly and has restrictions in terms of the selection of the substrate materials. Chemical exfoliation by a solution process has been suggested as a relatively cheap process [10], [11], [12], and yet presents difficulties for scalable synthesis due to complex synthesis steps and the requirement for a large amount of chemicals and acid. Recently, solid phase techniques, combined with ball-milling processes, have enabled production of scalable quantities of carbon-base nano-materials by applying shear forces on pristine agglomerated particles [13], [14], [15].

Even though one has developed a scalable process to produce few-layer graphene (FLG), an additional technical hurdle is in the uniform dispersion of the graphene in the metal matrix, which has closely packed atomic structures. Hence, graphene/metal composites have been seldom investigated compared to polymer matrix composites, although the great strength and light weight features of graphene/metal composites are expected to lead to applications of such composites in the automotive and aerospace industries.

Aluminum (Al) matrix composites reinforced with FLG have recently been produced using different synthesis techniques with powder metallurgy (PM) routes. Table 1 summarizes the fabrication processes and resulting properties of recently developed Al/FLG composites [16], [17], [18], [19], [20], [21]. Similar to other nanostructured composites, dispersion of nanoscale reinforcement is a critical issue in Al/FLG composites. Poorly dispersed FLG may act as defect sites, significantly deteriorating the performance of the final composites [16], [17]. Consolidation processes are also important for Al/FLG composites because a selection of high-processing temperatures to avoid insufficient powder consolidation leads to unfavorable reactions (e.g., transformation of FLG to carbides) [17], [18], [19], [20]. Even though some composites have been produced via cost-ineffective routes or using expensive materials (e.g., graphene oxide), they did not exhibit tensile elongation or they exhibited very limited tensile strength (<300 MPa). Furthermore, the microstructure of Al/FLG composites with an atomic-scale resolution has not been well reported; atomic-scale resolution images may provide detailed information on the morphology of FLG and the interface between Al and FLG [17], [20], [21]. Reinforcement in composites may enhance the strength of the matrix by (i) carrying a great amount of load instead of the matrix and by (ii) interrupting the plastic deformation of the matrix. Hence, two important factors to determine the strengthening efficiency of reinforcement, other than its intrinsic mechanical properties and volume fraction, are (i) how much load can be effectively transmitted from the matrix to the reinforcement and (ii) how much the stress distribution can be altered by the reinforcement. Both are affected by bonding strength between the matrix and reinforcement, morphology/surface area of the reinforcement, and spatial distribution of the reinforcement [22], [23]. Although experimental work on the effect of volume fraction of the reinforcement on the strength of composites [24], [25] and theoretical work on the bonding strength between metal and carbon-based nano materials [26], [27], [28], [29] has been conducted, the role of morphology and surface area on the reinforcement has not been extensively investigated. In particular, a comparison study on the strengthening behavior of reinforcements with a variety of shapes (e.g., fullerene–sphere/0-D, carbon nanotube–tube/1-D, and graphene–planar/2-D), but with similar intrinsic mechanical properties, would be highly interesting.

The primary objective of this work is to produce Al matrix composites with well-dispersed FLG using a scalable powder metallurgy approach. Here, we introduce a favorable route to produce centimeter-scale Al/FLG composites with excellent performances. This work also aims to examine tensile properties of the Al/FLG composite as a function of volume fraction of FLG, so as to compare the strengthening behavior of FLG with that of multi-walled carbon nanotube (MWCNT). The present study also carefully investigates the microstructure of the composites at an atomic scale to provide detailed information on the structure of nano-carbon materials and nano-carbon/Al interface structure. Further, this work quantifies the effect of shape factor (i.e., tube versus sheet) and specific surface area of reinforcement on the composite strength.

Section snippets

Sample preparation

Aluminum (Al)-based composites containing FLG were fabricated by hot-rolling of ball-milled powder. At first, graphite flakes (6–8 nm thickness and 120–150 m2/g typical specific surface area) were mechanically exfoliated by planetary ball milling in the presence of isopropyl alcohol ((CH3)2CHOH). A stainless steel bowl (500 mL) was charged with graphite flakes (2 g) and stainless steel balls (∼5 mm diameter, 30 g) at a ball-to-powder weight ratio of 15:1, together with 50 mL of isopropyl alcohol.

Microstructures

Morphologies of ball-milled Al/FLG composite powders are shown in Fig. 1. Exfoliated FLG sheets with sizes below 10 μm are observed on the surface of the Al powder, where FLG is marked by an arrow in Fig. 1a. Fig. 1b displays magnified images of rectangles in Fig. 1a, where FLG is thin enough to transmit the electron beam so the Al powder underneath the FLG can be seen. Fig. 1c exhibits the powder morphology after attrition milling. FLG is not observed on the powder surface even in the magnified

Conclusion

Al matrix composite containing FLG was successfully produced through a novel fabrication approach that combines mechanical milling and hot rolling. FLG was mechanically exfoliated using wet ball milling, and was then uniformly dispersed in the Al matrix using high energy ball milling. The strengths of the Al/FLG composites are significantly enhanced with the volume fraction of FLG. With an addition of only 0.7 vol% FLG, the composite exhibits ∼440 MPa of tensile strength, about two times higher

Acknowledgements

This research was supported by the National Research Foundation of Korea (NRF) funded by the Ministry of Education (2013R1A2A2A01068931). H.J. Choi acknowledges the support of the NRF funded by the Science, ICT & Future Planning (MSIP) (2013R1A1A3005759 and 2013K1A4A3055679).

References (43)

  • M.K. Yeh et al.

    Mechanical behavior of phenolic-based composites reinforced with multi-walled carbon nanotubes

    Carbon

    (2006)
  • S. Park et al.

    Chemical methods for the production of graphenes

    Nat Nanotechnol

    (2009)
  • A.K. Geim et al.

    The rise of graphene

    Nat Mater

    (2007)
  • A. Martinez et al.

    Mechanical exfoliation of graphene for the passive mode-locking of fiber lasers

    Appl Phys Lett

    (2011)
  • Y. Hernandez et al.

    High-yield production of graphene by liquid-phase exfoliation of graphite

    Nat Nanotechnol

    (2008)
  • A.N. Sidorov et al.

    Graphene nanoribbons exfoliated from graphite surface dislocation bands by electrostatic force

    Nanotechnology

    (2010)
  • X.K. Lu et al.

    Tailoring graphite with the goal of achieving single sheets

    Nanotechnology

    (1999)
  • K. Kim et al.

    Large-scale pattern growth of graphene films for stretchable transparent electrodes

    Nature

    (2009)
  • X.B. Wang et al.

    Large-scale synthesis of few-layered graphene using CVD

    Chem Vapor Depos

    (2009)
  • S.K. Bae et al.

    Roll-to-roll production of 30-inch graphene films for transparent electrodes

    Nat Nanotech

    (2010)
  • S. Stankovich et al.

    Graphene-based composite materials

    Nature

    (2006)
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