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Acta Metall Sin  2021, Vol. 57 Issue (9): 1087-1106    DOI: 10.11900/0412.1961.2021.00120
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Progress on Graphene/Copper Composites Focusing on Reinforcement Configuration Design: A Review
ZHAO Naiqin(), GUO Siyuan, ZHANG Xiang, HE Chunnian, SHI Chunsheng
School of Materials Science and Engineering, Tianjin University, Tianjin 300350, China
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ZHAO Naiqin, GUO Siyuan, ZHANG Xiang, HE Chunnian, SHI Chunsheng. Progress on Graphene/Copper Composites Focusing on Reinforcement Configuration Design: A Review. Acta Metall Sin, 2021, 57(9): 1087-1106.

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Abstract  

Copper matrix composites have extensive application prospects in electronics and electrical engineering because of their excellent functional and mechanical properties. Graphene has excellent properties and a two-dimensional structure, making it an ideal reinforcement material. Compared with other reinforcements such as particles and whiskers, graphene has better performance matching with copper. Moreover, its distribution in the copper matrix can be controlled well, which can significantly improve the comprehensive properties of the composite. Therefore, controlling the distribution of graphene using novel fabrication processes is essential. This review focuses on the configuration of graphene distributed in a copper matrix (uniform configuration, layered configuration, and network configuration) and the corresponding fabrication processes. The effects of different graphene configurations on the properties of various copper matrix composites are discussed. New ideas for graphene configuration design, future development trends, and potential applications of graphene/copper matrix composites with unique configurations are anticipated.
Key words:  graphene      copper matrix composites      distribution configuration      fabrication process      comprehensive property     
Received:  24 March 2021     
ZTFLH:  TG146.2  
Fund: National Natural Science Foundation of China(51771130)
About author:  ZHAO Naiqin, professor, Tel: (022)85356661, E-mail: nqzhao@tju.edu.cn
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Naiqin ZHAO
Siyuan GUO
Xiang ZHANG
Chunnian HE
Chunsheng SHI

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https://www.ams.org.cn/EN/10.11900/0412.1961.2021.00120     OR     https://www.ams.org.cn/EN/Y2021/V57/I9/1087

Fig.1  Schematic of configuration design of graphene reinforced copper matrix composites
Fig.2  Schematic of the fabrication procedures to fabricate silver nanoparticles modified RGO/Cu composites (GO—graphene oxide, RGO or rGO—reduced graphene oxide) (a), SEM image of distribution of silver nanoparticles modified RGO in the copper matrix (b), and TEM image of RGO/Cu interface (c)[20]
Fig.3  Schematic of RGO/Cu composite powder by electrostatic adsorption (CTAB—cetyl trimethyl ammonium bromide) (a)[23], SEM image of the distribution of RGO in the copper matrix (b)[23], and SEM image of the distribution of RGO on the surface of copper powder after ball milling (Inset shows the magnified image) (c)[24]
Fig.4  Schematic of GNPs/Cu composite prepared by direct current (DC) electrodeposition (GNPs—graphene nanoplatelets, Gr—graphene) (a)[25], schematic diagram of Gr/Cu composite prepared by pulse electrodeposition (i—current density, t—time, Fon—forward pulse duration, Foff—forward pulse off duration, Ron—reverse pulse duration, Roff—reverse pulse off duration) (b)[26], and optical images of copper matrix composite grains obtained by DC electrodeposition (c)[26] and pulse electrodeposition (d)[26]
Fig.5  Preparation of RGO/Cu composites by molecular mixing method (a) and SEM image of the distribution of RGO in the copper matrix (Inset shows the magnified image) (b)[27]
Fig.6  Schematic of Gr/Cu composite prepared by in situ reaction with CH4 as carbon source (CVD—chemical vapor deposition, NPs—nano powders) (a)[28], schematic diagram of Gr/Cu composite prepared by in situ reaction with polymethyl methacrylate (PMMA) as carbon source (b)[29], schematic of graphene-like carbon nanosheet/Cu composite prepared by in situ reaction with oleic acid as carbon source (OA—oleic acid, SPS—spark plasma sintering, GNS—graphene-like carbon nanosheets) (c)[30], and schematic of Gr/Cu composite prepared by in situ reaction with naphthalene and naphthol as carbon source (SAH—small aromatic hydrocarbon) (d)[31]
Fig.7  Schematic of layered distributed graphene/Cu composites prepared by cumulative rolling method (a)[32], schematic of layered distributed RGO/Cu composites prepared by biomimetic method (GrO—graphene oxide, GrO and GO have the same meaning, and GrO is only used in Fig.7; RGrO—reduced graphene oxide, RGrO and RGO have the same meaning, and RGrO is only used in Fig.7) (b)[33], SEM image of RGrO dispersed within copper matrix (c)[33], schematic of preparation of layered distributed GNPs/Cu composites by vacuum filtration (d)[36], and distributions of GNPs with different contents in copper matrix (e, f)[36]
Fig.8  Schematic of layered distributed Gr/Cu composites prepared by in-situ reaction combined with flake powder metallurgy (a)[38], SEM image of Gr dispersed within copper matrix (b)[38], schematic of layered distributed GNPs/Cu composites prepared by in-situ synthesis and rolling (c)[39], and SEM images of microstructure of high content GNPs in the copper matrix (d, e)[39]
Fig.9  Schematic of local continuous three-dimensional network Gr/Cu composites (a)[40], the corresponding G-mode mapping of the selected area of local continuous three-dimensional network Gr/Cu composites from confocal Raman (b)[40], TEM images of three-dimensional network Gr/Cu powders (c, d)[40], schematic of fabrication of continuous three-dimensional networked Gr/Cu composites using PMMA as carbon source (GN—graphene network) (e)[41], TEM image of three-dimensional networked Gr obtained by etching composite powder (Inset shows the magnified image of Gr) (f)[41], SEM image of three-dimensional networked Gr dispersed within copper matrix (g)[41], and TEM image of three-dimensional networked Gr obtained by etching the bulk composite (h)[41]
Fig.10  Schematic diagram of fabrication of continuous three-dimensional networked graphene/copper composites using sucrose as carbon source (RTA—rapid thermal annealing, GLNs—graphene-like nanosheets, GLNN—graphene-like nanosheet network, HP—hot pressing, HR—hot rolling) (a)[42], TEM image of three-dimensional networked Gr obtained by etching composite powder (b)[42], 3D reconstructions of the distribution of Gr in the copper matrix composites after hot pressing and hot rolling processes (c, d)[42], schematic diagram of continuous 3D graphene/copper composites prepared by chemical vapor deposition of copper template (NPC—nano porous Cu, HG—hydrogenated graphite) (e)[43], SEM image of three-dimensional networked Gr dispersed within copper matrix (Inset is a partial enlargment of the sample) (f)[43], and TEM image of three-dimensional networked Gr (g)[43]
Fig.11  Typical load-displacement plot for a double cantilever beam Cu/RGO/Cu specimen (a)[27], the interface bonding model of RGO/Cu composite (b)[47], TEM image of semicoherent interface of Mo2C/Cu (Inset is the superposition of fast Fourier transform of area 1 and area 2) (c)[48], and TEM analyses of semicoherent interface of Cr7C3/Cu (d, e)[49]
Fig.12  SEM images of graphene/Cu composites before (a)[56] and after (b)[56] compression, molecular dynamics simulation of dislocation storage at the graphene/Cu interface during tension (ε—strain) (c)[57], and SEM images of RGO bridging and deflection of cracks in RGO/Cu matrix composites during tensile process (d, e)[33]
Fig.13  SEM images of dynamic tensile process of three-dimensional networked Gr/Cu composites (a, b) and molecular dynamics simulation of the pull-out process of two-dimensional and three-dimensional Gr from copper matrix (c)[42]
DistributionPreparation methodStrength ofTensileRef.
configurationcomposite materialelongation
MPa%
HomogenousRGO modified by Ag + balling milling + HPSRe: 33223.8[20]
distributionRm: 478
RGO modified by Cu/Ni + SPSRe(Cu): 16422[22]
Re(Ni): 18121
RGO modified by Ni + wet mixing + SPSRe: 26812[21]
Rm: 320
Gr/Cu modified by PVA + wet mixing + SPSRe: 1728[18]
Rm: 187
Cu modified by CTAB + SPSRm: 21218[23]
Flake Cu modified by CTAB + SPSRe: 17123[24]
Rm: 233
Molecular-level mixing + SPSRm: 33514[27]
In situ grown Gr + HPSRe: 14437[29]
Rm: 274
In situ grown graphene-like nanosheet + SPS + rollingRm: 41012[30]
In situ grown Gr + SPS + rollingRe: 3933.7[31]
Rm: 477
NetworkIn situ grown discontinuous 3D Gr-like network + SPSRe: 30129[40]
distributionRm: 318
In situ grown 3D Gr network + HPSRe: 29022[41]
Rm: 308
In situ grown 3D Gr network + HPS + rollingRe: 29225.4[42]
Rm: 319
In situ grown 3D Gr network + rolling + sinteringRe: 28116.5[43]
Rm: 354
LaminateBioinspired strategy + HPSRe: 23326[33]
distributionRm: 308
Flaky powder metallurgy + rollingRe: 55710.5[57]
Rm: 705
In situ grown of high content GNPs + HPS + rollingRe: 25514[39]
Rm: 274
In situ grown Gr + flaky powder metallurgy + HPSRe: 20032.3[38]
Rm: 378
Table 1  Mechanical properties of graphene/Cu composites with different configurations[18,20-24,27,29-31,33,38-43,57]
Distribution configurationPreparation method

Electrical conductivity

%IACS

Ref.
Homogenous distributionMechanical milling + HPS94[60]
Ultrasound assisted electroplating44[61]
In situ grown Mo2C@GNPs + HPS + rolling93[48]
Network distributionIn situ grown 3D Gr network + HPS + rolling103[42]
In situ grown 3D Gr network + rolling + sintering98[43]
Laminate distributionIn situ grown Gr + flaky powder metallurgy + HPS97.1[38]
Impregnation reduction + SPS90[62]
In situ grown Gr + HPS117[59]
Table 2  The conductivities of graphene/Cu composites with different configurations[38,42,43,48,59-62]
Fig.14  Schematic of the mechanism of improving electrical conductivity by covering copper films with graphene (GB—grain boundary) (a, b)[67], and schematic of graphene coated copper wires prepared by plasma enhanced chemical vapor deposition (PECVD) method (LT—low temperature) (c)[68]
Distribution configurationPreparation method

Thermal conductivity

W·m-1·K-1

Ref.
Homogenous distributionElectrostatic self-assembly + HPS370-396[23]
Vacuum filtration + SPS275-325[36]
Network distributionIn situ grown 3D Gr network + HPS + rolling413[42]
Laminate distributionIn situ grown of high content GNPs + HPS + rolling441[39]
Vacuum filtration + vortex mixing + SPS525[36]
Vacuum filtration + vortex mixing + SPS458[37]
In situ grown Gr + HPS375[71]
In situ grown Gr + hot isostatic pressing + roll-to-roll394[72]
Table 3  The thermal conductivities of graphene/Cu composites with different configurations[23,36,37,39,42,71,72]
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