Supporting Information

Aligning graphene in bulk copper: nacre-inspired

nanolaminated architecture coupled with in-situ

processing for enhanced mechanical properties and

high electrical conductivity

Mu Cao a, Ding-Bang Xiong a,*, Zhanqiu Tan a, Gang Ji b, Behnam Amin-Ahmadi c, Qiang Guo a,

Genlian Fan a, Cuiping Guo a, Zhiqiang Li a, and Di Zhang a,**

a State Key Laboratory of Metal Matrix Composites, Shanghai Jiao Tong University, Shanghai

200240, China

b Unité Matériaux et Transformations (UMET) CNRS UMR 8207, Université Lille1, 59655

Villeneuve d’Ascq, France

c Electron Microscopy for Materials Science (EMAT), University of Antwerp,

Groenenborgerlaan 171, 2020- Antwerp, Belgium

* Corresponding auther

** Corresponding auther

E-mail address: xiongdingbang@sjtu.edu.cn (Ding-Bang Xiong), zhangdi@sjtu.edu.cn (Di

Zhang)

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Figure S1. SEM illustration of fabrication of nacre-inspired Gr/Cu nanolaminated composites.

Spherical Cu powder (a) was first transformed into flaky Cu powder (b) by a ball-milling

process. (c) The as-obtained flaky Cu powder was soaked in an anisole solution of PMMA

(typically less than 1wt%) and then dried in vacuum, forming a uniform PMMA coating on the

surface. (d) The coated PMMA was used as carbon source for in-situ growing graphene at

elevated temperature. (e) The Gr/Cu composite powder was self-assembled into green compact

by gravity and then hot-pressed. (f) The composite was further densified by a rolling process.

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Figure S2. SEM illustration of the surface of Gr/Cu composite powder obtained from (a) 0.1 wt

%, (b) 0.25 wt%, (c) 0.5 wt%, (d) 1.0 wt% anisole solution of PMMA.

Figure S3. Raman spectroscopy of graphene detached from the composite powder by etching the

Cu substrate.

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Figure S4. X-ray photoelectron spectroscopy (XPS) confirmed the sp2-hybridized carbon orbitals

of graphene and indicated no chemical bonding between graphene and Cu in the as-obtained

Gr/Cu composite powder.

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Figure S5. An EBSD image of the controlled pure Cu sample, revealing equiaxed crystals with

an average size of ~2.02 μm.

Figure S6. Graphite nanoplates or few-layer graphene at interface with different thickness

controlled by the concentration of carbon source PMMA solution.

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Figure S7. Interface bonding strength test. SEM illustration of the fractured interface of (a), (b)

Cu-foil/CVD graphene/Cu-foil sample and (c), (d) Cu foil/ graphene oxide/Cu foil sample.

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Figure S8. Definition on Surface Roughness: (Left) Roughness (2D) parameter: arithmetical

mean deviation of the roughness profile (Ra); (b) Roughness (3D) parameter: arithmetic mean

height (Sa). 3D parameter is expanded from the roughness (2D) parameter Ra. It expresses the

average of the absolute values of Z(x,y) in the measured area. It is equivalent to the arithmetic

mean of the measured region on the three-dimensional display diagram when valleys have been

changed to peaks by conversion to absolute values. Source from

http://www.olympus-ims.com/en/knowledge/metrology/roughness/

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