Highly conductive graphene paper for flexible electronics applications


A high quality graphene paper has been fabricated using drop-casting of a custom developed stable ink mixture. The graphene/ethyl cellulose mixture can produce graphene paper coating on Kapton substrate at fairly large scales by finely adjusting the viscosity of the ethyl cellulose solvent blend. It was possible to produce a morphologically intact 300 nm-thick stacked structures of high purity graphene platelets after annealing at 300 °C, as characterized by SEM, Raman Spectroscopy and AFM. The electrical resistivity of a large batch of samples was measured and the results thoroughly evaluated, using a design of experiments approach. The resistivity values achieved were found to be lower or comparable to the best results reported in the literature. As expected, resistivity is inherently related to the concentration of the as-prepared ink and subsequent annealing conditions. However, prolonged annealing time can deteriorate mechanical properties as determined by cyclic bending and shear tests. It is anticipated that the present graphene paper has potential use in flexible electronics applications since the lowest resistivity and structure achieved were generally unaffected by the range of mechanical loadings studied.

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The main author, K. Karimi, gratefully acknowledges the financial support from the University of Waterloo. This work would not have been possible without the use of equipment and assistance of the technical staff of the Multiscale Additive Manufacturing Lab (MSAM) and the Composites and Adhesives Lab in the Department of Mechanical and Mechatronics Engineering.

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Correspondence to Elahe Jabari.

Appendix: Details of experimental methods

Appendix: Details of experimental methods

Electrical resistance measurement fixture

In this study, an electrical fixture was built, as schematically shown in Fig. 9 to obtain an electrical field that would be linear and with minimal error when testing the graphene paper samples (Fig. 10).

Fig. 9

2D representation of the electrical fixture with its components

Fig. 10

3D representation of the electrical fixture with its components

Cyclic bending test setup

A bending fatigue test was conducted to study the effect of repeated bending on the electrical properties of graphene paper. The specimen used was the same size as in the sheet resistance tests. In this test, 15 different samples with five different annealing times (Fig. 3) were subjected up to 400 cycles to investigate the effect of cyclic bending on the graphene paper structures produced by different annealing times. In each cycle, to apply reproducible bending strains, each sample was completely bent over a cylinder with specific radius, held for a second and then released. The first 200 cycles were completed using an 8 mm radius of curvature, followed by 200 cycles using a 4 mm radius of curvature, as illustrated in Fig. 11.

Fig. 11

Fatigue bending graphene paper sample and set-up

Adhesion test procedure


The test setup comprised a load cell on a horizontal platform with a film gripper at one end and an electronic chip controlling the load cell at the other end. The electronic chip controls the load cell such that it always pulls the sample with constant velocity regardless of the amount of the force being applied. As schematically shown in Fig. 12, samples were mounted on the film gripper while they had a backing underneath. Then, a layer of soft tissue, Kimwipe, was placed on the sample. Different weights were placed on the tissue and retained with the help of a retort stand holding a rubber ring. Therefore, friction force was applied on the surface of the graphene paper by the surface of the tissue when the sample as being pulled by the load cell. Finally, the desired results were recorded by visually checking the tissue for residue and reading the force value displayed on the load cell (Fig. 13).

Fig. 12

Adhesion test setup and its components

Fig. 13

Adhesion test setup and its components


Figure 14 illustrates the free body diagram of the sample mounted on the adhesion test setup described in Fig. 12. Accordingly, the force acting on the surface of the graphene paper should be known.

Fig. 14

Free body diagram of graphene paper coating with Kapton substrate mounted on the adhesion test setup

It is noted that the force from load cell is applied to the graphene paper and kapton substrate simultaneously since both are held by the film gripper attached to the end of the load cell. Also, Fig. 14 represents an equation with two unknowns since the coefficient of the kinetic friction between acrylic and kapton is not known. An estimated value is required before conducting the adhesion experiment. To do so, a kapton film without any graphene coating was mounted on the setup. An acrylic block with a known mass was placed on the kapton. The coefficient of kinetic friction between kapton and acrylic could be derived since the same material has been used above and underneath the sample. Accordingly, the value was calculated to be \({\mu _{k~(Acrylic - Kapton)}}=0.2\).

Newton’s first law applies for the adhesion test because the sample is pulled with constant velocity. Therefore:

$$\sum F = 0 \to ~F_{{Loadcell}} - F_{{Acrylic - Kapton}} - F_{{KimWipe - Graphene}} = 0~ \to F_{{KimWipe - Graphene}} = ~F_{{Loadcell}} + F_{{Acrylic - Kapton}} = ~F_{{Loadcell}} + ~\mu _{{k~(Acrylic - Kapton)}} ~{\text{mg}}$$

where m is the mass of the weights measured in kg and g is gravitational acceleration measured in m/s2.

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Karimi, K., Jabari, E., Toyserkani, E. et al. Highly conductive graphene paper for flexible electronics applications. J Mater Sci: Mater Electron 29, 2537–2549 (2018). https://doi.org/10.1007/s10854-017-8176-8

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