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Investigating Stress Transfer and Failure Mechanisms in Graphene Oxide-Cellulose Nanocrystals Films



Graphene oxide (GO) films have great potential for aerospace, electronics, and renewable energy applications. GO sheets are low-cost and water-soluble and retain some of Graphene’s exceptional properties once reduced. GO or reduced GO (rGO) sheets within a film interact with each other via secondary bonds and cross-linkers. These interfacial interactions include non-covalent bonds such as hydrogen bonding, ionic bonding, and π-π stacking. Stress transfer and failure mechanisms in GO and rGO films, specifically how linkers affect them, are not well understood. The present study investigates the influence of inter-particle interactions and film structures, focusing on hydrogen bonds introduced via cellulose nanocrystals (CNC), on failure and stress-transfer of the GO and rGO films. To this end, GO films with CNC crosslinkers were made, followed by a chemical reduction. The few-micron thick films were characterized using tensile testing. All tested films exhibited a brittle failure and achieved tensile strengths and modulus in the ~40-85 MPa and ~3.5-9 GPa ranges, respectively. To reveal stress transfer mechanisms in each sample, tensile in-situ Raman spectroscopy testing was carried out. By monitoring the changes in bandwidth and position of Raman bands while stretching the film, useful information such as sheet slippage and cross-linker interactions were gathered. The addition of CNC enhanced modulus but degraded strength for both GO and rGO films. Interestingly, the Raman G-peak shift at failure, indicative of stress transfer to individual GO/rGO particles, is commensurate with the films’ strengths. Correlating these results with the structure and composition of different films reveals new understanding of stress transfer between GO/rGO particles, paving the way for the scalable manufacturing of strong and stiff GO-based films.


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L. Liu, J. Zhang, J. Zhao, and F. Liu, "Mechanical properties of graphene oxides," Nanoscale,

vol. 4, no. 19, p. 5910, 2012, doi: 10.1039/c2nr31164j.

S. Pei, J. Zhao, J. Du, W. Ren, and H.-M. Cheng, "Direct reduction of graphene oxide films

into highly conductive and flexible graphene films by hydrohalic acids," Carbon, vol. 48, no.

, pp. 4466-4474, 2010/12 2010, doi: 10.1016/j.carbon.2010.08.006.

C. Cao, M. Daly, C. V. Singh, Y. Sun, and T. Filleter, "High strength measurement of

monolayer graphene oxide," Carbon, vol. 81, pp. 497-504, 2015/01 2015, doi:


V. B. Mohan, R. Brown, K. Jayaraman, and D. Bhattacharyya, "Characterisation of reduced

graphene oxide: Effects of reduction variables on electrical conductivity," Materials Science

and Engineering: B, vol. 193, pp. 49-60, 2015/03 2015, doi: 10.1016/j.mseb.2014.11.002.

J. Chen, H. Li, L. Zhang, C. Du, T. Fang, and J. Hu, "Direct Reduction of Graphene

Oxide/Nanofibrillated Cellulose Composite Film and its Electrical Conductivity Research," (in

eng), Sci Rep, vol. 10, no. 1, pp. 3124-3124, 2020, doi: 10.1038/s41598-020-59918-z.

A. Pareek and S. Venkata Mohan, "Graphene and Its Applications in Microbial

Electrochemical Technology," in Microbial Electrochemical Technology, ed: Elsevier, 2019,

pp. 75-97.

O. C. Compton et al., "Tuning the Mechanical Properties of Graphene Oxide Paper and Its

Associated Polymer Nanocomposites by Controlling Cooperative Intersheet Hydrogen

Bonding," ACS Nano, vol. 6, no. 3, pp. 2008-2019, 2012/02/22 2012, doi:


Y. Liu, B. Xie, Z. Zhang, Q. Zheng, and Z. Xu, "Mechanical properties of graphene papers,"

Journal of the Mechanics and Physics of Solids, vol. 60, no. 4, pp. 591-605, 2012/04 2012, doi:


B. Mohan, G. Freihofer, B. Wirth, and S. Raghavan, "Measuring Tensile Stresses in

CNF/Polymer composites using Raman Spectroscopy," presented at the 52nd

AIAA/ASME/ASCE/AHS/ASC Structures, Structural Dynamics and Materials Conference,

/04/04, 2011. [Online]. Available:

M. S. Dresselhaus, A. Jorio, M. Hofmann, G. Dresselhaus, and R. Saito, "Perspectives on

Carbon Nanotubes and Graphene Raman Spectroscopy," Nano Letters, vol. 10, no. 3, pp. 751-

, 2010/01/19 2010, doi: 10.1021/nl904286r.

M. Yang et al., "Interlayer crosslinking to conquer the stress relaxation of graphene laminated

materials," Materials Horizons, vol. 5, no. 6, pp. 1112-1119, 2018, doi: 10.1039/c8mh00817e.

N. V. Medhekar, A. Ramasubramaniam, R. S. Ruoff, and V. B. Shenoy, "Hydrogen Bond

Networks in Graphene Oxide Composite Paper: Structure and Mechanical Properties," ACS

Nano, vol. 4, no. 4, pp. 2300-2306, 2010/04/09 2010, doi: 10.1021/nn901934u.

E. I. Bîru and H. Iovu, "Graphene Nanocomposites Studied by Raman Spectroscopy," in

Raman Spectroscopy, ed: InTech, 2018.

K. N. Kudin, B. Ozbas, H. C. Schniepp, R. K. Prud'homme, I. A. Aksay, and R. Car, "Raman

Spectra of Graphite Oxide and Functionalized Graphene Sheets," Nano Letters, vol. 8, no. 1,

pp. 36-41, 2007/12/22 2007, doi: 10.1021/nl071822y.

W. Liu and G. Speranza, "Tuning the Oxygen Content of Reduced Graphene Oxide and

Effects on Its Properties," (in eng), ACS Omega, vol. 6, no. 9, pp. 6195-6205, 2021, doi:


N. Ferralis, "Probing mechanical properties of graphene with Raman spectroscopy," Journal of

Materials Science, vol. 45, no. 19, pp. 5135-5149, 2010/06/15 2010, doi: 10.1007/s10853-010-


S. Wan et al., "Sequentially bridged graphene sheets with high strength, toughness, and

electrical conductivity," (in eng), Proc Natl Acad Sci U S A, vol. 115, no. 21, pp. 5359-5364,

, doi: 10.1073/pnas.1719111115.

L. Cao, Q. Sun, H. Wang, X. Zhang, and H. Shi, "Enhanced stress transfer and thermal

properties of polyimide composites with covalent functionalized reduced graphene oxide,"

Composites Part A: Applied Science and Manufacturing, vol. 68, pp. 140-148, 2015/01 2015,

doi: 10.1016/j.compositesa.2014.10.007.


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