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With the rapid development of wearable and portable electronic devices, it is increasingly important to develop conductive paper-like films (CPFs) with the characteristics of light, thin and self-supporting. In this paper, nanofibrillated cellulose (NFC) was used as reinforcing phase of film-forming to combine with graphene oxide (GO). Then graphene-based CPFs were prepared by directly reducing the GO/NFC composite film without any additional adhesives, which effectively avoided the difficulties of dispersion and combination with other materials caused by direct using of high content graphene. Meanwhile, three representative reduction methods for direct reduction of GO/NFC composite films were also compared. The results show that 450 °C thermal reduction and hydroiodic acid reduction were more effective than ascorbic acid reduction. On this basis, hydroiodic acid reduction and thermal reduction were used to discuss the effect of NFC addition to the conductivity of the film. This occured when increasing the content of NFC from 10% to 50%, the electrical conductivity of the composite film by hydroiodic acid reduction decreased from 153.8 S/m to 22.2 S/m. While the conductivity of composite film increased first and then decreased after thermal reduction both at 450 °C and 550 °C. What’s more, when NFC content was about 16.6% the electrical conductivity reached a high level which was 86.21 S/m and 168.9 S/m, respectively. This study provides a groundwork for the further development of graphene-based CPFs with low square resistance and high conductivity in large-scale preparation.

Direct Reduction of Graphene Oxide/Nanofibrillated Cellulose Composite Film and its Electrical Conductivity Research