Bulk-scale synthesis of randomly stacked graphene with high crystallinity

Zizhao Xu, Shingo Nakamura, Taiki Inoue, Yuta Nishina, Yoshihiro Kobayashi

Research output: Contribution to journalArticlepeer-review

1 Citation (Scopus)


Since the strong interlayer interaction of AB-stacked graphene in bulk form degrades the superior property of single-layer graphene, formation of randomly stacked graphene is required to apply the high performances of graphene to macroscopic devices. However, conventional methods to obtain bulk-scale graphene suffer from a low crystallinity and/or the formation of a thermodynamically stable AB-stacked structure. This study develops a novel approach to produce bulk-scale graphene with a high crystallinity and high fractions of random stacking by utilizing the porous morphology of a graphene oxide sponge and an ultrahigh temperature treatment of 1500–1800 °C with ethanol vapor. Raman spectroscopy indicates that the obtained bulk-scale graphene sponge possesses a high crystallinity and a high fraction of random stacking of 80%. The large difference in the random-stacking ratio between the sponge and the aggregate samples confirms the importance of accessibility of ethanol-derived species into the internal area. By investigating the effect of treatment temperature, a higher random-stacking ratio is obtained at 1500 °C. Moreover, the AB-stacking fraction was reduced to less than 10% by introducing cellulose nanofiber as a spacer to prevent direct stacking of graphene. The proposed method is effective for large-scale production of high-performance bulk-scale graphene.

Original languageEnglish
Pages (from-to)368-375
Number of pages8
Publication statusPublished - Nov 15 2021


  • Bulk-scale graphene
  • Interlayer interaction
  • Reduced graphene oxide
  • Stacking order
  • Thermal reduction

ASJC Scopus subject areas

  • Chemistry(all)
  • Materials Science(all)


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