Ultrastiff, Strong, and Highly Thermally Conductive Crystalline Graphitic Films with Mixed Stacking Order

Bin Wang, Benjamin V. Cunning, Na Yeon Kim, Fariborz Kargar, Sun Young Park, Zhancheng Li, Shalik R. Joshi, Li Peng, Vijayakumar Modepalli, Xianjue Chen, Yongtao Shen, Won Kyung Seong, Youngwoo Kwon, Jeongsu Jang, Haofei Shi, Chao Gao, Gun Ho Kim, Tae Joo Shin, Kwanpyo Kim, Ju Young KimAlexander A. Balandin, Zonghoon Lee, Rodney S. Ruoff

Research output: Contribution to journalArticlepeer-review

38 Citations (Scopus)


A macroscopic film (2.5 cm × 2.5 cm) made by layer-by-layer assembly of 100 single-layer polycrystalline graphene films is reported. The graphene layers are transferred and stacked one by one using a wet process that leads to layer defects and interstitial contamination. Heat-treatment of the sample up to 2800 °C results in the removal of interstitial contaminants and the healing of graphene layer defects. The resulting stacked graphene sample is a freestanding film with near-perfect in-plane crystallinity but a mixed stacking order through the thickness, which separates it from all existing carbon materials. Macroscale tensile tests yields maximum values of 62 GPa for the Young's modulus and 0.70 GPa for the fracture strength, significantly higher than has been reported for any other macroscale carbon films; microscale tensile tests yield maximum values of 290 GPa for the Young's modulus and 5.8 GPa for the fracture strength. The measured in-plane thermal conductivity is exceptionally high, 2292 ± 159 W m−1 K−1 while in-plane electrical conductivity is 2.2 × 105 S m−1. The high performance of these films is attributed to the combination of the high in-plane crystalline order and unique stacking configuration through the thickness.

Original languageEnglish
Article number1903039
JournalAdvanced Materials
Issue number29
Publication statusPublished - 2019 Jul 19

Bibliographical note

Funding Information:
The authors appreciate comments by Peter Thrower, Revathi Bacsa, and Leonard Interrante. This work was supported by the Institute for Basic Science (IBS-R019-D1). Z.L. and H.S. acknowledge financial support from the National Natural Science Foundation of China (No.51402291). A.A.B. and F.K. acknowledge support from the Spins and Heat in Nanoscale Electronic Systems (SHINES) Center funded by the U.S. Department of Energy under Award # SC0012670. Experiments at PLS-II 6D UNIST-PAL beamline were supported in part by MIST, POSTECH, and UCRF. R.S.R. supervised the project. B.W., B.V.C., and R.S.R. conceived the experiments. B.W., V.M., and Y.S. prepared the stacked graphene samples. B.W., B.V.C., L.P., C.G., and X.C. contributed to the heat treatment of the samples. W.K.S., B.V.C., V.M., and Y.K. put efforts into the heating systems design. T.J.S. helped with the synchrotron GIWAXS measurement and analysis. N.Y.K. and Z.L. performed TEM analysis. S.-Y.P. and J.-Y.K. contributed to the mechanical measurement and analysis. J.J. and K.K. measured the electrical resistance of the materials. F.K. and A.A.B. analyzed the thermal conductivity data with assistance from S.R.K and G.-H.K. Z.L., and H.S. provided the monolayer graphene film samples. B.W., B.V.C., and R.S.R. wrote the manuscript. All co-authors revised and commented on the manuscript.

Publisher Copyright:
© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

All Science Journal Classification (ASJC) codes

  • Materials Science(all)
  • Mechanics of Materials
  • Mechanical Engineering


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