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 Kim; Alexander A. Balandin; Zonghoon Lee; Rodney S. Ruoff

doi:10.1002/adma.201903039

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

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Abstract

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 language	English
Article number	1903039
Journal	Advanced Materials
Volume	31
Issue number	29
DOIs	https://doi.org/10.1002/adma.201903039
State	Published - Jul 19 2019
Externally published	Yes

Funding

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.

Funders	Funder number
MIST
Spins and Heat in Nanoscale Electronic Systems
UCRF
U.S. Department of Energy	SC0012670
U.S. Department of Energy
National Natural Science Foundation of China	51402291
National Natural Science Foundation of China
Pohang University of Science and Technology
Korea Basic Science Institute
Institute for Basic Science	IBS-R019-D1
Institute for Basic Science

Keywords

graphene
layer-by-layer
mechanical, thermal

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10.1002/adma.201903039

Cite this

Wang, B., Cunning, B. V., Kim, N. Y., Kargar, F., Park, S. Y., Li, Z., Joshi, S. R., Peng, L., Modepalli, V., Chen, X., Shen, Y., Seong, W. K., Kwon, Y., Jang, J., Shi, H., Gao, C., Kim, G. H., Shin, T. J., Kim, K., ... Ruoff, R. S. (2019). Ultrastiff, Strong, and Highly Thermally Conductive Crystalline Graphitic Films with Mixed Stacking Order. Advanced Materials, 31(29), Article 1903039. https://doi.org/10.1002/adma.201903039

@article{d57bdf64630e4803b55bed6dab297d3e,

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

abstract = "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.",

keywords = "graphene, layer-by-layer, mechanical, thermal",

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

note = "Publisher Copyright: {\textcopyright} 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim",

year = "2019",

month = jul,

day = "19",

doi = "10.1002/adma.201903039",

language = "English",

volume = "31",

journal = "Advanced Materials",

issn = "0935-9648",

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Wang, B, Cunning, BV, Kim, NY, Kargar, F, Park, SY, Li, Z, Joshi, SR, Peng, L, Modepalli, V, Chen, X, Shen, Y, Seong, WK, Kwon, Y, Jang, J, Shi, H, Gao, C, Kim, GH, Shin, TJ, Kim, K, Kim, JY, Balandin, AA, Lee, Z & Ruoff, RS 2019, 'Ultrastiff, Strong, and Highly Thermally Conductive Crystalline Graphitic Films with Mixed Stacking Order', Advanced Materials, vol. 31, no. 29, 1903039. https://doi.org/10.1002/adma.201903039

TY - JOUR

T1 - Ultrastiff, Strong, and Highly Thermally Conductive Crystalline Graphitic Films with Mixed Stacking Order

AU - Wang, Bin

AU - Cunning, Benjamin V.

AU - Kim, Na Yeon

AU - Kargar, Fariborz

AU - Park, Sun Young

AU - Li, Zhancheng

AU - Joshi, Shalik R.

AU - Peng, Li

AU - Modepalli, Vijayakumar

AU - Chen, Xianjue

AU - Shen, Yongtao

AU - Seong, Won Kyung

AU - Kwon, Youngwoo

AU - Jang, Jeongsu

AU - Shi, Haofei

AU - Gao, Chao

AU - Kim, Gun Ho

AU - Shin, Tae Joo

AU - Kim, Kwanpyo

AU - Kim, Ju Young

AU - Balandin, Alexander A.

AU - Lee, Zonghoon

AU - Ruoff, Rodney S.

PY - 2019/7/19

Y1 - 2019/7/19

N2 - 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.

AB - 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.

KW - graphene

KW - layer-by-layer

KW - mechanical, thermal

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U2 - 10.1002/adma.201903039

DO - 10.1002/adma.201903039

M3 - Article

C2 - 31155773

AN - SCOPUS:85066996083

SN - 0935-9648

VL - 31

JO - Advanced Materials

JF - Advanced Materials

IS - 29

M1 - 1903039

ER -

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

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