Three-Dimensional Highly Thermally Conductive Graphene Blocks by Multiscale Blending and Multistage Pressure Induction

Liyu Zhang , Haitao Hu , Xuan Li , Haihan Xu , Xiaoying Gao , Ruishi Lin , Yingze Meng , Jiaxin He , Shoujin Chang , Guoliang Ding

Carbon Energy ›› 2026, Vol. 8 ›› Issue (6) : e70210

PDF (6919KB)
Carbon Energy ›› 2026, Vol. 8 ›› Issue (6) :e70210 DOI: 10.1002/cey2.70210
RESEARCH ARTICLE
Three-Dimensional Highly Thermally Conductive Graphene Blocks by Multiscale Blending and Multistage Pressure Induction
Author information +
History +
PDF (6919KB)

Abstract

The thermal conductivity of graphene materials rapidly decreases with the increase of thickness, seriously hindering its application potential in high heat flow scenarios. Here, a novel strategy for synthesizing expandable-thickness graphene block (GPB) with high thermal conductivity is proposed via multiscale blending and multistage pressure induction (MBP). The reduction of the in-plane thermal conductivity with the increase of thickness of the proposed GPB-MBP is lowered by more than 94% compared to existing graphene materials, and the maximum thickness of GPB-MBP reaches 12.1 mm, which is more than 10 times that of the existing graphene materials. Compared with the thickest existing graphene material of 1.05 mm, the in-plane thermal conductivity and cross-plane thermal conductivity of GPB-MBP are 4.7–7.4 times and 6.2–6.6 times higher, respectively. The maximum thermal diffusion ability of GPB-MBP reaches 6.3 W/K, which is 8–53 times higher than that of existing graphene materials. Furthermore, the proportional relationship between in-plane thermal conductivity and the logarithm of length was discovered on macroscopic graphene materials for the first time. The new strategy for synthesizing expandable-thickness GPB offers a new approach for high-heat-flux thermal management.

Cite this article

Download citation ▾
Liyu Zhang, Haitao Hu, Xuan Li, Haihan Xu, Xiaoying Gao, Ruishi Lin, Yingze Meng, Jiaxin He, Shoujin Chang, Guoliang Ding. Three-Dimensional Highly Thermally Conductive Graphene Blocks by Multiscale Blending and Multistage Pressure Induction. Carbon Energy, 2026, 8 (6) : e70210 DOI:10.1002/cey2.70210

登录浏览全文

4963

注册一个新账户 忘记密码

References

[1]

F. Lin, Z. Zhu, X. Zhou, et al., “Orientation Control of Graphene Flakes by Magnetic Field: Broad Device Applications of Macroscopically Aligned Graphene,” Advanced Materials 29, no. 1 (2017): 1604453.

[2]

G. Xin, T. Yao, H. Sun, et al., “Highly Thermally Conductive and Mechanically Strong Graphene Fibers,” Science 349, no. 6252 (2015): 1083–1087.

[3]

J. Yang, M. Li, S. Fang, et al., “Water-Induced Strong Isotropic Mxene-Bridged Graphene Sheets for Electrochemical Energy Storage,” Science 383, no. 6684 (2024): 771–777.

[4]

X. Li, Z. Tao, B. Hao, et al., “Reduced Graphene Oxide Bubbles With Tunable Electromagnetic Shielding Effectiveness,” Scripta Materialia 187 (2020): 407–412.

[5]

A. A. Balandin, S. Ghosh, W. Bao, et al., “Superior Thermal Conductivity of Single-Layer Graphene,” Nano Letters 8, no. 3 (2008): 902–907.

[6]

R. Yan, X. Wo, X. Yu, et al., “A Secondary Molding Process for Achieving Increased Thickness in High Thermal Conductivity Graphene Films,” Materials Today Chemistry 38 (2024): 102116.

[7]

T.-W. Pan, W.-S. Kuo, and N.-H. Tai, “Tailoring Anisotropic Thermal Properties of Reduced Graphene Oxide/Multi-Walled Carbon Nanotube Hybrid Composite Films,” Composites Science and Technology 151 (2017): 44–51.

[8]

T. Wu, Y. Xu, H. Wang, Z. Sun, and L. Zou, “Efficient and Inexpensive Preparation of Graphene Laminated Film With Ultrahigh Thermal Conductivity,” Carbon 171 (2021): 639–645.

[9]

H. Jia, Q.-Q. Kong, X. Yang, et al., “Dual-Functional Graphene/Carbon Nanotubes Thick Film: Bidirectional Thermal Dissipation and Electromagnetic Shielding,” Carbon 171 (2021): 329–340.

[10]

Y. Kaburagi, T. Kimura, A. Yoshida, and Y. Hishiyama, “Thermal and Electrical Conductivity and Magnetoresistance of Graphite Films Prepared From Aromatic Polyimide Films,” Tanso 2012, no. 253 (2012): 106–115.

[11]

C. Teng, D. Xie, J. Wang, Z. Yang, G. Ren, and Y. Zhu, “Ultrahigh Conductive Graphene Paper Based on Ball-Milling Exfoliated Graphene,” Advanced Functional Materials 27, no. 20 (2017): 1700240.

[12]

Q. Q. Kong, Z. Liu, J. G. Gao, et al., “Hierarchical Graphene–Carbon Fiber Composite Paper as a Flexible Lateral Heat Spreader,” Advanced Functional Materials 24, no. 27 (2014): 4222–4228.

[13]

A. Akbari, B. V. Cunning, S. R. Joshi, et al., “Highly Ordered and Dense Thermally Conductive Graphitic Films From a Graphene Oxide/Reduced Graphene Oxide Mixture,” Matter 2, no. 5 (2020): 1198–1206.

[14]

X. Meng, H. Pan, C. Zhu, et al., “Coupled Chiral Structure in Graphene-Based Film for Ultrahigh Thermal Conductivity in Both In-Plane and Through-Plane Directions,” ACS Applied Materials & Interfaces 10, no. 26 (2018): 22611–22622.

[15]

H. Lu, J. Zhang, J. Luo, et al., “Enhanced Thermal Conductivity of Free-Standing 3D Hierarchical Carbon Nanotube-Graphene Hybrid Paper,” Composites, Part A: Applied Science and Manufacturing 102 (2017): 1–8.

[16]

X. Li, M. Fang, W. Wang, et al., “Graphene Heat Dissipation Film for Thermal Management of Hot Spot in Electronic Device,” Journal of Materials Science: Materials in Electronics 27, no. 7 (2016): 7715–7721.

[17]

Y. Liu, M. Zhang, Q. Huang, et al., “Vertical Graphene on Graphene Composite Film for Heat Dissipation and Electromagnetic Shielding,” ACS Applied Nano Materials 7, no. 5 (2024): 5074–5084.

[18]

S. Cui, F. Jiang, N. Song, L. Shi, and P. Ding, “Flexible Films for Smart Thermal Management: Influence of Structure Construction of a Two-Dimensional Graphene Network on Active Heat Dissipation Response Behavior,” ACS Applied Materials & Interfaces 11, no. 33 (2019): 30352–30359.

[19]

R. Chein and G. Huang, “Thermoelectric Cooler Application in Electronic Cooling,” Applied Thermal Engineering 24, no. 14 (2004): 2207–2217.

[20]

L. Peng, Z. Xu, Z. Liu, Y. Guo, P. Li, and C. Gao, “Ultrahigh Thermal Conductive Yet Superflexible Graphene Films,” Advanced Materials 29, no. 27 (2017): 1700589.

[21]

G. Xin, H. Sun, T. Hu, et al., “Large-Area Freestanding Graphene Paper for Superior Thermal Management,” Advanced Materials 26, no. 26 (2014): 4521–4526.

[22]

S. Yang, Z. Tao, Q. Kong, et al., “Preparation of Graphitic Foil With High Thermal Conductivity Using Vitamin C as Reductant and Binder,” Chemical Engineering Journal 473 (2023): 145330.

[23]

Y. Hao, X. Ming, J. Lu, et al., “Bidirectionally High-Thermally Conductive and Environmentally Adaptive Graphene Thick Films Enabled by Seamless Bonding Assembly for Extreme Thermal Management,” Advanced Functional Materials 34 (2024): 2400110.

[24]

S. Chen, Q. Wang, M. Zhang, et al., “Scalable Production of Thick Graphene Film for Next Generation Thermal Management Application,” Carbon 167 (2020): 270–277.

[25]

Z. Pan, Y. Wu, H. Yuan, et al., “Ascorbic Acid-Assisted Defect Healing and Stack Ordering of Graphene Films Towards High Power Thermal Dispersion,” Carbon 182 (2021): 799–805.

[26]

X. Zhang, Y. Guo, Y. Liu, et al., “Ultrathick and Highly Thermally Conductive Graphene Films by Self-Fusion,” Carbon 167 (2020): 249–255.

[27]

H. Zheng, P. He, S. Yang, et al., “Achieving Ultra-High Heat Flux Transfer in Graphene Films via Tunable Gas Escape Channels,” Advanced Science 12 (2025): 2410913.

[28]

M. Shtein, R. Nadiv, M. Buzaglo, K. Kahil, and O. Regev, “Thermally Conductive Graphene–Polymer Composites: Size, Percolation, and Synergy Effects,” Chemistry of Materials 27, no. 6 (2015): 2100–2106.

[29]

A. Yousefzadi Nobakht and S. Shin, “Anisotropic Control of Thermal Transport in Graphene/Si Heterostructures,” Journal of Applied Physics 120, no. 22 (2016): 225111.

[30]

M. Bahri, S. H. Gebre, M. A. Elaguech, et al., “Recent Advances in Chemical Vapour Deposition Techniques for Graphene-Based Nanoarchitectures: From Synthesis to Contemporary Applications,” Coordination Chemistry Reviews 475 (2023): 214910.

[31]

B. Deng, Z. Liu, and H. Peng, “Toward Mass Production of CVD Graphene Films,” Advanced Materials 31, no. 9 (2019): 1800996.

[32]

S. N. Alam, N. Sharma, and L. Kumar, “Synthesis of Graphene Oxide (GO) by Modified Hummers Method and Its Thermal Reduction to Obtain Reduced Graphene Oxide (rGO),” Graphene 06, no. 1 (2017): 1–18.

[33]

M. S. Eluyemi, M. A. Eleruja, A. V. Adedeji, et al., “Synthesis and Characterization of Graphene Oxide and Reduced Graphene Oxide Thin Films Deposited by Spray Pyrolysis Method,” Graphene 5, no. 3 (2016): 143–154.

[34]

M. G. Sumdani, M. R. Islam, A. N. A. Yahaya, and S. I. Safie, “Recent Advances of the Graphite Exfoliation Processes and Structural Modification of Graphene: A Review,” Journal of Nanoparticle Research 23 (2021): 253.

[35]

C. Knieke, A. Berger, M. Voigt, R. N. K. Taylor, J. Röhrl, and W. Peukert, “Scalable Production of Graphene Sheets by Mechanical Delamination,” Carbon 48, no. 11 (2010): 3196–3204.

[36]

S. D. Silva-Santos, R. S. Alencar, A. L. Aguiar, et al., “From High Pressure Radial Collapse to Graphene Ribbon Formation in Triple-Wall Carbon Nanotubes,” Carbon 141 (2019): 568–579.

[37]

C. Chen, Y. Lin, W. Zhou, et al., “Sub-10-nm Graphene Nanoribbons With Atomically Smooth Edges From Squashed Carbon Nanotubes,” Nature Electronics 4, no. 9 (2021): 653–663.

[38]

E. Tatarova, A. Dias, J. Henriques, et al., “Microwave Plasmas Applied for the Synthesis of Free Standing Graphene Sheets,” Journal of Physics D: Applied Physics 47, no. 38 (2014): 385501.

[39]

A. Dato, “Graphene Synthesized in Atmospheric Plasmas—A Review,” Journal of Materials Research 34, no. 1 (2019): 214–230.

[40]

J. Sun, Y. Chen, M. K. Priydarshi, et al., “Direct Chemical Vapor Deposition-Derived Graphene Glasses Targeting Wide Ranged Applications,” Nano Letters 15, no. 9 (2015): 5846–5854.

[41]

Y. Chen, J. Sun, J. Gao, et al., “Growing Uniform Graphene Disks and Films on Molten Glass for Heating Devices and Cell Culture,” Advanced Materials 27, no. 47 (2015): 7839–7846.

[42]

H. Feng, R. Cheng, X. Zhao, X. Duan, and J. Li, “A Low-Temperature Method to Produce Highly Reduced Graphene Oxide,” Nature Communications 4, no. 1 (2013): 1539.

[43]

D. Voiry, J. Yang, J. Kupferberg, et al., “High-Quality Graphene via Microwave Reduction of Solution-Exfoliated Graphene Oxide,” Science 353, no. 6306 (2016): 1413–1416.

[44]

Y. Xie, P. Yuan, T. Wang, N. Hashemi, and X. Wang, “Switch on the High Thermal Conductivity of Graphene Paper,” Nanoscale 8, no. 40 (2016): 17581–17597.

[45]

L. Wang, B. Hu, and B. Li, “Logarithmic Divergent Thermal Conductivity in Two-Dimensional Nonlinear Lattices,” Physical Review E 86, no. 4 (2012): 040101.

[46]

O. Narayan and S. Ramaswamy, “Anomalous Heat Conduction in One-Dimensional Momentum-Conserving Systems,” Physical Review Letters 89, no. 20 (2002): 200601.

[47]

L. F. C. Pereira and D. Donadio, “Divergence of the Thermal Conductivity in Uniaxially Strained Graphene,” Physical Review B 87, no. 12 (2013): 125424.

[48]

N. Bonini, J. Garg, and N. Marzari, “Acoustic Phonon Lifetimes and Thermal Transport in Free-Standing and Strained Graphene,” Nano Letters 12, no. 6 (2012): 2673–2678.

[49]

W. J. Evans, L. Hu, and P. Keblinski, “Thermal Conductivity of Graphene Ribbons From Equilibrium Molecular Dynamics: Effect of Ribbon Width, Edge Roughness, and Hydrogen Termination,” Applied Physics Letters 96, no. 20 (2010): 3435465.

[50]

S. Lepri, “Thermal Conduction in Classical Low-Dimensional Lattices,” Physics Reports 377, no. 1 (2003): 1–80.

[51]

I. A. Starkov and A. S. Starkov, “Maxwell–Garnett Model for Thermoelectric Materials,” International Journal of Solids and Structures 202 (2020): 226–233.

[52]

I. L. Skryabin, A. V. Radchik, P. Moses, and G. B. Smith, “The Consistent Application of Maxwell–Garnett Effective Medium Theory to Anisotropic Composites,” Applied Physics Letters 70, no. 17 (1997): 2221–2223.

[53]

Y. Guo and M. Wang, “Heat Transport in Two-Dimensional Materials by Directly Solving the Phonon Boltzmann Equation Under Callaway's Dual Relaxation Model,” Physical Review B 96, no. 13 (2017): 134312.

[54]

D. L. Nika and A. A. Balandin, “Two-Dimensional Phonon Transport in Graphene,” Journal of Physics: Condensed Matter 24, no. 23 (2012): 233203.

[55]

J. Chen, B. Liu, and X. Gao, “Thermal Properties of Graphene-Based Polymer Composite Materials: A Molecular Dynamics Study,” Results in Physics 16 (2020): 102974.

[56]

C. Liu, P. Lu, W. Chen, Y. Zhao, and Y. Chen, “Phonon Transport in Graphene Based Materials,” Physical Chemistry Chemical Physics 23, no. 46 (2021): 26030–26060.

[57]

N. Wang, M. K. Samani, H. Li, et al., “Tailoring the Thermal and Mechanical Properties of Graphene Film by Structural Engineering,” Small 14, no. 29 (2018): 1801346.

[58]

A. Akbari, B. V. Cunning, S. R. Joshi, et al., “Highly Ordered and Dense Thermally Conductive Graphitic Films From a Graphene Oxide/Reduced Graphene Oxide Mixture,” Matter 2, no. 5 (2020): 1198–1206.

[59]

Q. Liang, X. Yao, W. Wang, Y. Liu, and C. P. Wong, “A Three-Dimensional Vertically Aligned Functionalized Multilayer Graphene Architecture: An Approach for Graphene-Based Thermal Interfacial Materials,” ACS Nano 5, no. 3 (2011): 2392–2401.

Rights & permissions

2026 The Author(s). Carbon Energy published by Wenzhou University and John Wiley & Sons Australia, Ltd.

PDF (6919KB)

0

Accesses

0

Citation

Detail

Sections
Recommended

/

〈 〉