• [Review]
  • Thermal Conductivity of CNT Composites Based on Hybrid Fillers

  • Inhye Shin , Jaeik Kim*, Sunwoo Kim*, and Won-Gyu Bae*,†

  • Department of Chemical Engineering, Soongsil University, Dongjak-gu 06978, Korea
    *Department of Electrical Engineering, Soongsil University, Dongjak-gu 06978, Korea

  • CNT 복합재를 기반으로 하는 하이브리드 필러의 열전도 특성

  • 신인혜 · 김재익* · 김선우* · 배원규*,†

  • 숭실대학교 화학공학과, *숭실대학교 전기공학부

  • Reproduction, stored in a retrieval system, or transmitted in any form of any part of this publication is permitted only by written permission from the Polymer Society of Korea.

References
  • 1. Lee Sanchez, W. A.; Li, J.-W.; Chiu, H.-T.; Cheng, C.-C.; Chiou, K.-C.; Lee, T.-M.; Chiu, C.-W. Highly Thermally Conductive Epoxy Composites with AlN/BN Hybrid Filler as Underfill Encapsulation Material for Electronic Packaging. Polymers 2022, 14, 2950.
  •  
  • 2. Rubel, R. I.; Ali, M. H.; Jafor, M. A.; Alam, M. M. Carbon Nanotubes Agglomeration in Reinforced Composites: A Review. AIMS Mater. Sci. 2019, 6, 756-780.
  •  
  • 3. Dyachkova, T. P.; Khan, Y. A.; Burakova, E. A.; Galunin, E. V.; Shigabaeva, G. N.; Stolbov, D. N.; Titov, G. A.; Chapaksov, N. A.; Tkachev, A. G. Characteristics of Epoxy Composites Containing Carbon Nanotubes/Graphene Mixtures. Polymers 2023, 15, 1476.
  •  
  • 4. Liu, B.; Sun, J.; Zhao, J.; Yun, X. Hybrid Graphene and Carbon Nanotube–reinforced Composites: Polymer, Metal, and Ceramic Matrices. Adv. Compos. Hybrid Mater. 2025, 8, 1.
  •  
  • 5. Lee, D.-K.; Yoo, J.; Kim, H.; Kang, B.-H.; Park, S.-H. Electrical and Thermal Properties of Carbon Nanotube Polymer Composites with Various Aspect Ratios. Materials 2022, 15, 1356.
  •  
  • 6. Tamayo-Vegas, S.; Muhsan, A.; Liu, C.; Tarfaoui, M.; Lafdi, K. The Effect of Agglomeration on the Electrical and Mechanical Properties of Polymer Matrix Nanocomposites Reinforced with Carbon Nanotubes. Polymers 2022, 14, 1842.
  •  
  • 7. Bera, S.; Singh, M.; Thantirige, R.; Tiwary, S. K.; Shook, B. T.; Nieves, E.; Raghavan, D.; Karim, A.; Pradhan, N. R. 2D-Nanofiller-Based Polymer Nanocomposites for Capacitive Energy Storage Applications. Small Sci. 2023, 3, 2300016.
  •  
  • 8. Jeevan Jyoti, B.; Singh, B. P. A Review on 3D Graphene–carbon Nanotube Hybrid Polymer Nanocomposites. J. Mater. Sci. 2021, 56, 17411-17456.
  •  
  • 9. Sanusi, O. M.; Jaafar, M. Development of Hybrid Fillers/Polymer Nanocomposites for Electronic Applications. In Hybrid Nanomaterials; Srivastava, S. K., Ed.; Wiley-Blackwell: Hoboken, NJ, USA, 2018; pp 349-369.
  •  
  • 10. Wang, J.; Wang, G. Nanocarbon-Based Hybrid Fillers in Thermally Conductive Polymer Composites: A Review. Adv. Eng. Mater. 2024, 26, 2301983.
  •  
  • 11. Aparna, A.; Sethulekshmi, A. S.; Jayan, J. S.; Joseph, K. Recent Advances in Boron Nitride Based Hybrid Polymer Nanocomposites. Mater. Adv. 2021.
  •  
  • 12. Guo, Y.; Cao, C.; Luo, F.; Huang, B.; Xiao, L.; Qian, Q.; Chen, Q. Largely Enhanced Thermal Conductivity and Thermal Stability of Ultra High Molecular Weight Polyethylene Composites via BN/CNT Synergy. RSC Adv. 2019, 9, 40800-40809.
  •  
  • 13. Gao, Y.; Luo, J.; Li, Z.; Teng, F.; Zhang, J.; Gao, S.; Ma, M.; Zhou, X.; Tao, X. Dispersion of Carbon Nanotubes in Aqueous Cementitious Materials: A Review. Nanotechnology Rev. 2023, 12, 20220560.
  •  
  • 14. Rennhofer, H.; Zanghellini, B. Dispersion State and Damage of Carbon Nanotubes and Carbon Nanofibers by Ultrasonic Dispersion: AReview. Nanomaterials 2021, 11, 1469.
  •  
  • 15. Yu, L.; Lin, Y.; Li, L.; Zong, H.; Zhou, Y.; Zhao, S.; Zhang, Z.; Grobert, N.; Maciejewska, B. M.; Qin, L. Understanding Interfacial Dynamics: Hydrostatic Pressure-Induced Sono-Dispersion of Carbon Nanotubes. Surfaces and Interfaces 2024, 51, 104740.
  •  
  • 16. Choi, Y. J.; Nacpil, E. J. C.; Han, J.; Zhu, C.; Kim, I. S.; Jeon, I. Recent Advances in Dispersant Technology for Carbon Nanotubes toward Energy Device Applications. Adv. Energy Sustain. Res. 2024, 5, 2300219.
  •  
  • 17. Benko, A.; Duch, J.; Gajewska, M.; Marzec, M.; Bernasik, A.; Nocuń, M.; Piskorz, W.; Kotarba, A. Covalently Bonded Surface Functional Groups on Carbon Nanotubes: From Molecular Modeling to Practical Applications. Nanoscale 2021, 13, 10152-10166.
  •  
  • 18. Jouni, M.; Fedorko, P.; Celle, C.; Djurado, D.; Chenevier, P.; Faure-Vincent, J. Conductivity vs Functionalization in Single-Walled Carbon Nanotube Films. SN Appl. Sci. 2022, 4, 132.
  •  
  • 19. Alosime, E. M. A Review on Surface Functionalization of Carbon Nanotubes: Methods and Applications. Discover Nano 2023, 18, 12.
  •  
  • 20. Zhao, X.; Ding, C.; Wang, S.; Song, C. Ageing Regulates the Migration of Carbon Nanotubes in Saturated Quartz Sand. J. Environ. Chem. Eng. 2024, 12, 112267.
  •  
  • 21. Fernandes, R. M. F.; Buzaglo, M.; Regev, O.; Furó, I.; Marques, E. F. Mechanical Agitation Induces Counterintuitive Aggregation of Pre-Dispersed Carbon Nanotubes. J. Colloid Interface Sci. 2017, 493, 398-404.
  •  
  • 22. Xiao, Y.-J.; Wang, W.-Y.; Chen, X.-J.; Lin, T.; Zhang, Y.-T.; Yang, J.-H.; Wang, Y.; Zhou, Z.-W. Hybrid Network Structure and Thermal Conductive Properties in Poly(vinylidene fluoride) Composites Based on Carbon Nanotubes and Graphene Nanoplatelets. Compos. Part A Appl. Sci. Manuf. 2016, 90, 614-625.
  •  
  • 23. Sun, Y.; Xu, H.; Zhao, Z.; Zhang, L.; Ma, L.; Zhao, G.; Song, G.; Li, X. Investigation of Carbon Nanotube Grafted Graphene Oxide Hybrid Aerogel for Polystyrene Composites with Reinforced Mechanical Performance. Polymers 2021, 13, 735.
  •  
  • 24. Stoyanova, S.; Ivanov, E.; Hegde, L. R.; Georgopoulou, A.; Clemens, F.; Bedoui, F.; Kotsilkova, R. PVDFHybrid Nanocomposites with Graphene and Carbon Nanotubes and Their Thermoresistive and Joule Heating Properties. Nanomaterials 2024, 14, 901.
  •  
  • 25. Long, R.; Liu, Y.; Tao, J.; Zhang, H.; Liu, Y.; Bao, R.; Li, F.; Li, C.; Yi, J. Synergistic Influence of Carbon Nanotube–Graphene Oxide Hybrid and Nanosized Interfacial TiC on the Mechanical Performance of Cu Matrix Composites. J. Mater. Res. Technol. 2023, 25, 2866-2879.
  •  
  • 26. González-Martínez, J. R.; López-Oyama, A. B.; Del Ángel-López, D.; García-Guendulain, C.; Rodríguez González, E.; Pulido-Barragan, E. U.; Barffuson-Domínguez, F.; Magallanes Vallejo, A. G.; Mogica-Cantú, P. J. Influence of Reduced Graphene Oxide and Carbon Nanotubes on the Structural, Electrical, and Photoluminescent Properties of Chitosan Films. Polymers 2024, 16, 1827.
  •  
  • 27. Chen, H.; Chen, N.; Ma, Q.; He, Y. Experimental Study on Preparation and Properties of Carbon Nanotubes-, Graphene–Natural Rubber Composites. J. Thermoplast. Compos. Mater. 2024, 37, 112-118.
  •  
  • 28. Ke, K.; Sang, Z.; Chen, X.; Rohm, K.; Manas-Zloczower, I. Tuning Mechanical and Electrical Properties of Elastomer Composite with Hybrid Network via Graphene for Stretchable Strain Sensors. Adv. Eng. Mater. 2022, 24, 2100703.
  •  
  • 29. Singh, B.; Han, J.; Meziani, M.J.; Cao, L.; Yerra, S.; Collins, J.; Dumra, S.; Sun, Y.-P. Polymeric Nanocomposites of Boron Nitride Nanosheets for Enhanced Directional or Isotropic Thermal Transport Performance. Nanomaterials 2024, 14, 1259.
  •  
  • 30. Zhang, Y.; Wang, S.; Wu, H.; Guo, S. Constructing Heterostructured MWCNT-BN Hybrid Fillers in Electrospun TPU Films to Achieve Superior Thermal Conductivity and Electrical Insulation Properties. Polymers 2024, 16, 2139.
  •  
  • 31. Zhang, X.; Tan, W.; Carey, T.; Wen, B.; He, D.; Arbab, A.; Groombridge, A.; Smail, F.; de La Verpilliere, J.; Yao, C.; Wang, Y.; Wei, X.; Liu, H.; Xie, S.; Torrisi, F.; De Volder, M.; Zhou, W.; Boies, A. Enhanced Composite Thermal Conductivity by Percolated Networks of In-Situ Confined-Grown Carbon Nanotubes. Nano Res. 2023, 16, 12821-12829.
  •  
  • 32. Zhang, T.; Xu, H.; Dai, C.; Zhang, C.; Zhang, Y.; Chi, Q. Carbon Nanotubes and Hexagonal Boron Nitride Nanosheets Co‐filled Ethylene Propylene Diene Monomer Composites: Improved Electrical Property for Cable Accessory Applications. High Voltage, 2024, 9, 546-555.
  •  
  • 33. Almansoori, A.; Balázsi, K.; Balázsi, C. Advances, Challenges, and Applications of Graphene and Carbon Nanotube-Reinforced Engineering Ceramics. Nanomaterials 2024, 14, 1881.
  •  
  • 34. Hughes, K. J.; Iyer, K. A.; Bird, R. E.; Ivanov, J.; Banerjee, S.; Georges, G.; Zhou, Q. A. Review of Carbon Nanotube Research and Development: Materials and Emerging Applications. ACS Appl. Nano Mater. 2024, 7, 18695-18713.
  •  
  • 35. Kochetov, R.; Andritsch, T.; Lafont, U.; Morshuis, P. H. F.; Picken, S. J.; Smit, J. J. Preparation and Dielectric Properties of Epoxy - BN and Epoxy - AlN Nanocomposites. 2009 IEEE Electrical Insulation Conference, Montreal, QC, Canada, 2009, 31, May-03, June, pp. 397-400.
  •  
  • 36. Matsumoto, N.; Futaba, D. N.; Yamada, T.; Kokubo, K. Enhancing the Thermal Conductivity of CNT/AlN/Silicone Rubber Composites by Using CNTs Directly Grown onAlNtoAchieve a Reduced Filler Filling Ratio. Nanomaterials 2024, 14, 528.
  •  
  • 37. Ji, P.; Lu, X. Microstructure and Thermal Conductivity of Nano-Carbon/AlN Composites. Diamond Relat. Mater. 2021, 121, 108710.
  •  
  • 38. Gao, J.; Xiong, H.; Han, X.; An, F.; Chen, T. Synergistic Effect of Aluminum Nitride and Carbon Nanotube-Reinforced Silicon Rubber Nanocomposites. Molecules 2024, 29, 2864.
  •  
  • 39. Zhang, X. S.; Yang, L. W.; Liu, H. T.; Zu, M. A Novel High-content CNT-reinforced SiC Matrix Composite-fiber by Precursor Infiltration and Pyrolysis Process. RSC Advances, 2017, 7, 23334-23341.
  •  
  • 40. Tang, C.; Zhang, S.; Zhang, J.; Zhang, X.; Hang, Z.; Li, Y.; Yang, Z. Silicon Carbide Coated Carbon Nanotube Porous Sponge with Super Elasticity, Low Density, High Thermal Resistivity, and Synergistically Enhanced Electromagnetic Interference Shielding Performances. Chem. Eng. J. 2023, 469, 144011.
  •  
  • 41. Yoo, S. C.; Kang, B.; Trinh, P. V.; Phuong, D. D.; Hong, S. H. Enhanced Mechanical and Wear Properties of Al6061 Alloy Nanocomposite Reinforced by CNT-Template-Grown Core–Shell CNT/SiC Nanotubes. Sci. Rep. 2020, 10, 12896.
  •  
  • 42. Ghosh, P.; Ramajeyathilagam, K. Experimental and Numerical Investigations on the Effect of MWCNT-COOHandAl2O3 Hybrid Nanofillers Dispersed CFRP Laminates Subjected to Projectile Impact. Processes 2023, 11, 1435.
  •  
  • 43. Akter, J.; Hanif, M. A.; Islam, M. A.; Sapkota, K. P.; Hahn, J. R. Selective Growth of Ti3+/TiO2/CNT and Ti3+/TiO2/Carbon Nanocomposites for Enhanced Visible-Light Utilization to Degrade Organic Pollutants by Lowering TiO2 Bandgap. Sci. Rep. 2021, 11, 9490.
  •  
  • 44. Wan, L.; Deng, C.; Zhao, Z.-Y.; Zhao, H.-B.; Wang, Y.-Z. A Titanium Dioxide–Carbon Nanotube Hybrid to Simultaneously Achieve the Mechanical Enhancement of Natural Rubber and Its Stability under Extreme Frictional Conditions. Mater. Adv. 2021, 2, 2408-2418.
  •  
  • 45. Niu, C.; Zhang, Q.; Cheng, L.; Ye, F.; Zhang, L.; Huang, M.; Yang, T. Enhanced Thermal Conductivity and Mechanical Properties of 2D Cf/SiC Composites Modified by In-Situ Grown Carbon Nanotubes. J. Adv. Ceram. 2024, 13, 19-33.
  •  
  • 46. Li, K.; McGuire, M.; Lupini, A.; Skolrood, L.; List, F.; Ozpineci, B.; Ozcan, S.; Aytug, T. Copper−Carbon Nanotube Composites Enabled by Electrospinning for Advanced Conductors. ACS Appl. Nano Mater. 2020, 3, 6863-6875.
  •  
  • 47. Gholami-Kermanshahi, M.; Hsiao, Y.-C.; Lange, G.; Chang, S.-H. Effects of Carbon Nanotube Addition on the Microstructures, Martensitic Transformation, and Internal Friction of Cu–Al–Ni Shape-Memory Alloys. Sci. Rep. 2023, 13, 21181.
  •  
  • 48. Wang, D.; Yan, A.; Liu, Y.; Wu, Z.; Gan, X.; Li, F.; Tao, J.; Li, C.; Yi, J. Interfacial Bonding Improvement through Nickel Decoration on Carbon Nanotubes in Carbon Nanotubes/Cu Composite Foams Reinforced Copper Matrix Composites. Nanomaterials 2022, 12, 2548.
  •  
  • 49. Isacfranklin, M.; Rathinam, Y.; Ganesan, R.; Velauthapillai, D. Direct Growth of Binder-Free CNTs on a Nickel Foam Substrate for Highly Efficient Symmetric Supercapacitors. ACS Omega 2023, 8, 11700-11708.
  •  
  • 50. Wu, Z.; Dong, J.; Teng, C.; Li, X.; Zhao, X.; Qin, X.; Ji, C.; Zhang, Q. Polyimide-Based Composites Reinforced by Carbon Nanotube-Grafted Carbon Fiber for Improved Thermal Conductivity and Mechanical Property. Compos. Commun. 2023, 39, 101543.
  •  
  • 51. Wang, C.; Cong, B.; Zhao, J.; Zhao, X.; Wang, D.; Zhou, H.; Chen, C. In Situ Synthesis of MWCNT-Graft-Polyimides: Thermal Stability, Mechanical Property, and Thermal Conductivity. RSC Adv. 2020, 10, 13517-13524.
  •  
  • 52. Lu, C.; Lin, F.; Shao, H.; Bi, S.; Chen, N.; Shao, G.; Jiang, J. Carboxylated Carbon Nanotube/Polyimide Films with LowThermal Expansion Coefficient and Excellent Mechanical Properties. Polymers 2022, 14, 4565.
  •  
  • 53. Yan, Y.; Zhang, B.; Wang, J.; Cao, C.; Yan, F. MWCNT–Polyimide Fiber-Reinforced Composite for High-Temperature Tribological Applications. Coatings 2024, 14, 181.
  •  
  • 54. Cao, J.; Yang, S.; Liao, Y.; Wang, Y.; He, J.; Xiong, C.; Shi, K.; Hu, X. Evaluation of Polyetheretherketone Composites Modified by Calcium Silicate and Carbon Nanotubes for Bone Regeneration: Mechanical Properties, Biomineralization, and Induction of Osteoblasts. Front. Bioeng. Biotechnol. 2023, 11, 1271140.
  •  
  • 55. Silva, S.; Barbosa, J.M.; Sousa, J.D.; Paiva, M.C.; Teixeira, P.F. High-Performance PEEK/MWCNT Nanocomposites: Combining Enhanced Electrical Conductivity and Nanotube Dispersion. Polymers 2024, 16, 583.
  •  
  • 56. Ye, X.; Hu, Z.; Li, X.; Wang, S.; Wang, B.; Zhao, Y.; He, J.; Liu, J.; Zhang, J. Effect of Annealing and Carbon Nanotube Infill on the Mechanical and Electrical Properties of Additively Manufactured Polyether-Ether-Ketone Nanocomposites via Fused Filament Fabrication. Addit. Manuf. 2022, 59, 103188.
  •  
  • 57. Lee Sanchez, W.A.; Huang, C.-Y.; Chen, J.-X.; Soong, Y.-C.; Chan, Y.-N.; Chiou, K.-C.; Lee, T.-M.; Cheng, C.-C.; Chiu, C.-W. Enhanced Thermal Conductivity of Epoxy Composites Filled with Al2O3/Boron Nitride Hybrids for Underfill Encapsulation Materials. Polymers 2021, 13, 147.
  •  
  • 58. Mohanraman, R.; Steiner, P.; Kocabas, C.; Kinloch, I. A.; Bissett, M. A. Synergistic Improvement in the Thermal Conductivity of Hybrid Boron Nitride Nanotube/Nanosheet Epoxy Composites. ACS Appl. Nano Mater. 2024, 7, 13142-13146.
  •  
  • 59. He, X.; Feng, L.; Zhang, Z.; Hou, X.; Ye, X.; Song, Q.; Yang, Y.; Suo, G.; Zhang, L.; Fu, Q.-G.; Li, H. High-Performance Multifunctional Carbon–Silicon Carbide Composites with Strengthened Reduced Graphene Oxide. ACS Nano 2021, 15, 2880-2892.
  •  
  • 60. Zhou, T.; Wang, X.; Liu, X.; Xiong, D. Improved Thermal Conductivity of Epoxy Composites Using a Hybrid Multi-walled Carbon Nanotube/micro-SiC Filler. Carbon 2010, 48, 1171-1176.
  •  
  • 61. Chai, G.; Chen, Q. Characterization Study of the Thermal Conductivity of Carbon Nanotube Copper Nanocomposites. J. Compos. Mater. 2010, 44, 2863-2873.
  •  
  • 62. Yamanaka, S.; Gonda, R.; Kawasaki, A.; Sakamoto, H.; Mekuchi, Y.; Kuno, M.; Tsukada, T. Fabrication and Thermal Properties of Carbon Nanotube/nickel Composite by Spark Plasma Sintering Method. Mater. Trans. 2007, 48, 2506-2512.
  •  
  • 63. Seki, Y.; Tokgöz, M. M.; Öner, F.; Sarikanat, M.; Altay, L. Carbon Nanotube-, Boron Nitride-, and Graphite-Filled Polyketone Composites for Thermal Energy Management. ACS Omega 2023, 8, 19265-19272.
  •  
  • 64. Wang, Y.; Li, Z.; Liu, Y.; Pei, P. Dynamic Thermo-Mechanical Properties of Carbon Nanotube Resin Composite Films. Polymers 2024, 16, 3307.
  •  
  • Polymer(Korea) 폴리머
  • Frequency : Bimonthly(odd)
    ISSN 2234-8077(Online)
    Abbr. Polym. Korea
  • 2024 Impact Factor : 0.6
  • Indexed in SCIE

This Article

  • 2026; 50(3): 374-382

    Published online May 25, 2026

  • 10.7317/pk.2026.50.3.374
  • Received on Nov 18, 2025
  • Revised on Apr 6, 2026
  • Accepted on Apr 6, 2026

Correspondence to

  • Won-Gyu Bae

  • *Department of Electrical Engineering, Soongsil University, Dongjak-gu 06978, Korea

  • E-mail: wgbae@ssu.ac.kr