Thermal conductivity properties of the graphene-carbon nanotube hybrid / Al2O3 interface

M.M. Slepchenkov

, O.E. Glukhova

, A.A. Petrunin show affiliations and emails

Received 23 April 2025; Accepted 11 May 2025;

Citation: M.M. Slepchenkov, O.E. Glukhova, A.A. Petrunin. Thermal conductivity properties of the graphene-carbon nanotube hybrid / Al2O3 interface. Lett. Mater., 2025, 15(2) 127-133

BibTex https://doi.org/10.48612/letters/2025-2-127-133

Abstract

The thermal conductivity properties of the graphene-nanotube film/Al2O3 interface are investigated using the molecular dynamics method. Both films and nanoparticles of Al2O3 are considered.

A pressing task of modern materials science is the creation of interfaces based on carbon nanostructures and metal oxides for subsequent use in nanoelectronic and spintronic devices. One of the central problems in the operation of nanoelectronic devices is the problem of heat removal, which imposes serious requirements on the thermal conductivity of carbon / metal oxide interfaces. This paper investigates the thermal conductivity properties of the graphene-nanotube hybrid / metal oxide interface. A quasi-2D nanomaterial in the form of a seamless junction of graphene and vertically oriented single-walled carbon nanotubes (SWCNTs) with chirality indices (16, 0) is considered as a graphene-nanotube hybrid. Thin films (2D) and nanoparticles (0D) of aluminum oxide Al2O3 are considered as a metal oxide. The self-consistent-charge density-functional tight-binding method (SCC-DFTB) is used to identify the equilibrium configurations of the supercells of the graphene-nanotube hybrid / 2D-Al2O3 and graphene-nanotube hybrid / 0D-Al2O3 interfaces, characterized by a minimum value of the total energy. Using the molecular dynamics (MD) method with the empirical force field ReaxFF, we established the patterns of the influence of Al2O3 on the thermal conductivity properties of the graphene-SWCNT (16, 0) hybrid nanomaterial. It is shown that the thermal conductivity of the graphene-SWCNT (16,0) / 2D-Al2O3 and SWCNT (16, 0) / 0D-Al2O3 interfaces at a temperature of 300 K exceeds the thermal conductivity of the graphene-SWCNT (16, 0) hybrid by several orders of magnitude. The thermal conductivity coefficient of both graphene-nanotube hybrid / Al2O3 interfaces decreases by ≈6 times with an increase in temperature from 100 to 600 K. At the same time, it remains an order of magnitude higher compared to the carbon material graphene-SWCNT (16, 0). The results obtained open up broad prospects for the use of graphene-SWCNT / Al2O3 nanomaterials as thermal interfaces in nanoelectronic devices.

References (46)

1. V. Georgakilas, J. A. Perman, J. Tucek, R. Zboril, Broad Family of Carbon Nanoallotropes: Classification, Chemistry, and Applications of Fullerenes, Carbon Dots, Nanotubes, Graphene, Nanodiamonds, and Combined Superstructures, Chem. Rev. 115 (2015) 4744 - 4822

2. O. S. Ayanda, A. O. Mmuoegbulam, O. Okezie, N. I. Durumin Iya, S. E. Mohammed, P. H. James, A. B. Muhammad, A. A. Unimke, S. A. Alim, S. M. Yahaya, A. Ojo, T. O. Adaramoye, S. K. Ekundayo, A. Abdullahi, H. Badamasi, Recent progress in carbon-based nanomaterials: critical review, J. Nanopart. Res. 26 (2024) 106

3. D. Jariwala, V. K. Sangwan, L. J. Lauhon, T. J. Marks, M. C. Hersam, Carbon nanomaterials for electronics, optoelectronics, photovoltaics, and sensing, Chem. Soc. Rev. 42 (2013) 2824 - 2860

4. R. Atif, F. Inam, Reasons and remedies for the agglomeration of multilayered graphene and carbon nanotubes in polymers, Beilstein J. Nanotechnol. 7 (2016) 1174 -1196

5. P. N. Nirmalraj, P. E. Lyons, S. De, J. N. Coleman, J. J. Boland, Electrical connectivity in single-walled carbon nanotube networks, Nano Lett. 9 (2009) 3890 - 3895

6. S. Nardecchia, D. Carriazo, M. C. Gutiérrez, M. L. Ferrer, F. del Monte, Three dimensional macroporous architectures and aerogels built of carbon nanotubes and / or graphene: synthesis and applications, Chem. Soc. Rev. 42 (2013) 794 - 830

7. C.-Y. Lin, Z. Zhao, J. Niu, Z. Xia, Synthesis, Properties and Applications of 3D Carbon Nanotube − Graphene Junctions, J. Phys. D Appl. Phys. 49 (2016) 443001

8. E. Yoo, J. Kim, E. Hosono, H. S. Zhou, T. Kudo, I. Honma, Large reversible Li storage of graphene nanosheet families for use in rechargeable lithium ion batteries, Nano Lett. 8 (2008) 2277 - 2282

9. J. P. John, T. E. Mary Nancy, T. K. Bindu Sharmila, A comprehensive review on the environmental applications of graphene-carbon nanotube hybrids: recent progress, challenges and prospects, Mater. Adv. 2 (2021) 6816 - 6838

10. A. Gbaguidi, S. Namilae, D. Kim, Synergy effect in hybrid nanocomposites based on carbon nanotubes and graphene nanoplatelets, Nanotechnology 31 (2020) 255704

11. X. Zhao, L. Qiu, D. Kong, Y. Huang, J. Liu, Effects of Three-Dimensional Graphene-Carbon Nanotube Hybrid on the Mechanical Properties and Microstructure of Cement Paste, Materials 16 (2023) 6571

12. M. R. Zakaria, M. F. Omar, M. S. Zainol Abidin, H. Md Akil, M. M. A. B. Abdullah, Recent progress in the three-dimensional structure of graphene-carbon nanotubes hybrid and their supercapacitor and high-performance battery applications, Compos. - A: Appl. Sci. Manuf. 154 (2022) 106756

13. A. B. Felix, M. Pacheco, P. Orellana, A. Latgé, Vertical and In-Plane Electronic Transport of Graphene Nanoribbon / Nanotube Heterostructures, Nanomaterials 12 (2022) 3475

14. M. M. Slepchenkov, P. V. Barkov, D. A. Kolosov, O. E. Glukhova, Ab Initio Study of Optical Properties of Hybrid Films Based on Bilayer Graphene and Single-Walled Carbon Nanotubes, C 9 (2023) 51

15. S. Pyo, Y. Eun, J. Sim, K. Kim, J. Choi, Carbon nanotube-graphene hybrids for soft electronics, sensors, and actuators, Micro Nano Syst. Lett. 10 (2022) 9

16. S. C. Qin, Y. D. Liu, H. Z. Jiang, Y. Xu, Y. Shi, R. Zhang, F. Wang, All-carbon hybrids for high-performance electronics, optoelectronics and energy storage, Sci. China Inf. Sci. 62 (2019) 220403

17. B. Liu, J. Sun, J. Zhao, X. Yun, Hybrid graphene and carbon nanotube-reinforced composites: polymer, metal, and ceramic matrices, Adv. Compos. Hybrid Mater. 8 (2025) 1

18. X. Wu, F. Mu, H. Zhao, Recent progress in the synthesis of graphene / CNT composites and the energy-related applications, J. Mater. Sci. Technol. 55 (2020) 16 - 34

19. W. Du, Z. Ahmed, Q. Wang, C. Yu, Z. Feng, G. Li, M. Zhang, C. Zhou, R. Senegor, C. Y. Yang, Structures, properties, and applications of CNT-graphene heterostructures, 2D Mater. 6 (2019) 042005

20. J. Sheng, Z. Han, G. Jia, S. Zhu, Y. Xu, X. Zhang, Y. Yao, Y. Li, Covalently Bonded Graphene Sheets on Carbon Nanotubes: Direct Growth and Outstanding Properties, Adv. Funct. Mater. 33 (2023) 2306785

21. V. T. Dang, D. D. Nguyen, T. T. Cao, P. H. Le, D. L. Tran, N. M. Phan, V. C. Nguyen, Recent trends in preparation and application of carbon nanotube − graphene hybrid thin films, Adv. Nat. Sci.: Nanosci. Nanotechnol. 7 (2016) 033002

22. L. Cai, X. Xue, M. Liu, H. Li, X. Zhou, G. Yu, One-step synthesis of seamless graphene-carbon nanotube heterojunctions by chemical vapor deposition, APL Mater. 9 (2021) 041110

23. Z. Li, Z. H. Li, Y. Zhang, X. Xu, Y. Cheng, Y. Zhang, J. Zhao, N. Wei, Highly Sensitive Weaving Sensor of Hybrid Graphene Nanoribbons and Carbon Nanotubes for Enhanced Pressure Sensing Function, ACS Sens. 9 (2024) 2499 - 2508

24. Y. Li, Q. Ai, L. Mao, T. Gong, Y. Lin, G. Wu, W. Huang, X. Zhang, Hybrid strategy of graphene / carbon nanotube hierarchical networks for highly sensitive, flexible wearable strain sensors, Sci Rep 11 (2021) 21006

25. Z. Hong, Z. Zheng, L. Kong, L. Zhao, S. Liu, W. Li, J. Shi, Welded Carbon Nanotube − Graphene Hybrids with Tunable Strain Sensing Behavior for Wide-Range Bio-Signal Monitoring, Polymers 16 (2024) 238

26. T. Xu, J. Jiang, On the Configuration of Graphene / Carbon Nanotube / Graphene Van der Waals Heterostructure, Phys. Chem. Chem. Phys. 25 (2023) 5066 - 5072

27. M. Gao, Z. L. Huang, B. Zeng, T. S. Pan, Y. Zhang, H. B. Peng, Y. Lin, Carbon nanotube-graphene junctions studied by impedance spectra, Appl. Phys. Lett. 106 (2015) 051601

28. M. Lan, X. Jia, R. Tian, L. Feng, D. Shao, H. Song, Advancing multifunctional thermal management with multistate graphene / CNTs conjugated hybrids, Carbon 219 (2024) 118850

29. K. Xiong, C. Ma, J. Wang, X. Ge, W. Qiao, L. Ling, Highly thermal conductive graphene / carbon nanotubes films with controllable thickness as thermal management materials, Ceram. Int. 49 (2023) 8847 - 8855

30. Y. Jiang, S. Song, M. Mi, L. Yu, L. Xu, P. Jiang, Y. Wang, Improved Electrical and Thermal Conductivities of Graphene − Carbon Nanotube Composite Film as an Advanced Thermal Interface Material, Energies 16 (2023) 1378

31. Z. Wang, J. Li, K. Yuan, Molecular dynamics simulation of thermal boundary conductance between horizontally aligned carbon nanotube and graphene, Int. J. Therm. Sci. 132 (2018) 589 - 596

32. V. Panneerselvam, S. P. Sathian, Thermal transport in a defective pillared graphene network: insights from equilibrium molecular dynamics simulation, Phys. Chem. Chem. Phys. 26 (2024) 10650 - 10659

33. B. Hourahine, B. Aradi, V. Blum, F. Bonafé, A. Buccheri, C. Camacho, C. Cevallos, M. Y. Deshaye, T. Dumitrică, A. Dominguez, S. Ehlert, M. Elstner, T. van der Heide, J. Hermann, S. Irle, J. J. Kranz, C. Köhler, T. Kowalczyk, T. Kubař, I. S. Lee, V. Lutsker, R. J. Maurer, S. K. Min, I. Mitchell, C. Negre, T. A. Niehaus, A. M. N. Niklasson, A. J. Page, A. Pecchia, G. Penazzi, M. P. Persson, J. Řezáč, C. G. Sánchez, M. Sternberg, M. Stöhr, F. Stuckenberg, A. Tkatchenko, V. W. Z. Yu, T. Frauenheim, DFTB+, a software package for efficient approximate density functional theory based atomistic simulations, J. Chem. Phys. 152 (2020) 124101

34. F. Spiegelman, N. Tarrat, J. Cuny, L. Dontot, E. Posenitskiy, C. Martí, A. Simon, M. Rapacioli, Density-functional tight-binding: basic concepts and applications to molecules and clusters, Adv. Phys.: X 5 (2020) 1710252

35. DFTB+. Available online: https://dftbplus.org/ (accessed on 1 February 2024).

36. G. Zhang, O. E. Glukhova, New automatic method for generating atomistic models of multi-branched and arbitrary-shaped seamless junctions of carbon nanostructures, Comput. Mater. Sci. 184 (2020) 109943

37. LAMMPS Molecular Dynamics Simulator. Available online: https://www.lammps.org/ (accessed on 21 January 2025).

38. A. Van Duin, S. Dasgupta, F. Lorant, W. A. Goddard III, ReaxFF: A reactive force field for hydrocarbons, J. Phys. Chem. A 105 (2001) 9396 - 9409

39. S. Hong, A. C. Van Duin, Atomistic-scale analysis of carbon coating and its effect on the oxidation of aluminum nanoparticles by ReaxFF-molecular dynamics simulations, J. Phys. Chem. C 120 (2016) 9464 - 9474

40. D. Frenkel, B. Smit, Understanding Molecular Simulation. From Algorithms to Applications, Academic Press, New York, 2023, 728 p.

41. M. S. Green, Markoff random processes and the statistical mechanics of time‐dependent phenomena. II. Irreversible processes in fluids, J. Chem. Phys. 22 (1954) 398 - 413

42. R. Kubo, Statistical-mechanical theory of irreversible processes. I. General theory and simple applications to magnetic and conduction problems, J. Phys. Soc. Jpn. 12 (1957) 570 - 586

43. A. A. Balandin, S. Ghosh, W. Bao, I. Calizo, D. Teweldebrhan, F. Miao, C. N. Lau, Superior thermal conductivity of single-layer graphene, Nano Lett. 8 (2008) 902 - 907

44. J. H. Zou, Z. Q. Ye, B. Y. Cao, Phonon thermal properties of graphene from molecular dynamics using different potentials, J. Chem. Phys. 145 (2016) 134705

45. L. Cui, X. Du, G. Wei, Y. Feng, Thermal conductivity of graphene wrinkles: a molecular dynamics simulation, J. Phys. Chem. C 120 (2016) 23807 - 23812

46. P. K. Schelling, S. R. Phillpot, P. Keblinski, Comparison of atomic-level simulation methods for computing thermal conductivity, Phys. Rev. B 65 (2001) 144306

Funding

1. Russian Science Foundation - 24-79-10316