Abstract
Thermal management is significant to maintain the reliability and durability of electronic devices. Heat can be dissipated using thermal interface materials (TIMs) comprised of thermally conductive polymers and fillers. Furthermore, it is important to enhance the thermal conductivity of TIMs through the formation of a heat transfer pathway. This paper reports a polymer composite containing vertically aligned electrochemically exfoliated graphite (EEG). We modify the EEG via edge selective oxidation to decorate the surface with iron oxides and enhance the dispersibility of EEG in polymer resin. During the heat treatment and curing process, a magnetic field is applied to the polymer composites to align the iron oxide decorated EEG. The resulting polymer composite containing 25 wt% of filler has a remarkable thermal conductivity of 1.10 W m−1 K−1 after magnetic orientation. These results demonstrate that TIM can be designed with a small amount of filler by magnetic alignment to form an efficient heat transfer pathway.
![](http://media.springernature.com/m312/springer-static/image/art%3A10.1007%2Fs42823-022-00378-y/MediaObjects/42823_2022_378_Fig1_HTML.png)
![](http://media.springernature.com/m312/springer-static/image/art%3A10.1007%2Fs42823-022-00378-y/MediaObjects/42823_2022_378_Fig2_HTML.png)
![](http://media.springernature.com/m312/springer-static/image/art%3A10.1007%2Fs42823-022-00378-y/MediaObjects/42823_2022_378_Fig3_HTML.png)
![](http://media.springernature.com/m312/springer-static/image/art%3A10.1007%2Fs42823-022-00378-y/MediaObjects/42823_2022_378_Fig4_HTML.png)
![](http://media.springernature.com/m312/springer-static/image/art%3A10.1007%2Fs42823-022-00378-y/MediaObjects/42823_2022_378_Fig5_HTML.png)
References
Suh D, Moon CM, Kim D, Baik S (2016) Ultrahigh thermal conductivity of interface materials by silver-functionalized carbon nanotube phonon conduits. Adv Mater 28(33):7220–7227
Xu S, Zhang J (2020) Vertically aligned graphene for thermal interface materials. Small Struct 1(3):2000034
Ci H, Chang H, Wang R, Wei T, Wang Y, Chen Z, Sun Y, Dou Z, Liu Z, Li J, Gao P, Liu Z (2019) Enhancement of heat dissipation in ultraviolet light-emitting diodes by a vertically oriented graphene nanowall buffer layer. Adv Mater 31(29):1901624
Dai W, Lv L, Lu J, Hou H, Yan Q, Alam FE, Li Y, Zeng X, Yu J, Wei Q, Xu X, Wu J, Jiang N, Du S, Sun R, Xu J, Wong C, Lin C-T (2019) A paper-like inorganic thermal interface material composed of hierarchically structured graphene/silicon carbide nanorods. ACS Nano 13(2):1547–1554
Huang S, Zhao J, Gong L, Duan X (2017) Thermal performance and structure optimization for slotted microchannel heat sink. Appl Therm Eng 115:1266–1276
Qi C, Hu J, Liu M, Guo L, Rao Z (2017) Experimental study on thermo-hydraulic performances of CPU cooled by nanofluids. Energy Convers Manag 153:557–565
Razeeb KM, Dalton E, Cross GLW, Robinson AJ (2018) Present and future thermal interface materials for electronic devices. Int Mater Rev 63(1):1–21
**a G, Cao L, Bi G (2017) A review on battery thermal management in electric vehicle application. J Power Sources 367:90–105
Yan Q, Alam FE, Gao J, Dai W, Tan X, Lv L, Wang J, Zhang H, Chen D, Nishimura K, Wang L, Yu J, Lu J, Sun R, **ang R, Maruyama S, Zhang H, Wu S, Jiang N, Lin C-T (2021) Soft and self-adhesive thermal interface materials based on vertically aligned, covalently bonded graphene nanowalls for efficient microelectronic cooling. Adv Funct Mater 31(36):2104062
Dai W, Ma T, Yan Q, Gao J, Tan X, Lv L, Hou H, Wei Q, Yu J, Wu J, Yao Y, Du S, Sun R, Jiang N, Wang Y, Kong J, Wong C, Maruyama S, Lin C-T (2019) Metal-level thermally conductive yet soft graphene thermal interface materials. ACS Nano 13(10):11561–11571
Hansson J, Nilsson TM, Ye L, Liu J (2018) Novel nanostructured thermal interface materials: a review. Int Mater Rev 63(1):22–45
Kang D-G, Ko H, Koo J, Lim S-I, Kim JS, Yu Y-T, Lee C-R, Kim N, Jeong K-U (2018) Anisotropic thermal interface materials: directional heat transfer in uniaxially oriented liquid crystal networks. ACS Appl Mater Interfaces 10(41):35557–35562
Ebrahimi H, Roghani-Mamaqani H, Salami-Kalajahi M, Shahi S, Abdollahi A (2020) Chemical incorporation of epoxy-modified graphene oxide into epoxy/novolac matrix for the improvement of thermal characteristics. Carbon Lett 30(1):13–22
Oh Y, Kang JS, Kang CS, Kwon KC, Lee GW (2020) Investigation of mechanical, thermal and electrical properties of hybrid composites reinforced with multi-walled carbon nanotubes and fused silica particles. Carbon Lett 30(4):353–365
Balandin AA, Ghosh S, Bao W, Calizo I, Teweldebrhan D, Miao F, Lau CN (2008) Superior thermal conductivity of single-layer graphene. Nano Lett 8(3):902–907
Chung S-H, Kim H, Jeong SW (2018) Improved thermal conductivity of carbon-based thermal interface materials by high-magnetic-field alignment. Carbon 140:24–29
Chen H, Ginzburg VV, Yang J, Yang Y, Liu W, Huang Y, Du L, Chen B (2016) Thermal conductivity of polymer-based composites: Fundamentals and applications. Prog Polym Sci 59:41–85
Zhang F, Feng Y, Feng W (2020) Three-dimensional interconnected networks for thermally conductive polymer composites: design, preparation, properties, and mechanisms. Mater Sci Eng R: Rep 142:100580
Chen J, Huang X, Sun B, Wang Y, Zhu Y, Jiang P (2017) Vertically aligned and interconnected boron nitride nanosheets for advanced flexible nanocomposite thermal interface materials. ACS Appl Mater Interfaces 9(36):30909–30917
Kong Q, Bodelot L, Lebental B, Lim YD, Shiau LL, Gusarov B, Tan CW, Liang K, Lu C, Tan CS, Coquet P, Tay BK (2018) Novel three-dimensional carbon nanotube networks as high performance thermal interface materials. Carbon 132:359–369
Ma J, Shang T, Ren L, Yao Y, Zhang T, **e J, Zhang B, Zeng X, Sun R, Xu J-B, Wong C-P (2020) Through-plane assembly of carbon fibers into 3D skeleton achieving enhanced thermal conductivity of a thermal interface material. Chem Eng J 380:122550
Kwon YJ, Kwon Y, Park HS, Lee JU (2019) Mass-produced electrochemically exfoliated graphene for ultrahigh thermally conductive paper using a multimetal electrode system. Adv Mater Interfaces 6(9):1900095
Park J, Kim YS, Sung SJ, Kim T, Park CR (2017) Highly dispersible edge-selectively oxidized graphene with improved electrical performance. Nanoscale 9(4):1699–1708
Park JH, Oh YJ, Park DY, Lee J, Park JS, Park CR, Kim JH, Kim T, Yang SJ (2021) A new class of carbon nanostructures for high-performance electro-magnetic and-chemical barriers. Adv Sci 8(22):2102718
Park JS, Han YB, So SH, Kim J, Ryu JH, Choi J, Park DH, Park CR, Kim JH, Yang SJ (2022) Concentration-driven polymorphic mesocrystal and morphosynthetic transformation toward omni-adsorbent with the widest range of pores. Chem Eng J 433:133871
Shin G-J, Rhee K, Park S-J (2016) Improvement of CO2 capture by graphite oxide in presence of polyethylenimine. Int J Hydrog Energy 41(32):14351–14359
Kang W-S, Rhee KY, Park S-J (2016) Thermal, impact and toughness behaviors of expanded graphite/graphite oxide-filled epoxy composites. Compos B Eng 94:238–244
Dam B, Jamatia R, Gupta A, Pal AK (2017) Metal-free greener syntheses of pyrimidine derivatives using a highly efficient and reusable graphite oxide carbocatalyst under solvent-free reaction conditions. ACS Sustain Chem Eng 5(12):11459–11469
Wang L, Liu F, Shao W, Cui S, Zhao Y, Zhou Y, He J (2019) Graphite oxide do** polyimide nanofiber membrane via electrospinning for high performance lithium-ion batteries. Compos Commun 16:150–157
Agostini M, Brutti S, Hassoun J (2016) High voltage Li-ion battery using exfoliated graphite/graphene nanosheets anode. ACS Appl Mater Interfaces 8(17):10850–10857
Shin MC, Kim JH, Nam S, Oh YJ, ** HJ, Park CR, Zhang Q, Yang SJ (2020) Atomic-distributed coordination state of metal-phenolic compounds enabled low temperature graphitization for high-performance multioriented graphite anode. Small 16(33):2003104
Oh YJ, Park JH, Park JS, Kim SS, Hong SJ, Na YW, Kim JH, Nam SH, Yang SJ (2022) Fast-chargeable N-doped multi-oriented graphitic carbon as a Li-intercalation compound. Energy Storage Mater 44:416–424
Lee MH, Kim HY, Kim J, Han JT, Lee Y-S, Woo JS (2020) Influence of oxyfluorinated graphite on fluorinated ethylene–propylene composites as bipolar plates. Carbon Lett 30(3):345–352
Na YW, Cheon JY, Kim JH, Jung Y, Lee K, Park JS, Park JY, Song KS, Lee SB, Kim T, Yang SJ (2022) All-in-one flexible supercapacitor with ultrastable performance under extreme load. Sci Adv 8(1):eabl8631
Hu J, Liang C, Li J, Liang Y, Li S, Li G, Wang Z, Dong D (2021) Flexible reduced graphene oxide@ Fe3O4/silicone rubber composites for enhanced microwave absorption. Appl Surf Sci 570:151270
Jiang S, Qian K, Yu K, Zhou H, Weng Y, Zhang Z (2020) Controllable synthesis and microwave absorption properties of Fe3O4@ f-GNPs nanocomposites. Compos Commun 20:100363
Zhao Q, Liu J, Wang Y, Tian W, Liu J, Zang J, Ning H, Yang C, Wu M (2018) Novel in-situ redox synthesis of Fe3O4/rGO composites with superior electrochemical performance for lithium-ion batteries. Electrochim Acta 262:233–240
Kim KH, Han J-I, Kang D-H, Lee Y-S (2018) Improved heat-spreading properties of fluorinated graphite/epoxy film. Carbon Lett 28:96–99
Xu B, Mao N, Zhao Y, Tong L, Zhang J (2021) Polarized Raman spectroscopy for determining crystallographic orientation of low-dimensional materials. J Phys Chem Lett 12(31):7442–7452
Yan H, Wang R, Li Y, Long W (2015) Thermal conductivity of magnetically aligned graphene–polymer composites with Fe3O4-decorated graphene nanosheets. J Electron Mater 44(2):658–666
Huang L, Zhu P, Li G, Lu DD, Sun R, Wong C (2014) Core–shell SiO2@RGO hybrids for epoxy composites with low percolation threshold and enhanced thermo-mechanical properties. J Mater Chem 2(43):18246–18255
Lin Z, Liu Y, Raghavan S, Moon K-s, Sitaraman SK, Wong C-p (2013) Magnetic alignment of hexagonal boron nitride platelets in polymer matrix: toward high performance anisotropic polymer composites for electronic encapsulation. ACS Appl Mater Interfaces 5(15):7633–7640
Mao D, Chen J, Ren L, Zhang K, Yuen MM, Zeng X, Sun R, Xu J-B, Wong C-P (2019) Spherical core-shell Al@Al2O3 filled epoxy resin composites as high-performance thermal interface materials. Compos A Appl Sci Manuf 123:260–269
Min C, Yu D, Cao J, Wang G, Feng L (2013) A graphite nanoplatelet/epoxy composite with high dielectric constant and high thermal conductivity. Carbon 55:116–125
Wang X, Wu P (2018) Melamine foam-supported 3D interconnected boron nitride nanosheets network encapsulated in epoxy to achieve significant thermal conductivity enhancement at an ultralow filler loading. Chem Eng J 348:723–731
Yang F, Sun X, Guo Q, Yao Z (2019) Improvement of thermal conductivities for epoxy composites via incorporating poly (vinyl benzal)-coated h-BN fillers and solvent-assisted dispersion. Ind Eng Chem Res 58(40):18635–18643
Acknowledgements
This work was supported by Inha University Research Grant (65427).
Author information
Authors and Affiliations
Corresponding authors
Ethics declarations
Conflict of interest
The authors declare that there is no conflict of interest.
Additional information
Publisher's Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Supplementary Information
Below is the link to the electronic supplementary material.
Rights and permissions
About this article
Cite this article
Ryu, J.H., Yang, S.M., Lee, J.U. et al. Magnetic alignment of electrochemically exfoliated graphite in epoxy as a thermal interface material with high through-plane thermal conductivity. Carbon Lett. 32, 1433–1439 (2022). https://doi.org/10.1007/s42823-022-00378-y
Received:
Revised:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s42823-022-00378-y