Abstract
Silicone rubber (SR) composites are most widely used as thermal interface materials (TIMs) for electronics heat dissipation. Thermal impedance as the main bottleneck limiting the performance of TIMs is usually neglected. Herein, the thermal impedance of SR composites loaded with different levels of hexagonal boron nitride (h-BN) as TIMs was elaborated for the first time by the ASTM D 5470 standard test and finite element analysis. It was found that elastic modulus and surface roughness of SR composites increased with the increase of h-BN content, indicating that the conformity was reduced. When the assembly pressure was 0.69 MPa, there existed an optimal h-BN content at which the contact resistance was minimum (0.39 K·cm2·W−1). Although the decreased bond line thickness (BLT) by increasing the assembly pressure was beneficial to reduce the thermal impedance, the proper assembly pressure should be selected to prevent the warpage of the contact surfaces and the increase in contact resistance, according to the compression properties of the SR composites. This study provides valuable insights into fabrication of high-performance TIMs for modern electronic device applications.
Similar content being viewed by others
References
Razeeb, K. M.; Dalton, E.; Cross, G. L. W.; Robinson, A. J. Present and future thermal interface materials for electronic devices. Int. Mater. Rev. 2018, 63, 1–21.
Swamy, M. C. K.; Satyanarayan. A review of the performance and characterization of conventional and promising thermal interface materials for electronic package applications. J. Electron. Mater. 2019, 48, 7623–7634.
Zhao, Y.; Zeng, X.; Ren, L.; Xia, X.; Zeng, X.; Zhou, J. Heat conduction of electrons and phonons in thermal interface materials. Mater. Chem. Front. 2021, 5, 5617–5638.
Li, J.; Liu, X.; Feng, Y.; Yin, J. Recent progress in polymer/two-dimensional nanosheets composites with novel performances. Prog. Polym. Sci. 2022, 126, 101505.
Huang, T.; Yang, F.; Wang, T.; Wang, J.; Li, Y.; Huang, J.; Chen, M.; Wu, L. Ladder- structured boron nitride nanosheet skeleton in flexible polymer films for superior thermal conductivity. Appl. Mater. Today 2022, 26, 101299.
Niu, H.; Guo, H.; Ren, Y.; Ren, L.; Lv, R.; Kang, L.; Bashir, A.; Bai, S. Spherical aggregated BN/AlN filled silicone composites with enhanced through-plane thermal conductivity assisted by vortex flow. Chem. Eng. J. 2022, 430, 133155.
Zhao, N.; Li, J.; Wang, W.; Gao, W.; Bai, H. Isotropically ultrahigh thermal conductive polymer composites by assembling anisotropic boron nitride nanosheets into a biaxially oriented network. ACS Nano 2022, 16, 18959–18967.
Song, H.; Liu, J.; Liu, B.; Wu, J.; Cheng, H. M.; Kang, F. Two-dimensional materials for thermal management applications. Joule 2018, 2, 442–463.
Chaudhry, A. U.; Mabrouk, A. N.; Abdala, A. Thermally enhanced polyolefin composites: fundamentals, progress, challenges, and prospects. Sci. Technol. Adv. Mater. 2020, 21, 737–766.
Zhang, R.; Liu, Z.; Sun, Z.; He, X.; Lin, Q.; Xiang, Y.; Fang, X.; Li, S.; Fu, X.; Liu, Q.; Hu, S.; Ping Wong, C. A scalable highly thermal conductive silicone rubber composite with orientated graphite by pre-vulcanizing and multilayer stacking method. Compos. Part A: Appl. Sci. Manuf. 2022, 157, 106944.
Hu, Q.; Bai, X.; Zhang, C.; Zeng, X.; Huang, Z.; Li, J.; Li, J.; Zhang, Y. Oriented BN/silicone rubber composite thermal interface materials with high out-of-plane thermal conductivity and flexibility. Compos. Part A: Appl. Sci. Manuf. 2022, 152, 106681.
Yin, Z.; Guo, J.; Jiang, X. Significantly improved thermal conductivity of silicone rubber and aligned boron nitride composites by a novel roll-cutting processing method. Compos. Sci. Technol. 2021, 209, 108794.
Feng, C. P.; Wan, S. S.; Wu, W. C.; Bai, L.; Bao, R. Y.; Liu, Z. Y.; Yang, M. B.; Chen, J.; Yang, W. Electrically insulating, layer structured SiR/GNPs/BN thermal management materials with enhanced thermal conductivity and breakdown voltage. Compos. Sci. Technol. 2018, 167, 456–462.
Xue, Y.; Li, X.; Wang, H.; Zhao, F.; Zhang, D.; Chen, Y. Improvement in thermal conductivity of through-plane aligned boron nitride/silicone rubber composites. Mater. Des. 2019, 165, 107580.
Zhou, W. Y.; Qi, S. H.; Zhao, H. Z.; Liu, N. L. Thermally conductive silicone rubber reinforced with boron nitride particle. Polym. Compos. 2007, 28, 23–28.
Kong, S. M.; Mariatti, M.; Busfield, J. J. C. Effects of types of fillers and filler loading on the properties of silicone rubber composites. J. Reinf. Plast. Compos. 2011, 30, 1087–1096.
Li, S. J.; Li, J. C.; Ji, P. Z.; Zhang, W. F.; Lu, Y. L.; Zhang, L. Q. Bubble-templated construction of three-dimensional ceramic network for enhanced thermal conductivity of silicone rubber composites. Chinese J. Polym. Sci. 2021, 39, 789–795.
Zhang, J.; Li, C.; Yu, C.; Wang, X.; Li, Q.; Lu, H.; Zhang, Q.; Zhao, J.; Songfeng, E.; Hu, M.; Yao, Y. Large improvement of thermal transport and mechanical performance of polyvinyl alcohol composites based on interface enhanced by SiO2 nanoparticle-modified-hexagonal boron nitride. Compos. Sci. Technol. 2019, 169, 167–175.
Zhao, C.; Li, Y.; Liu, Y.; Xie, H.; Yu, W. A critical review of the preparation strategies of thermally conductive and electrically insulating polymeric materials and their applications in heat dissipation of electronic devices. Adv. Compos. Hybrid Mater. 2022, 6, 27.
Chen, Y.; Zhang, H.; Chen, J.; Guo, Y.; Jiang, P.; Gao, F.; Bao, H.; Huang, X. Thermally conductive but electrically insulating polybenzazole nanofiber/boron nitride nanosheets nanocomposite paper for heat dissipation of 5G base stations and transformers. ACS Nano 2022, 16, 14323–14333.
Guerra, V.; Wan, C.; McNally, T. Thermal conductivity of 2D nano-structured boron nitride (BN) and its composites with polymers. Prog. Mater. Sci. 2019, 100, 170–186.
Rasul, M. G.; Kiziltas, A.; Arfaei, B.; Shahbazian-Yassar, R. 2D boron nitride nanosheets for polymer composite materials. npj 2D Mater. Appl. 2021, 5, 56.
Weng, Q.; Wang, X.; Wang, X.; Bando, Y.; Golberg, D. Functionalized hexagonal boron nitride nanomaterials: emerging properties and applications. Chem. Soc. Rev. 2016, 45, 3989–4012.
Yu, S.; Shen, X.; Kim, J. K. Beyond homogeneous dispersion: oriented conductive fillers for high kappa nanocomposites. Mater. Horiz. 2021, 8, 3009–3042.
Khanum, K. K.; Jayaram, S. H. Improved thermal properties and erosion resistance of silicone composites with hexagonal boron nitride. IEEE Trans. Ind. Appl. 2022, 58, 6583–6590.
Qu, J.; Fan, L.; Mukerabigwi, J. F.; Liu, C.; Cao, Y. A silicon rubber composite with enhanced thermal conductivity and mechanical properties based on nanodiamond and boron nitride fillers. Polym. Compos. 2021, 42, 4390–4396.
Chen, Q.; Xi, B.; Zhang, J.; Yang, H.; Wang, X.; Chi, M. Dielectric properties and thermal conductivity of micro-BN-modified LSR used for high-voltage direct current cable accessories. J. Mater. Sci.: Mater. Electron. 2020, 31, 16583–16591.
Gu, J.; Meng, X.; Tang, Y.; Li, Y.; Zhuang, Q.; Kong, J. Hexagonal boron nitride/polymethyl-vinyl siloxane rubber dielectric thermally conductive composites with ideal thermal stabilities. Compos. Part A: Appl. Sci. Manuf. 2017, 92, 27–32.
Kemaloglu, S.; Ozkoc, G.; Aytac, A. Properties of thermally conductive micro and nano size boron nitride reinforced silicon rubber composites. Thermochim. Acta 2010, 499, 40–47.
Li, Y. T.; Liu, W. J.; Shen, F. X.; Zhang, G. D.; Gong, L. X.; Zhao, L.; Song, P.; Gao, J. F.; Tang, L. C. PProcessing, thermal conductivity and flame retardant properties of silicone rubber filled with different geometries of thermally conductive fillers: a comparative studyP. Compos. Part B:Eng. 2022, 238, 109907.
Liu, P.; Li, L.; Wang, L.; Huang, T.; Yao, Y.; Xu, W. Effects of 2D boron nitride (BN) nanoplates filler on the thermal, electrical, mechanical and dielectric properties of high temperature vulcanized silicone rubber for composite insulators. J. Alloys Compd. 2011, 774, 396–404.
Zhang, P.; Yuan, P.; Jiang, X.; Zhai, S.; Zeng, J.; Xian, Y.; Qin, H.; Yang, D. A theoretical review on interfacial thermal transport at the nanoscale. Small 2018, 14, 1702769.
Chung, D. D. L. Performance of thermal interface materials. Small 2022, 18, 2200693.
Zhao, D.; Qian, X.; Gu, X.; Jajja, S. A.; Yang, R. Measurement techniques for thermal conductivity and interfacial thermal conductance of bulk and thin film materials. J. Electron. Packag. 2016, 138, 040802.
Grujicic, M.; Zhao, C. L.; Dusel, E. C. The effect of thermal contact resistance on heat management in the electronic packaging. Appl. Surf. Sci. 2005, 246, 290–302.
Due, J.; Robinson, A. J. Reliability of thermal interface materials: a review. Appl. Therm. Eng. 2013, 50, 455–463.
Leong, C.-K.; Chung, D. D. L. Carbon black dispersions as thermal pastes that surpass solder in providing high thermal contact conductance. Carbon 2003, 41, 2459–2469.
Hu, K.; Chung, D. D. L. Flexible graphite modified by carbon black paste for use as a thermal interface material. Carbon 2011, 49, 1075–1086.
Goel, N.; Anoop, T. K.; Bhattacharya, A.; Cervantes, J. A.; Mongia, R. K.; Machiroutu, S. V.; Lin, H. L.; Huang, Y. C.; Fan, K. C.; Denq, B. L.; Liu, C. H.; Lin, C. H.; Tien, C. W.; Pan, J. H. Technical review of characterization methods for thermal interface materials (Tim). 2008 11thIntersociety Conference on Thermal and Thermomecha Phenomena in Electronic Systems 2008, 248–258.
Chen, J.; Huang, X.; Sun, B.; Wang, Y.; Zhu, Y.; Jiang, P. Vertically aligned and interconnected boron nitride nanosheets for advanced flexible nanocomposite thermal interface materials. ACS Appl. Mater. Interfaces 2017, 9, 30909–30917.
Du, X.; Yang, W.; Zhu, J.; Fu, L.; Li, D.; Zhou, L. Aligning diamond particles inside BN honeycomb for significantly improving thermal conductivity of epoxy composite. Compos. Sci. Technol. 2022, 222, 109370.
Zhu, Z.; Li, C.; Songfeng, E.; Xie, L.; Geng, R.; Lin, C. T.; Li, L.; Yao, Y. Enhanced thermal conductivity of polyurethane composites via engineering small/large sizes interconnected boron nitride nanosheets. Compos. Sci. Technol. 2019, 170, 93–100.
Li, Z.; Ju, D.; Han, L.; Dong, L. Formation of more efficient thermally conductive pathways due to the synergistic effect of boron nitride and alumina in poly(3-hydroxylbutyrate). Thermochim. Acta 2017, 652, 9–16.
Tanimoto, M.; Yamagata, T.; Miyata, K.; Ando, S. Anisotropic thermal diffusivity of hexagonal boron nitride-filled polyimide films: effects of filler particle size, aggregation, orientation, and polymer chain rigidity. ACS Appl. Mater. Interfaces 2013, 5, 4374–4382.
Zhang, X.; Zhang, J.; Xia, L.; Li, C.; Wang, J.; Xu, F.; Zhang, X.; Wu, H.; Guo, S. Simple and consecutive melt extrusion method to fabricate thermally conductive composites with highly oriented boron nitrides. ACS Appl. Mater. Interfaces 2017, 9, 22977–22984.
Xie, Y.; Yu, Y.; Feng, Y.; Jiang, W.; Zhang, Z. Fabrication of stretchable nanocomposites with high energy density and low loss from cross-linked PVDF filled with poly(dopamine) encapsulated BaTiO3. ACS Appl. Mater. Interfaces 2017, 9, 2995–3005.
Zhang, F.; Feng, Y.; Qin, M.; Gao, L.; Li, Z.; Zhao, F.; Zhang, Z.; Lv, F.; Feng, W. Stress controllability in thermal and electrical conductivity of 3D elastic graphene-crosslinked carbon nanotube sponge/polyimide nanocomposite. Adv. Funct. Mater. 2019, 29, 1901383.
He, H.; Peng, W.; Liu, J.; Chan, X. Y.; Liu, S.; Lu, L.; Le Ferrand, H. Microstructured BN composites with internally designed high thermal conductivity paths for 3D electronic packaging. Adv. Mater. 2022, 34, e2205120.
Guo, H.; Niu, H.; Zhao, H.; Kang, L.; Ren, Y.; Lv, R.; Ren, L.; Maqbool, M.; Bashir, A.; Bai, S. Highly anisotropic thermal conductivity of three-dimensional printed boron nitride-filled thermoplastic polyurethane composites: effects of size, orientation, viscosity, and voids. ACS Appl. Mater. Interfaces 2022, 14, 14568–14578.
Prasher, R. S.; Shipley, J.; Prstic, S.; Koning, P.; Wang, J. L. Thermal resistance of particle laden polymeric thermal interface materials. ASME. J. Heat Transfer. 2003, 125, 1170–1177.
Acknowledgments
This work was financially supported by Sichuan Science and Technology Program (No. 2022YFH0090) and the Fundamental Research Funds for the Central Universities.
Author information
Authors and Affiliations
Corresponding author
Ethics declarations
The authors declare no interest conflict.
Rights and permissions
About this article
Cite this article
Ji, Y., Han, SD., Wu, H. et al. Understanding the Thermal Impedance of Silicone Rubber/Hexagonal Boron Nitride Composites as Thermal Interface Materials. Chin J Polym Sci 42, 352–363 (2024). https://doi.org/10.1007/s10118-023-3023-2
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s10118-023-3023-2