Flame-Retardant Bio-Based Thermo-Flexible Phase-Change Composites with Antivibration and Low-Contact Resistance for Advanced Battery Thermal Management

Abstract

Batteries face critical challenges in thermal management, including overheating risks, poor interfacial contact, and mechanical vibration–induced performance attenuation. To address these issues, we developed a flame-retardant bio-based thermo-flexible phase-change composite (VHPs) by integrating vanillin-derived polyols (VED), hexachlorocyclotriphosphazene-modified expanded graphite (HPEG), and polyethylene glycol (PEG). The HPEG hybrid filler effectively suppresses the “popcorn effect” of EG while significantly enhancing thermal conductivity, achieving a 246.90% improvement over neat polyurethane (PU). The thermally flexible polyurethane matrix reduces interfacial thermal resistance by 40% at 60 °C due to PEG soft-segment melting, enabling conformal wrapping around batteries. During 36 000 s of charge/discharge cycles, the VHPs reduced the battery temperature by 10 °C and increased the discharge capacity by 53.84% at 3C rates. Compared to the reported phase-change materials, VHPs uniquely integrate flame retardancy (peak of heat release rate reduced to 136.58 kW m⁻²), vibration resistance (compressive strength of 0.28 MPa at 50% strain), and infrared stealth (IR transmittance <0.04% in 3–25 μm). This work provides a sustainable, multifunctional solution for advanced battery thermal management, enhancing both safety and energy efficiency in high-power applications.

Keywords

battery thermal management / bio-based phase-change composites / flameretardance / low-contact thermal resistance / thermo-flexible

References

[1] L. Andaloro, A. Arista, G. Agnello, G. Napoli, F. Sergi, V. Antonucci, Int. J. Hydrog. Energy 2017, 42, 3166.

[2] Y. Mao, Y. Chen, M. Chen, Batteries 2024, 10, 307.

[3] D. Santos-Carballal, O. Lupan, N. Magariu, N. Ababii, H. Krüger, M. T. Bodduluri, N. H. de Leeuw, S. Hansen, R. Adelung, Nano Energy 2023, 109, 108301.

[4] Y. Guo, G. J. H. Lim, V. Verma, Y. Cai, K. K. Chan, E. J. J. Tang, M. Srinivasan, Chem. Eng. J. 2024, 498, 155329.

[5] U. Prasad, J. Prakash, A. N. M. Kannan, V. Kamavaram, G. K. Arumugam, Batter. Energy 2023, 2, 20230008.

[6] J. Nei, M. Wang, Int. J. Hydrog. Energy 2024, 49, 19.

[7] X. D. Lu, H. X. Li, S. X. Lun, Y. A. Ni, AIP Adv. 2024, 14, 15249.

[8] M. Jhariya, A. K. Dewangan, S. Q. Moinuddin, S. Kumar, A. Ahmad, A. K. Yadav, J. Therm. Anal. Calorim. 2024, 149, 13653.

[9] L. Wang, J. Phys. Conf. Ser. 2023, 2592, 12060.

[10] C. Wu, X. Yuan, B. Kong, Y. Zou, H. Shi, J. Energy Storage 2024, 81, 110485.

[11] W. Luo, L. Zhao, M. Chen, Appl. Therm. Eng. 2024, 236, 121608.

[12] J. Lyu, Z. Liu, X. Wu, G. Li, D. Fang, X. Zhang, ACS Nano 2019, 13, 2236.

[13] X. Cao, R. Zhang, N. Zhang, L. Chen, X. Li, J. Energy Storage 2023, 72, 108641.

[14] J. Y. Do, N. Son, J. Shin, R. K. Chava, S. W. Joo, M. Kang, Mater. Des. 2021, 198, 109357.

[15] Y. Yang, Q. Yin, F. Xu, L. Sun, Y. Xia, Y. Guan, L. Liao, T. Zhou, J. Lao, Y. Wang, Y. Wang, L. Song, D. Li, Thermochim. Acta 2022, 718, 179363.

[16] P. Rolka, T. Przybylinski, R. Kwidzinski, M. Lackowski, Sustain Energy Technol Assess 2024, 66, 103821.

[17] M. Wu, T. Li, P. Wang, S. Wu, R. Wang, J. Lin, Small 2022, 18, 2105647.

[18] G. Zhou, L. Li, S.-Y. Lee, F. Zhang, J. Xie, B. Ye, W. Geng, K. Xiao, J.-H. Lee, S.-J. Park, Z. Yang, C. Huang, Y. Zhang, Compos. Sci. Technol. 2023, 243, 110256.

[19] G. Zhu, M. Zou, W. Luo, Y. Huang, W. Chen, X. Hu, X. Jiang, Q. Li, Chem. Eng. J. 2024, 488, 150930.

[20] C. Wang, Y. Xia, J. Electrochem. Soc. 2023, 170, 60543.

[21] B. Liu, Y. Jia, C. Yuan, L. Wang, X. Gao, S. Yin, J. Xu, Energy Storage Mater 2020, 24, 85.

[22] P. C. Zhao, Z. Q. Liu, X. Y. Wang, Y. T. Pan, I. Kuehnert, M. Gehde, D. Y. Wang, A. Leuteritz, RSC Adv. 2018, 8, 42189.

[23] S. Wang, S. Ma, C. Xu, Y. Liu, J. Dai, Z. Wang, X. Liu, J. Chen, X. Shen, J. Wei, J. Zhu, Macromolecules 2017, 50, 1892.

[24] F. Feng, L. Qian, Polym. Compos. 2014, 35, 301.

[25] J. Wang, B. Xu, X. Wang, Y. Liu, Polym. Degrad. Stab. 2021, 186, 109516.

[26] Y. Wang, J. Zhao, M. Xiaojing, Prog. Org. Coat. 2019, 132, 178.

[27] M. Zhi, S. Yue, L. Zheng, B. Su, J. Fu, Q. Sun, J. Energy Storage 2024, 89, 111570.

[28] X.-L. Chen, F.-R. Zeng, W.-X. Li, L. Zhang, C. Deng, Y. Tan, M.-J. Chen, S.-C. Huang, B.-W. Liu, Y.-Z. Wang, H.-B. Zhao, J. Mater. Sci. Technol. 2023, 162, 179.

[29] Y. Chen, Z. Bai, X. Xu, J. Guo, X. Chen, S. L. Hsu, Z. Lu, H. Wu, Polymer 2023, 283, 126268.

[30] K. Jiang, W. Chen, X. Liu, Y. Wang, D. Han, Q. Zhang, Eur. Polym. J. 2022, 179, 111572.

[31] S. Wang, K. Wei, W. Shi, P. Cheng, J. Shi, B. Ma, J. Energy Storage 2022, 56, 105970.

[32] Y. Yang, B. Liu, T. Zhang, Y. Wu, P. Wang, C. Liu, Y. Shi, S. Mu, Prog. Org. Coat. 2025, 201, 109098.

[33] Z. Liu, K. Wei, S. Wang, B. Ma, X. Wang, W. Shi, J. Xu, Constr. Build. Mater. 2021, 300, 124007.

[34] X. Shen, B. Wang, N. Li, Y. Zhang, H. Ju, Y. Xiao, P. He, J. Lei, J. Energy Storage 2025, 108, 115061.

[35] R. Wang, L. Chen, Q. Lei, J. Shi, C. Chen, Polym. Eng. Sci. 2022, 62, 664.

[36] G. Chen, Z.-Y. Hu, N. Chen, Z. Zhao, C. Li, Y. Xie, Mater. Chem. Phys. 2024, 314, 128842.

[37] X. Zhao, D. Zou, S. Wang, Chem. Eng. J. 2022, 431, 134231.

[38] N. Sun, X. Li, J. Mater. Sci. 2021, 56, 15937.

[39] A. Alonso, D. Lázaro, M. Lázaro, D. Alvear, Combust. Sci. Technol. 2023, 195, 1509.

[40] E. Gallo, W. Stöcklein, P. Klack, B. Schartel, Fire Mater. 2017, 41, 768.

[41] N. Zhu, X. Wang, Q. Huang, C. Ding, J. Wang, J. Therm. Anal. Calorim. 2023, 148, 6119.

[42] A. Sun, K. Harada, D. Nii, Fire. Technol 2024, 60, 2559.

[43] J. W. Park, O. K. Lim, W. J. You, Energies 2020, 13, 3644.

[44] L. Z. Pires, O. L. Santos, A. Kairytė, J. Šeputytė-Jucikė, S. Makowska, D. Battegazzore, A. Frache, R. D. Delucis, P. H. de Cademartori, A. P. Acosta, Appl. Sci. 2024, 14, 3450.

[45] Y. Pan, J. Zhan, H. F. Pan, W. Wang, H. Ge, L. Song, Y. Hu, RSC Adv. 2015, 5, 67878.

[46] S. M. Goller, S. Krüger, B. Schartel, Polym. Degrad. Stab. 2023, 209, 110276.

[47] S. Xu, M. Zhang, S. Y. Li, H. Y. Zeng, J. Z. Du, C. R. Chen, K. Wu, X. Y. Tian, Y. Pan, Appl. Clay Sci. 2020, 185, 105348.

[48] W.-H. Rao, W. Liao, H. Wang, H.-B. Zhao, Y.-Z. Wang, J. Hazard. Mater. 2018, 360, 651.

[49] W. Xi, L. Qian, Z. Huang, Y. Cao, L. Li, Polym. Degrad. Stab. 2016, 130, 97.

[50] W. Lin, C. Liang, J. Zeng, J. Cheng, Y. Wang, F. Zhang, S. Li, J. Build. Eng. 2024, 89, 109257.

[51] J. Cheng, C. Liang, W. Lin, J. Zeng, C. Li, S. Li, F. Zhang, Y. Wang, J. Energy Storage 2024, 80, 110357.

[52] S. Niu, J. Cheng, Y. Zhao, M. Kang, Y. Liu, Constr. Build. Mater. 2022, 347, 128628.

[53] S. Niu, M. Kang, Y. Liu, W. Lin, C. Liang, Y. Zhao, J. Cheng, Energy 2023, 268, 126652.

[54] Y. Luo, D. Zhou, W. Yang, C. Li, H. Liu, W. Qiang, X. Yang, G. Zhao, C. Bi, T. Wang, X. Yang, X. Li, Appl. Therm. Eng. 2025, 258, 124763.

[55] X. Du, J. Qiu, S. Deng, Z. Du, X. Cheng, H. Wang, Renew. Energy 2021, 164, 1.

[56] X. Du, L. Jin, S. Deng, M. Zhou, Z. Du, X. Cheng, H. Wang, ACS Appl. Mater. Interfaces 2021, 13, 42991.

[57] Z. Xu, W. Chen, T. Wu, C. Wang, Z. Liang, Surf Interfaces 2023, 36, 102558.

[58] S. Bai, K. Zhang, Q. Zhang, Y. Zhu, W. Wang, J. Zhang, X. Li, X. Zhang, R. Wang, ACS Appl. Mater. Interfaces 2023, 15, 48613.

[59] H. Han, F. Xiong, M. Qin, Y. Jin, H. K. Chu, S. Han, K. Jia, A. Usman, S. Gao, R. Zhong, Z. Shen, R. Zou, Energy Storage Mater 2025, 77, 104175.

[60] L. Zhang, L. Peng, S. Liang, Z. Chen, S. Lyu, S. Wang, J. Clean. Prod. 2024, 446, 141417.

[61] J.-L. He, W. Luo, T. Wang, L. He, J.-N. Deng, Z.-C. Fu, J. C. Grunlan, M.-J. Chen, ACS Appl. Mater. Interfaces 2022, 14, 54225.

[62] Z. L. Wang, W. Z. Wu, X. Gong, Mater. Horiz. 2025, 12, 3036.

[63] W. X. Wu, J. Z. Liu, M. Liu, Z. H. Rao, H. Deng, Q. Wang, X. Qi, S. F. Wang, Energy Convers. Manag. 2020, 221, 113145.

[64] M. J. Brand, S. F. Schuster, T. Bach, E. Fleder, M. Stelz, S. Gläser, J. Müller, G. Sextl, A. Jossen, J. Power Sources 2015, 288, 62.

[65] N. Joshy, M. Hajiyan, A. R. M. Siddique, S. Tasnim, H. Simha, S. Mahmud, J. Power Sources 2020, 450, 227717.

[66] Q. Huang, X. Li, G. Zhang, Y. Kan, C. Li, J. Deng, C. Wang, Appl. Energy 2022, 309, 118434.

[67] Q. Xu, Y. Xie, X. Li, L. Li, K. Zheng, S. Bei, Energy 2024, 308, 132847.

[68] X. Zhu, J. Liu, L. Zhang, W. Zhao, Y. Cao, X. Liu, Small 2024, 20, 2405694.

[69] Z. Chen, X. Wu, Q. Kang, H. Liu, K. Yu, K. Zhang, Int. Commun. Heat Mass Transfer 2024, 159, 108265.

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2026 The Author(s). Energy & Environmental Materials published by John Wiley & Sons Australia, Ltd on behalf of Zhengzhou University.