

FOLLOWUS
a.School of Environmental and Chemical Engineering, Jiangsu Ocean University, Lianyungang 222005, China
b.Jiangsu Institute of Marine Resources Development, Jiangsu Ocean University, Lianyungang 222005, China
licj_poly@jou.edu.cn
Received:02 December 2024,
Revised:2025-01-04,
Accepted:17 January 2025,
Online First:04 March 2025,
Published:01 April 2025
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Guo, J. X.; Cai, S. Y.; Han, X.; Sun, Y.; Li, C. L.; Zheng, K.; Xu, Y. Z.; Li, R. G.; Li, C. J. Recyclable, flexible and highly thermally conductive phase change composites with dynamic networks for thermal management. Chinese J. Polym. Sci. 2025, 43, 625–639
Jun-Xia Guo, Shuang-Yu Cai, Xu Han, et al. Recyclable, Flexible and Highly Thermally Conductive Phase Change Composites with Dynamic Networks for Thermal Management[J]. Chinese Journal of Polymer Science, 2025, 43(4): 625-639.
Guo, J. X.; Cai, S. Y.; Han, X.; Sun, Y.; Li, C. L.; Zheng, K.; Xu, Y. Z.; Li, R. G.; Li, C. J. Recyclable, flexible and highly thermally conductive phase change composites with dynamic networks for thermal management. Chinese J. Polym. Sci. 2025, 43, 625–639 DOI: 10.1007/s10118-025-3299-5.
Jun-Xia Guo, Shuang-Yu Cai, Xu Han, et al. Recyclable, Flexible and Highly Thermally Conductive Phase Change Composites with Dynamic Networks for Thermal Management[J]. Chinese Journal of Polymer Science, 2025, 43(4): 625-639. DOI: 10.1007/s10118-025-3299-5.
The GNR/PW/CGNP composites with dynamic ionic crosslinking exhibit recyclable processability
excellent shape stability
highly thermal conductivity
and high latent heat
which makes the composites the promising candidate for thermal management applications in electronic devices.
Flexible phase change materials (PCMs) have become increasingly critical to address the demand for thermal management in electronic technologies and energy conversion. However
their application remains challenging because of their rigidity
liquid leakage
and insufficient thermal conductivity. Herein
flexible glutamic acid@natural rubber/paraffin wax (PW)/carbon nanotubes-graphene nanoplatelets (GNR/PW/CGNP) phase change composites with high thermal conductivity
excellent shape stability
and recyclability were reported. Zn
2+
-based dynamic crosslinking was constructed through the reaction of zinc acetate and carboxyl groups on glutamic acid@natural rubber (GNR)
which was used as a flexible matrix to physically blend with paraffin wax/carbon nanotubes/graphene nanoplatelets (PW/CGNP) to achieve uniform dispersion of PW/CGNP
continuous thermal conductivity networks
and good encapsulation of PW. The GNR/PW/CGNP composites showed excellent mechanical strength
flexibility
and recycling ability
and effective encapsulation prevented the outflow of melted PW during the phase transition. Also
the phase change enthalpy could attain 111.1 J/g with a higher thermal conductivity of 1.055 W/mK
428% higher than that of pure PW owing to the formation of efficient thermal conductive pa
thways
which exhibited outstanding thermal management performance and superior temperature control behavior in electronic devices. The developed flexible composite PCMs may open new possibilities for next-generation flexible thermal management electronics.
Sun, N.; Luo, Q.; Li, X.; Wang, Z. High-flexible phase change composites with enhanced thermal conductivity for electronic thermal management. ACS Appl. Polym. Mater. 2024 , 6 , 778−786..
Liu, Z.; He, F.; Jiang, Z.; Li, Y.; Wang, P.; He, G.; Yang, W. Flexible and thermally conductive phase-change films with a two-level network for dual-mode thermal management of batteries. ACS Sustain. Chem. Eng. 2024 , 12 , 4605−4618..
Zhang, Y.; Ruan, K.; Zhou, K.; Gu, J. Controlled distributed Ti 3 C 2 T x hollow microspheres on thermally conductive polyimide composite films for excellent electromagnetic interference shielding. Adv. Mater. 2023 , 35 , 2211642..
Yang, C.; Hao, W.; Xu, X.; Hu, L.; Zheng, X.; Zhu, C. Heat storage and release in binary paraffin-hexadecyl amine composites for solar greenhouses in cold climates. Appl. Therm. Eng. 2024 , 240 , 122269..
Yang, A. S.; Huang, R.; Zhang, Q. P.; Jiang, Z.; Li, Y.; He, F.; Yang, W. Poly(ethylene glycol)-based reprocessed solid–solid phase change materials with dynamic semi-interpenetrating network for efficient energy storage and thermal management. ACS Sustain. Chem. Eng. 2024 , 12 , 7778−7790..
Gong, J.; Tan, X.; Yuan, Q.; Liu, Z.; Ying, J.; Lv, L.; Dai, W. A spiral graphene framework containing highly ordered graphene microtubes for polymer composites with superior through-plane thermal conductivity. Chin. J. Chem. 2022 , 40 , 329−336..
Fang, H.; Zeng, J.; Shao, X.; Hu, D. Advanced electromagnetic shielding and excellent thermal management of flexible phase change composite films. Carbon. 2023 , 215 , 118442..
Lin, Y.; Kang, Q.; Wei, H.; Bao, H.; Jiang, P.; Mai, Y. W.; Huang, X. Spider web-inspired graphene skeleton-based high thermal conductivity phase change nanocomposites for battery thermal management. Nano-Micro Lett. 2021 , 13 , 180..
Sun, B.; Huang, X. Seeking advanced thermal management for stretchable electronics. Npj Flex. Electron . 2021 , 5 , 12..
Ghosh, D.; Ghose, J.; Datta, P.; Kumari, P.; Paul, S. Strategies for phase change material application in latent heat thermal energy storage enhancement: status and prospect. J. Energy Storage 2022 , 53 , 105179..
Tao, J.; Luan, J.; Liu, Y.; Qu, D.; Yan, Z.; Ke, X. Technology development and application prospects of organic-based phase change materials: an overview. Renewable Sustain. Energy Rev. 2022 , 159 , 112175..
Mehrizi, A. A., Karimi-Maleh, H., Naddafi, M., & Karimi, F. Application of bio-based phase change materials for effective heat management. J. Energy Storage 2023 , 61 , 106859..
Umair, M. M.; Zhang, Y.; Iqbal, K.; Zhang, S.; Tang, B. Novel strategies and supporting materials applied to shape-stabilize organic phase change materials for thermal energy storage—a review. Appl. Energy 2019 , 235 , 846−873..
Luo, L.; Luo, W.; Chen, W.; Hu, X.; Ma, Y.; Xiao, S.; Jiang, X. Form-stable phase change materials based on graphene-doped PVA aerogel achieving effective solar energy photothermal conversion and storage. Sol. Energy 2023 , 255 , 146−156..
Jiang, Z.; Yang, W.; He, F.; Fan, J.; Wu, J.; Zhang, K. Microencapsulated paraffin phase-change material with calcium carbonate shell for thermal energy storage and solar-thermal conversion. Langmuir 2018 , 34 , 14254−14264..
Bayram, M.; Ustaoglu, A.; Kursuncu, B.; Hekimoglu, G.; Sari, A.; Uğur, L. O.; Ozbakkaloglu, T. 3D-printed polylactic acid-microencapsulated phase change material composites for building thermal management. Renewable Sustain. Energy Rev . 2024 , 191 , 114150..
Guo, Y.; Qiu, H.; Ruan, K.; Wang, S.; Zhang, Y.; Gu, J. Flexible and insulating silicone rubber composites with sandwich structure for thermal management and electromagnetic interference shielding. Compos. Sci. Technol. 2022 , 219 , 109253..
Hu, X.; Zhu, C.; Wu, H.; Li, X.; Lu , X.; Qu, J. Large-scale preparation of flexible phase change composites with synergistically enhanced thermally conductive network for efficient low-grade thermal energy recovery and utilization. Composites, Part A. 2022 , 154 , 106770..
Abdeali, G.; Abdollahi, M.; Bahramian, A. R. Synthesis and characterization of paraffin wax nanocapsules with polyurethane shell (PU/PW); the droplet size distribution: a key factor for thermal performance. Renew. Energy 2021 , 163 , 720−731..
Hu, D.; Han, L.; Zhou, W.; Li, P.; Huang, Y.; Yang, Z.; Jia, X. Flexible phase change composite based on loading paraffin into cross-linked CNT/SBS network for thermal management and thermal storage. Chem. Eng. J. 2022 , 437 , 135056..
Guo, M.; Xu, P.; Lv, J.; Gong, C.; Zhang, Z.; Li, C. Engineering nanocellulose/graphene hybrid aerogel for form-stable composite phase change materials with high phase change enthalpy for energy storage. Diam Relat Mater. 2022 , 127 , 109131..
Li, Y.; Sun, K.; Kou, Y.; Liu, H.; Wang, L.; Yin, N.; Shi, Q. One-step synthesis of graphene-based composite phase change materials with high solar-thermal conversion efficiency. Chem. Eng. J. 2022 , 429 , 132439..
Li, W.; Wang, F.; Cheng, W.; Chen, X.; Zhao, Q. Study of using enhanced heat-transfer flexible phase change material film in thermal management of compact electronic device. Energ. Convers. Manage. 2020 , 210 , 112680..
Kang, L.; Niu, H.; Ren, L.; Lv, R.; Guo, H.; Bai, S. A novel phase change composite with ultrahigh through-plane thermal conductivity and adjustable flexibility. Chem. Eng. J. 2023 , 463 , 142402..
Zhang, X.; Sun, K.; Liu, H.; Chen, J.; Yan, X.; Kou, Y.; Shi, Q. Flexible insulating phase change composite filmwith improved thermal conductivity for wearable thermal management. Nano Energy 2024 , 121 , 109256..
Gong, C.; Guo, J.; Xu, P.; Lv, J.; Li, R.; Li, C. Recyclable, self-healing, and highly thermal conductive natural rubber nanocomposites enabled by a dynamic covalent network with carboxylated boron nitride nanosheets. ACS Sustain. Chem. Eng . 2023 , 11 , 9087−9102..
Guo, J.; Han, X.; Ma, S.; Sun, Y.; Li, C.; Li, R.; Li, C. Form-stable phase change composites with high thermal conduct ivity and enthalpy enabled by graphene/carbon nanotubes aerogel skeleton for thermal energy storage. Appl. Therm. Eng. 2024 , 255 , 123954..
Boonluksiri, Y.; Siangdang, P.; Johns, J.; Nakaramontri, Y. Utilization of modified epoxidized natural rubber and zinc oxide on properties of polylactic acid/epoxidized natural rubber blends: mechanical properties, antibacterial efficiency and biodegradability. Ind. Crops. Prod. 2024 , 220 , 119102..
Li, X.; Zhao, Y.; Min, X.; Xiao, J.; Wu, X.; Mi, R.; Fang, M. Carbon nanotubes modified graphene hybrid aerogel-based composite phase change materials for efficient thermal storage. Energy Build. 2022 , 273 , 112384..
Huang, W.; Wang, Z.; Zhou, H.; Yu, Z.; Hao, Z.; Gao, Y.; Cai, J. Highly thermal conductive graphene/paraffin composite for efficient thermal management of electronics. Appl. Therm. Eng. 2024 , 246 , 122958..
Yu, M.; Fang, G.; Meng, K.; Sun, P.; Zhao, M. Paraffin/modified exfoliated graphite composite phase change materials with high performance and stability for thermal energy storage. Therm. Anal. Calorim . 2023 , 148 , 675−687..
Gong, C.; Cao, J.; Guo, M.; Cai, S.; Xu, P.; Lv, J.; Li, C. A facile strategy for high mechanical performance and recyclable EPDM rubber enabled by exchangeable ion crosslinking. Eur. Polym. J. 2022 , 175 , 111339..
Li, C.; Yuan, Z.; Ye L. Facile construction of enhanced multiple interfacial interactions in EPDM/zinc dimethacrylate (ZDMA) rubber composites: highly reinforcing effect and improvement mechanism of sealing resilience. Compos Part A-Appl S. 2019 , 126 , 105580−105580..
Cai, Z.; Liu, J.; Zhou, Y.; Dai, L.; Wang, H.; Liao, C.; Xu, Y. Flexible phase change materials with enhanced tensile strength, thermal conductivity and photo-thermal performance. Sol. Energy Mater Sol. Cells. 2021 , 219 , 110728..
Wu, H. Y.; Li, S. T.; Shao, Y. W.; X. Z.; Qi, X. D.; Yang, J. H.; Wang, Y. Melamine foam/reduced graphene oxide supported form-stable phase change materials with simultaneous shape memory property and light-to-thermal energy storage capability. Chem. Eng. J. 2020 , 379 , 122373..
Du, X., L.; Deng, S.; Zhou, M.; Du, Z.; Cheng, X.; Wang, H. Recyclable, self-healing, and flame-retard ant solid–solid phase change materials based on thermally reversible cross-links for sustainable thermal energy storage. ACS Appl. Mater. Interfaces 2021 , 13 , 42991−43001..
Xu, C.; Huang, X.; Li, C.; Chen, Y.; Lin, B.; Liang, X. Design of “Zn2+ salt-bondings” cross-linked carboxylated styrene butadiene rubber with reprocessing and recycling ability via rearrangements of ionic cross-linkings. ACS Sustain. Chem. Eng. 2016 , 4 , 6981−6990..
Larrue, C.; Bounor-Legaré, V.; Cassagnau, P. Enhancement of EPDM crosslinked elastic properties by association of both covalent and ionic networks. Polymers 2021 , 13 , 3161..
Wang, C.; Cheng, C., T.; Dong, H. Review on bio-based shape-stable phase change materials for thermal energy storage and utilization. J. Renew. Sustain. Energy 2022 , 14 , 52701..
Cao, H.; Li, Y.; Xu, W.; Yang, J.; Liu, Z.; Bai, L.; Yang, M. Leakage-proof flexible phase change gels with salient thermal conductivity for efficient thermal management. ACS Appl. Mater. Interfaces 2022 , 14 , 52411−52421..
Bao, Z.; Bing, N.; Yao, H. R.; Zhang, Y.; Xie, H.; Yu, W. Three-dimensional interpenetrating network phase-change composites with high photothermal conversion and rapid heat storage and release. ACS Appl. Energy Mater . 2021 , 4 , 7710−7720..
Wang, C.; Geng, X.; Chen, J.; Wang, H.; Wei, Z.; Huang, B.; He, X. Multiple H-bonding cross-linked supramolecular solid-solid phase change materials for thermal energy storage and management. Adv. Mater. 2024 , 36 , 2309723..
Tang, X.; Zhang, J.; Wang, J.; Xu, T.; Du, Y.; Fan, G.; Wu, H. Preparation and application of paraffin/expanded graphite-based phase change material floor for solar-heat pump combined radiant heating systems. ACS Sustain. Chem. Eng. 2023 , 11 , 2871−2884..
Wei, Q.; Yang, D.; Yu, L.; Zhang, L. Grafting of epoxidized natural rubber chains with BN platelets to obtain flexible and thermally conductive papers. Compos. Sci. Technol. 2021 , 212 , 108881..
Yu, L.; Yang, D.; Wei, Q.; Zhang, L. Constructing of strawberry-like core-shell structured Al 2 O 3 nanoparticles for improving thermal conductivity of nitrile butadiene rubber composites. Compos. Sci. Technol. 2021 , 209 , 108786..
Xu, W.; Yang, W.; Su, J.; Huang, J.; Min, Y.; Yu, Y.; Li, X. Diatom-based biomass composites phase change materials with high thermal conductivity for battery thermal management. J Energy Storage. 2024 , 96 , 112737..
Zhu, X.; Han, L.; Lu, Y.; Wei, F.; Jia, X. Geometry-induced thermal storage enhancement of shape-stabilized phase change materials based on oriented carbon nanotubes. Appl. Energy 2019 , 254 , 11368..
Liu, C.; Duan, X.; Zhang, W.; Huo, Q.; Sui, X.; Liu, Y.; Liang, C. Stable self-crosslinking phase change composites with vertically aligned boron nitride for high thermal conductivity thermal interface materials. Ceram. Int. 2024 , 50 , 19829−19837..
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