Multifunctional Polyurethane with High Strength, Toughness, and Self-healing Capacity <italic style="font-style: italic">via</italic> Tannic Acid-modified Cellulose Nanocrystals

Dan-Min Wu; Chao-Qun Wu; De-Xiang Sun; Xiao-Dong Qi; Jing-Hui Yang; Yong Wang

doi:10.1007/s10118-026-3670-1

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Multifunctional Polyurethane with High Strength, Toughness, and Self-healing Capacity via Tannic Acid-modified Cellulose Nanocrystals

RESEARCH ARTICLE | Updated：2026-05-27

- Multifunctional Polyurethane with High Strength, Toughness, and Self-healing Capacity via Tannic Acid-modified Cellulose Nanocrystals
- Chinese Journal of Polymer Science Vol. 44, Issue 8, Pages: 2619-2629(2026)
- Affiliations：
  
  Key Laboratory of Advanced Technologies of Materials (Ministry of Education), School of Chemistry, Southwest Jiaotong University, Chengdu 610031, China
- Author bio：
  
  chaoqunwu@swjtu.edu.cn (C.Q.W.)
  yongwang1976@swjtu.edu.cn (Y.W.)
- Funds：
- DOI：10.1007/s10118-026-3670-1
  CLC： [M
- Received：13 January 2026，
  
  Revised：2026-03-12，
  
  Accepted：16 March 2026，
  
  Online First：26 May 2026，
  
  Published：15 August 2026
- Accepted：
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Wu, D. M.; Wu, C. Q.; Sun, D. X.; Qi, X. D.; Yang, J. H.; Wang, Y. Multifunctional polyurethane with high strength, toughness, and self-healing capacity via tannic acid-modified cellulose nanocrystals. Chinese J. Polym. Sci. 2026, 44, 2619–2629

Dan-Min Wu, Chao-Qun Wu, De-Xiang Sun, et al. Multifunctional Polyurethane with High Strength, Toughness, and Self-healing Capacity via Tannic Acid-modified Cellulose Nanocrystals[J]. Chinese Journal of Polymer Science, 2026, 44(8): 2619-2629. DOI: 10.1007/s10118-026-3670-1.
Wu, D. M.; Wu, C. Q.; Sun, D. X.; Qi, X. D.; Yang, J. H.; Wang, Y. Multifunctional polyurethane with high strength, toughness, and self-healing capacity via tannic acid-modified cellulose nanocrystals. Chinese J. Polym. Sci. 2026, 44, 2619–2629 DOI： 10.1007/s10118-026-3670-1.

Dan-Min Wu, Chao-Qun Wu, De-Xiang Sun, et al. Multifunctional Polyurethane with High Strength, Toughness, and Self-healing Capacity via Tannic Acid-modified Cellulose Nanocrystals[J]. Chinese Journal of Polymer Science, 2026, 44(8): 2619-2629. DOI: 10.1007/s10118-026-3670-1. DOI：

摘要

Ultrahigh-density hydrogen-bonded elastomers were prepared by incorporating tannic-acid-functionalized cellulose nanocrystals (TA@CNC) into a waterborne polyurethane (WPU) matrix. The optimized material achieves a tensile strength of 48 MPa

elongation at break of 2667%

toughness of 700 MJ·m

–3

true fracture stress of 1319 MPa

and 84% room-temperature self-healing efficiency.

Abstract

There is an increasing demand for polyurethane (PU) elastomers that integrate high mechanical performance with environmental and economic sustainability to satisfy the demands of advanced applications. However

their development is hindered by a fundamental trade-off: enhancing strength typically compromises toughness

whereas incorporating self-healing capacity often diminishes mechanical robustness. To overcome this challenge

we presen

t a strategy based on an ultrahigh-density hydrogen-bonded network formed at the interface between tannic acid-functionalized cellulose nanocrystals (TA@CNC) and waterborne polyurethane (WPU) matrix. This dynamically cross-linked architecture enables efficient energy dissipation and supports intrinsic self-healing

thereby simultaneously enhancing both mechanical performance and self-healing capacity. The resulting elastomer demonstrates outstanding overall performance

achieving a tensile strength of 48 MPa

an elongation at break of 2667%

a toughness of 700 MJ·m

–3

a true fracture stress of 1319 MPa

and a room-temperature self-healing efficiency of 84%. The design strategy presented here opens new avenues for developing polyurethane elastomers with simultaneously enhanced mechanical performance and self-healing capacity

effectively paving the way for their application in demanding and sustainable scenarios.

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references

[Fu, M. Y.; Sun, H. J. Polyurethane elastomer and application . Beijing, Chemical Industry Press, 2006 ..

Allan, M. Structural behaviour of a prefabricated composite wall system made from rigid polyurethane foam and magnesium oxide board. Constr. Build. Mater. 2013 , 41 , 642−653..

Xu, W. L.; Zhang, Z.; Lu, H.; Wu, Y. F.; Liu, J.; Liu, S. W.; Yang, W. J. Biocompatible polyurethane conduit grafted with vascular endothelial growth factor-loaded hydrogel repairs the peripheral nerve defect in rats. Macromol. Biosci. 2022 , 22 , 2100397..

Zhu, Z. J.; Tian, Z. Y.; Zhang, F. X.; Li, Z.; Yang, D. Self-healing waterborne polyurethane-based wearable sensors with excellent thermal management and electromagnetic interference shielding for advanced biometric gait recognition. Adv. Funct. Mater. 2025 , 36 , 2511461..

Yuan, X.; Wang, W.; Wang, R. Z.; Liu, J. Y.; Zhao, Q. N.; Ji, W. H.; Chen, S. G. A novel Ti 3 C 2 T x -PANI composite polyurethane coating with dual corrosion resistance and noise reduction functionality. Prog. Org. Coat. 2024 , 197 , 108860..

Yang, Y.; Urban, M. W. Self-healing polymeric materials. Chem. Soc. Rev. 2013 , 42 , 7446−7467..

Yang, Y.; Ding, X. C.; Urban, M. W. Chemical and physical aspects of self-healing materials. Prog. Polym. Sci . 2015 , 49-50 , 34−59..

Hou, J.; Liu, M. S.; Zhang, H. C.; Song, Y. L.; Jiang, X. C.; Yu, A. B.; Jiang, L.; Su, B. Healable green hydrogen bonded networks for circuit repair, wearable sensor and flexible electronic devices. J. Mater. Chem. A 2017 , 5 , 13138−13144..

Li, X. K.; Wang, Y. Y.; Zhang, X. X. Strong, healable materials with bio-like ordered architectures and versatile functionality. SusMat 2024 , 4 , 224−255..

Tan, M. W. M.; Thornton, P. M.; Thangavel, G.; Bark, H.; Dauskardt, R.; Lee, P. S. Toughening self-healing elastomers with chain mobility. Adv. Sci. 2024 , 11 , 2308154..

Meyers, M. A.; Mckittrick, J.; Chen, P. Y. Structural biological materials: Critical mechanics-materials connections. Science 2013 , 339 , 773−779..

Chen, L. Y.; You, W.; Wang, J.; Yang, X.; Xiao, D.; Zhu, H. T. Z.; Zhang, Y. F.; Li, G. F.; Yu, W.; Sessler, J. L.; Huang, F. H. Enhancing the toughness and strength of polymers using mechanically interlocked hydrogen bonds. J. Am. Chem. Soc. 2023 , 146 , 1109−1121..

Xu, J. H.; Chen, J. Y.; Zhang, Y. N.; Liu, T.; Fu, J. J. A fast room-temperature self-healing glassy polyurethane. Angew. Chem. 2021 , 133 , 7947−7955..

Qian, Y. H.; Dong, F. H.; Wang, S. S.; Jiang, Y. M.; Xu, X.; Liu, H. Ultrarobust, stretchable, and highly elastic supramolecular elastomer with hydrogen-bond interactions via sp 2 hybridized boron-urethane bonds. Angew. Chem. Int. Ed. 2025 , 64 , 2421099..

Wu, J.; Zeng, F. X.; Fan, Z. Y.; Xuan, S. H.; Hua, Z.; Liu, G. M. Hierarchical hydrogen bonds endow supramolecular polymers with high strength, toughness, and self-healing properties. Adv. Funct. Mater. 2024 , 34 , 2410518..

Zhang, R. C.; Xiang, X. B.; Sheng, D. H.; Zhang, L.; Ren, W. M.; Xie, G. X.; Wei, S. T.; Dai, H. L. A mechanically robust polyurethane elastomer with excellent crack tolerance, recyclability and weathering resistance via microphase dynamic ordering. J. Mater. Chem. A 2025 , 13 , 40017−40028..

Xu, H. R.; Wang, S. L.; Li, W. L.; Hu, K. J.; Zhao, C.; Jin, H. C.; Tian, L. M.; Ren, L. Q. Mechanism exploration of spider-silk-inspired multiple-hydrogen-bond polyurethane healable elastomers for anticorrosion. Nano Lett. 2025 , 25 , 10513−10520..

Yu, C. S.; Zhang, D. X.; Huang, Z.; Miao, Y. G.; Chen, Z. M.; Zhang, X. X. Robust yet self-healing multimodal actuators enabled by noncovalent assembled nanostructure. Nano Lett. 2025 , 25 , 1 925−1931..

Gan, H.; Wang, L.; Sun, R.; Li, J. C.; Zhao, Z.R.; Chen, Y.; Tian, W. L.; Yang, F.; Huang, Q. Development of a graphene oxide-enhanced thermoresponsive self-healing waterborne polyurethane elastomer for abdominal wall defect repair. ACS Appl. Nano Mater. 2025 , 8 , 17576−17590..

Wang, L.; Wang, X. B.; Liu, T.; Sun, F. Y.; Li, S.N.; Geng, Y. H.; Yao, B. W.; Xu, J. Hua.; Fu, J. J. Bio-inspired self-healing and anti-corrosion waterborne polyurethane coatings based on highly oriented graphene oxide. npj Mater. Degrad. 2023 , 7 , 1−15..

Zhou, M.; Liu, W. Q.; Fu, He. Q. Construction of ultrathin self-healing films with highly efficient electromagnetic interference shielding and Joule heating capability by MXene decorating liquid metal. J. Alloy. Compd. 2023 , 968 , 171931..

Yan, N. S.; Zhu, X. Z.; Tian, L.; Han, J. B.; Zang, J. J.; Zhang, H. T. Self-healing waterborne polyurethane nanocomposites with high strength and toughness based on ureidopyrimidinone-modified cellulose nanocrystals. Carbohydr. Polym. 2025 , 365 , 123806..

Zhang, X.; Dong, F. H.; Yu, M. M.; Xu, X.; Liu, H.; Lu, H. Q. Multifunctional waterborne polyurethane-cellulose nanofiber composite: realizing ultrarobust, photoluminescence and swift self-healing via multi-dynamic bonding. Chem. Eng. J. 2025 , 507 , 160302..

Kim, S.; Gim, T.; Kang, S. M. Tannic acid-mediated surface pegylation for marine antifouling applications. ACS Appl. Mater. Interfaces 2015 , 7 , 6412−6416..

Wang, S. H.; Zhang, L.; Wang, Z. M.; Song, Z. Q.; Liu, H.; Tian, Z. Q.; Xu, X. Humidity-adaptive, mechanically robust, and recyclable bioplastic films amplified by nanoconfined assembly. Aggregate 2024 , 5 , 447−459..

Marx, V.; Mochida, Y.; Osawa, S.; Tockary, T. A.; Norimatsu, J.; Yokoo, H.; Oba, M.; Uchida, S. Poly(sarcosine) and poly(2-ethyl-2-oxazoline) tethered to mrna provide stealth properties to mRNA polyplexes. ACS Appl. Nano Mater. 2025 , 8 , 13628−13638..

Li, M.-C.; Wu, Q. L.; Song, K. L.; Lee, S.; Qing, Y.; Wu, Y. Q. Cellulose nanoparticles: Structure-morphology-rheology relationships. ACS Sustainable Chem. Eng. 2015 , 3 , 821−832..

Ying, W. B.; Yu, Z.; Kim, D. H.; Lee, K. J.; Hu, H.; Liu, Y. W.; Kong, Z. Y.; Wang, K.; Shang, J.; Zhang, R. Y.; Zhu, J.; Li, R.-W. Waterproof, highly tough, and fast self-healing polyurethane for durable electronic skin. ACS Appl. Mater. Interfaces 2020 , 12 , 11072−11083..

Xu, W.; Zhang, R. Y.; Liu, W.; Zhu, J.; Dong, X.; Guo, H. X.; Hu, G. H. A multiscale investigation on the mechanism of shape recovery for IPDI to PPDI hard segment substitution in polyurethane. Macromolecules 2016 , 49 , 5931−5944..

Yu, C. S.; Wang, Y. Y.; Qiu, X. Y.; Liu, J. Z.; Li, X. K.; Yang, X.; Huang, X.; Zhang, X. X.; Chen, Z. M. Ultrarobust self-healing elastomers with hydrogen bonding connected MXene network for actuator applications. Chem. Eng. J . 2023 , 475 , 146079..

Wang, Y. Y.; Huang, X.; Zhang, X. X. Ultrarobust, tough and highly stretchable self-healing materials based on cartilage-inspired noncovalent assembly nanostructure. Nat. Commun. 2021 , 12 , 1291..

Guo, R.; Zhang, Q.; Wu, Y. S.; Chen, H. B.; Liu, Y. H.; Wang, J. J.; Duan, X. L.; Chen, Q.; Ge, Z. S.; Zhang, Y. F. Extremely strong and tough biodegradable poly(urethane) elastomers with unprecedented crack tolerance via hierarchical hydrogen-bonding interactions. Adv. Mater. 2023 , 35 , 2212130..

Dong, F. H.; Yang, X. X.; Guo, L. Z.; Wang, Y. Q.; Shaghaleh, H.; Huang, Z.; Xu, X.; Wang, S. F.; Liu, H. Self-healing polyurethane with high strength and toughness based on a dynamic chemical strategy. J. Mater. Chem. A 2022 , 10 , 10139−10149..

Hormaiztegui, M. E. V.; Mucci, V. L.; Aranguren, M. I. Composite films obtained from a waterborne biopolyurethane. Incorporation of tartaric acid and nanocellulose. Ind. Crops. Prod. 2019 , 142 , 111879..

Neal, J. A.; Mozhdehi, D.; Guan, Z. B. Enhancing mechanical performance of a covalent self-healing material by sacrificial noncovalent bonds. J. Am. Chem. Soc. 2015 , 137 , 4846−4850..

Wang, Z. T.; Yuan, J.; Wang, X. H.; Zhang, Y. Z.; Wang, Z. Q.; Wang, Y. X.; Guo, B. H.; Shi, J. X.; Xu, J. Strong and anti-impact multi-functional elastomer via hierarchical hydrogen bonding design. Small 2025 , 21 , e2500381..

Wu, J. J.; Ren, M. Q.; Chen, M.; Liu, X. Y.; Jin, T.; Wu, L. L. Self-healing waterborne polyurethane elastomers based on multiple reversible bonds with good mechanical performance for composite conductors. Macromol. Chem. Phys. 2025 , 226 , 2400435..

Shen, R. L.; Lei, C. D.; Long, M. J.; Gao, W.; Yu, G. P.; Tang, J. T. Trajectory controlling and collision warning device based on self-healing and conductive castor oil-based waterborne polyurethane in automated guided vehicles. Adv. Funct. Mater. 2023 , 33 , 2212455..

Zhan, X.; Chen, J.; Yang, Z. Z.; Wu, G. M.; Kong, Z. W. Superhydrophobic film from silicone-modified nanocellulose and waterborne polyurethane through simple sanding process. Int. J. Biol. Macromol. 2023 , 232 , 123431..

Zhang, X. R.; Fu, Q. J.; Wang, Y. C.; Zhao, H. N.; Hao, S. W.; Ma, C.; Xu, F.; Yang, J. Tough liquid-free ionic conductive elastomers with robust adhesion and self-healing properties for ionotronic devices. Adv. Funct. Mater. 2024 , 34 , 2307400..

Hou, L. X.; Ju, H. Q.; Hao, X. P.; Zhang, H. K.; Zhang, L.; He, Z. Y.; Wang, J. J.; Zheng, Q.; Wu, Z. L. Intrinsic anti-freezing and uniq ue phosphorescence of glassy hydrogels with ultrahigh stiffness and toughness at low temperatures. Adv. Mater. 2023 , 35 , 2300244..

Wang, H.; Zhao, Z. M.; Zhang, L. M.; Su, Z. Y.; Chen, C. Y.; Yang, W. J.; Xu, P. W.; Niu, D. Y.; Ma, P. B.; Ma, P. M. High-performance low-temperature self-healing bio-based polyurethane triboelectric nanogenerator for wireless intelligent target systems. Nano Energy 2025 , 133 , 110438..

Sun, C. Q.; Yuan, B. G.; Han, Z.; Yang, D. Z.; Chen, J. C.; Xu, H. J.; Liu, C. T.; Shen, C. Y. Transformation of the strengthening and toughening modes of a poly(urethane) elastomer with hard segments of Ti 3 C 2 MXene and its excellent triboelectric performance. J. Mate. Chem. A. 2024 , 12 , 22112−22119..

Ghosh, G.; Bag, A.; Hanif, A.; Meeseepong, M.; Lee, Y. R.; Lee, N. E. Tough, bio-disintegrable and stretchable substrate reinforced with nanofibers for transient wearable electronics. Adv. Funct. Mater. 2023 , 33 , 2209277..

Liu, Z. X.; Guo, W.; Wang, W. Y.; Guo, Z. J.; Yao, L. F.; Xue, Y.; Liu, Q.; Zhang, Q. Y. Healable strain sensor based on tough and eco-friendly biomimetic supramolecular waterborne polyurethane. ACS Appl. Mater. Interfaces 2022 , 14 , 6016−6027..

Fan, X.; Zhang, L.; Dong, F. H.; Liu, H.; Xu, X. Room-temperature self-healing polyurethane-cellulose nanocrystal composites with strong strength and toughness based on dynamic bonds. Carbohydr. Polym. 2023 , 308 , 120654..

Shao, C. Y.; Wang, M.; Meng, L.; Chang, H. L.; Wang, B.; Xu, F.; Yang, J.; Wan, P. B. Mussel-inspired cellulose nanocomposite tough hydrogels with synergistic self-healing, adhesive, and strain-sensitive properties. Chem. Mater. 2018 , 30 , 3110−3121..

Huang, Y. W.; Xiao, L. Y.; Zhou, J.; Liu, T.; Yan, Y. Q.; Long, S. J.; Li, X. F. Strong tough polyampholyte hydrogels via the synergistic effect of ionic and metal-ligand bonds. Adv. Funct. Mater. 2021 , 31 , 2103917..

Chen, L.; Xu, J. H.; Zhu, M. M.; Zeng, Z. Y.; Song, Y. Y.; Zhang, Y. Y.; Zhang, X. L.; Deng, Y. K.; Xiong, R. H.; Huang, C. B. Self-healing polymers through hydrogen-bond cross-linking: synthesis and electronic applications. Mater. Horiz. 2023 , 10 , 4000−4032..

Ho ng, C.; Li, B.; Zhang, J. J.; Li, Y.; Sun, J. Q. Supramolecular polymer-based ionogels enable large-scale fabrication of stable smart windows with room-temperature closed-loop recyclability and self-healing capability. Adv. Funct. Mater. 2024 , 34 , 2313781..

Wen, J. L.; Xu, G. W.; Liang, Z. P.; Li, S. M.; Wang, Y. M.; Yang, J.; Nie, Y. J. Combing experimental methods and molecular simulations to study self-healing behaviors of polyurethane elastomers containing multiple hydrogen bond networks and flexible blocks. Phys. Chem. Chem. Phys. 2023 , 25 , 28162−28179..

Dufresne, A. Dynamic mechanical analysis of the interphase in bacterial polyester/cellulose whiskers natural composites. Compos. Interfaces 2000 , 7 , 53−67..

Xu, H.; Tu, J.; Ji, J.; Liang, L.; Li, H. Z.; Li, P. Y.; Zhang, X. Z.; Gong, Q. Y.; Guo, X. D. Ultra-high-strength self-healing supramolecular polyurethane based on successive loose hydrogen-bonded hard segment structures. Eur. Polym. J. 2022 , 177 , 111437..

Wang, S. S.; Chen, X. Y.; Guo, L. Z.; Wang, S. S.; Dong, F. H.; Liu, H.; Xu, X. A human muscle-inspired, high strength, good elastic recoverability, room-temperature self-healing, and recyclable polyurethane elastom er based on dynamic bonds. Compos. Sci. Technol. 2024 , 248 , 110457..

Mohamed, M. A.; Rumsey, C. L.; Trebbin, M.; Andreadis, S. T. Multifunctional polyurethane networks combining strength, toughness, and fast autonomous self-healing via the synergy of multiple dynamic bonds. Chem. Mater. 2023 , 35 , 6332−6345..

Zhu, X. B.; Zhang, W. J.; Lu, G. M.; Zhao, H. C.; Wang, L. P. Ultrahigh mechanical strength and robust room-temperature self-healing properties of a polyurethane-graphene oxide network resulting from multiple dynamic bonds. ACS Nano 2022 , 16 , 16724−16735..

Bao, C. Y.; Miao, R. X.; Yin, Y. L.; Xu, Y.; Ding, Y. H.; Liu, J.; Xin, Z. R. Mechanically robust yet body-temperature self-healable polyurethane elastomer via the cross-linking of dynamic boroxines. ACS Appl. Polym. Mater. 2023 , 6 , 797−805..

Duan, X. Y.; Cao, W. H.; He, X. N.; Wang, M. Q.; Cong, R. Y.; Zhang, Z. C.; Ning, C.; Wang, C. S.; Zhao, S. L.; Li, Z. Q.; Gao, W. Realization of dual crosslinked network robust, high toughness self-healing polyurethane elastomers for electronics applications. Chem. Eng. J. 2023 , 476 , 146536..

Guo, C. Y.; Chen, H. R.; Ye, J. F.; Ran, J. M.; Feng, L. B.; Liu, Y. H.; Zhang, J. B.; Li, D. M. Resolving mechanical properties and healing performance trade-off via TiO 2 CuS heterojunction nanoparticles for sunlight-driven self-healing polyurethane. Prog. Org. Coat. 2026 , 211 , 109842..

Xu, X.; Zhao, H. H.; Ji, S. L.; Li, S.; Zhang, L. Q.; Wen, S. P.; Liu, J. High-strength, self-healing waterborne polyurethane elastomers with enhanced mechanical, thermal, and electrical properties. Compos. Commun. 2024 , 51 , 102100..

Fan, Z. J.; Liu, Z.; Zhang, X. D.; Cui, X. X.; Li, H. Z.; Xu, H.; Guo, X. D. A cephalopod-inspired multi-environmental adaptive self-healing polyurethanes. Mater. Today Chem. 2025 , 44 , 102580..

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Multifunctional Polyurethane with High Strength, Toughness, and Self-healing Capacity via Tannic Acid-modified Cellulose Nanocrystals

DOI：10.1007/s10118-026-3670-1

摘要

Abstract

关键词

Keywords

references