Multi-stimuli Responsive Polyurethane-based Materials: Structure-Property Correlations

Yi-Sheng Huang; Han-Xin Jian; Hao Huang; Qing-Yun Guo; Shu-Guang Yang

doi:10.1007/s10118-026-3757-8

Your Location：

Home >

Browse articles >

Multi-stimuli Responsive Polyurethane-based Materials: Structure-Property Correlations

RESEARCH ARTICLE | Updated：2026-07-22

- Multi-stimuli Responsive Polyurethane-based Materials: Structure-Property Correlations
- Chinese Journal of Polymer Science Vol. 44, Pages: 1-13(2026)
- Affiliations：
  
  State Key Laboratory of Advanced Fibers Materials, Center for Advanced Low-dimension Materials, College of Materials Science and Engineering, Donghua University, Shanghai 201620, China
- Author bio：
  
  guoqy@dhu.edu.cn (Q.Y.G.)
  shgyang@dhu.edu.cn (S.G.Y.)
- Funds：
- DOI：10.1007/s10118-026-3757-8
  CLC：
- Received：20 April 2026，
  
  Accepted：27 May 2026，
  
  Online First：22 July 2026，
  
  Published：2026-06
- Accepted：
Scan QR Code
Huang, Y. S.; Jian, H. X.; Huang, H.; Guo, Q. Y.; Yang, S. G. Multi-stimuli responsive polyurethane-based materials: structure-property correlations. Chinese J. Polym. Sci. https://doi.org/10.1007/s10118-026-3757-8

Yi-Sheng Huang, Han-Xin Jian, Hao Huang, et al. Multi-stimuli Responsive Polyurethane-based Materials: Structure-Property Correlations[J/OL]. Chinese Journal of Polymer Science, 2026, 441-13.
Huang, Y. S.; Jian, H. X.; Huang, H.; Guo, Q. Y.; Yang, S. G. Multi-stimuli responsive polyurethane-based materials: structure-property correlations. Chinese J. Polym. Sci. https://doi.org/10.1007/s10118-026-3757-8 DOI：

Yi-Sheng Huang, Han-Xin Jian, Hao Huang, et al. Multi-stimuli Responsive Polyurethane-based Materials: Structure-Property Correlations[J/OL]. Chinese Journal of Polymer Science, 2026, 441-13. DOI： 10.1007/s10118-026-3757-8.

摘要

Abstract

Heat-

light-

and humidity-responsive materials were fabricated

via

chemical design and cold drawing processing. The crystallizable polyether/polyester diols were first reacted with isophorone diisocyanate (IPDI)

followed by chain extension with azobenzene units. The synthesized polyurethanes exhibited ductile behavior and drawing-induced orientation when the soft segments possessed high crystallinity. Upon heating or UV irradiation

the oriented polyurethane strips underwent bending

whereas the pristine strips did not. Under humid conditions

both oriented and pristine polyurethane strips containing poly(ethylene oxide) (PEO) soft segments bent

albeit in opposite directions. In contrast

polyurethane strips with polycaprolactone (PCL) and polytetramethylene ether glycol (PTMEG) soft segments showed no response to humidity

regardless of whether they were stretched. Mechanistic investigations revealed that the temperature increase resulting from the photothermal effect of the azobenzene moieties is the main reason for light-induced actuation

which differ

s from that in many other azobenzene-based materials. The entropic elastic energy stored during stretching is released upon UV irradiation

heating

or humidification to drive the bending deformation. This work presents a strategy for constructing multi-stimuli- responsive materials

via

molecular design and post-processing

highlighting the synergy between functional moieties and microscopic structures

which holds great significance for the development of advanced intelligent materials.

关键词

Keywords

references

Zhang, K. Y.; Liu, S.; Zhao, Q.; Huang, W. Stimuli–responsive metallopolymers. Coord. Chem. Rev. 2016 , 319 , 180−195..

Santos, A.; Balderrama, V. S.; Alba, M.; Formentín, P.; Ferré-Borrull, J.; Pallarès, J.; Marsal, L. F. Nanoporous Anodic alumina barcodes: towards smart optical biosensors. Adv. Mater. 2012 , 24 , 1050−1054..

Rogóż, M.; Zeng, H.; Xuan, C.; Wiersma, D. S.; Wasylczyk, P. Light-Driven soft robot mimics caterpillar locomotion in natural scale. Adv. Opt. Mater. 2016 , 4 , 1689−1694..

Sagara, Y.; Yamane, S.; Mitani, M.; Weder, C.; Kato, T. Mechanoresponsive luminescent molecular assemblies: an emerging class of materials. Adv. Mater. 2016 , 28 , 1073−1095..

Mackanic, D. G.; Kao, M.; Bao, Z. Enabling deformable and stretchable batteries. Adv. Energy Mater. 2020 , 10 , 2001424..

Roach, D. J.; Yuan, C.; Kuang, X.; Li, V. C. F.; Blake, P.; Romero, M. L.; Hammel, I.; Yu, K.; Qi, H. J. Long liquid crystal elastomer fibers with large reversible actuation strains for smart textiles and artificial muscles. ACS Appl. Mater. Interfaces. 2019 , 11 , 19514−19521..

Hu, J.; Meng, H.; Li, G.; Ibekwe, S. I. A review of stimuli-responsive polymers for smart textile applications. Smart Mater. Struct. 2012 , 21 , 053001..

Pilz da Cunha, M.; Ambergen, S.; Debije, M. G.; Homburg, E. F. G. A.; den Toonder, J. M. J.; Schenning, A. P. H. J. A soft transporter robot fueled by light. Adv. Sci. 2020 , 7 , 1902842..

Lugger, S. J. D.; Houben, S. J. A.; Foelen, Y.; Debije, M. G.; Schenning, A. P. H. J.; Mulder, D. J. Hydrogen-bonded supramolecular liquid crystal polymers: smart materials with stimuli-responsive, self-healing, and recyclable properties. Chem. Rev. 2022 , 122 , 4946−4975..

Ma, Y.; She, P.; Zhang, K. Y.; Yang, H.; Qin, Y.; Xu, Z.; Liu, S.; Zhao, Q.; Huang, W. Dynamic metal-ligand coordination for multicolour and water-jet rewritable paper. Nat. Commun. 2018 , 9 , 3..

She, P.; Qin, Y.; Wang, X.; Zhang, Q. Recent progress in external-stimulus-responsive 2D covalent organic frameworks. Adv. Mater. 2022 , 34 , 2101175..

Wang, J.; Zhao, Q.; Wang, Y.; Zeng, Q.; Wu, T.; Du, X. Self-unfolding flexible microelectrode arrays based on shape memory polymers. Adv. Mater. Technol. 2019 , 4 , 1900566..

Huang, Y.; Ning, L.; Zhang, X.; Zhou, Q.; Gong, Q.; Zhang, Q. Stimuli-fluorochromic smart organic materials. Chem. Soc. Rev. 2024 , 53 , 1090−1166..

Yang, P.; Zhu, F.; Zhang, Z.; Cheng, Y.; Wang, Z.; Li, Y. Stimuli-responsive polydopamine-based smart materials. Chem. Soc. Rev. 2021 , 50 , 8319−8343..

Xiao, Y. Y.; Jiang, Z. C.; Tong, X.; Zhao, Y. Biomimetic locomotion of electrically powered “Janus” soft robots using a liquid crystal polymer. Adv. Mater. 2019 , 31 , 1903452..

Yang, Q.; Peng, C.; Ren, J.; Zhao, W.; Zheng, W.; Zhang, C.; Hu, Y.; Zhang, X. A near-infrared photoactuator based on shape memory semicrystalline polymers towards light-fueled crane, grasper, and walker. Adv. Opt. Mater. 2019 , 7 , 1900784..

Huang, T.; Su, Z.; Hou, K.; Zeng, J.; Zhou, H.; Zhang, L.; Nunes, S. P. Advanced stimuli-responsive membranes for smart separation. Chem. Soc. Rev. 2023 , 52 , 4173−4207..

Zhuang, J.; Gordon, M. R.; Ventura, J.; Li, L.; Thayumanavan, S. Multi-stimuli responsive macromolecules and their assemblies. Chem. Soc. Rev. 2013 , 42 , 7421−7435..

Jochum, F. D.; Theato, P. Temperature- and light-responsive smart polymer materials. Chem. Soc. Rev. 2013 , 42 , 7468−7483..

Li, X.; Cai, X.; Gao, Y.; Serpe, M. J. Reversible bidirectional bending of hydrogel-based bilayer actuators. J. Mater. Chem. B. 2017 , 5 , 2804−2812..

Yamada, M.; Kondo, M.; Mamiya, J.-i.; Yu, Y.; Kinoshita, M.; Barrett, C. J.; Ikeda, T. Photomobile polymer materials: towardss light-driven plastic motors. Angew. Chem. Int. Ed. 2008 , 47 , 4986−4988..

Zhang, C.; Zhang, Z.; Liu, X. Closed-loop recyclable and totally renewable liquid crystal networks with room-temperature programmability and reconfigurable functionalities. Angew. Chem. Int. Ed. 2024 , 63 , e202411280..

Lang, C.; Lloyd, E. C.; Matuszewski, K. E.; Xu, Y.; Ganesan, V.; Huang, R.; Kumar, M.; Hickey, R. J. Nanostructured block copolymer muscles. Nat. Nanotechnol. 2022 , 17 , 752−758..

Yao, X.; Chen, H.; Qin, H.; Wu, Q. H.; Cong, H.-P.; Yu, S.-H. Solvent-adaptive hydrogels with lamellar confinement cellular structure for programmable multimodal locomotion. Nat. Commun. 2024 , 15 , 9254..

Guan, G.; Wu, M.; Han, M. Y. Stimuli-responsive hybridized nanostructures. Adv. Funct. Mater. 2020 , 30 , 1903439..

Wei, M.; Gao, Y.; Li, X.; Serpe, M. J. Stimuli-responsive polymers and their applications. Polym. Chem. 2017 , 8 , 127−143..

Hu, L.; Wan, Y.; Zhang, Q.; Serpe, M. J. Harnessing the power of stimuli-responsive polymers for actuation. Adv. Funct. Mater. 2020 , 30 , 1903471..

Hu, L.; Zhang, Q.; Li, X. ; Serpe, M. J. Stimuli-responsive polymers for sensing and actuation. Mater. Horiz. 2019 , 6 , 1774−1793..

Yan, H.; Jiang, Q.; Wang, J.; Cao, S.; Qiu, Y.; Wang, H.; Liao, Y.; Xie, X. A triple-stimuli responsive supramolecular hydrogel based on methoxy-azobenzene-grafted poly(acrylic acid) and β-cyclodextrin dimer. Polymer 2021 , 221 , 123617..

Chikh Alard, I.; Soubhye, J.; Berger, G.; Gelbcke, M.; Spassov, S.; Amighi, K.; Goole, J.; Meyer, F. Triple-stimuli responsive polymers with fine tuneable magnetic responses. Polym. Chem. 2017 , 8 , 2450−2456..

Li, X.; Han, J.; Wang, X.; Zhang, Y.; Jia, C.; Qin, J.; Wang, C.; Wu, J.-R.; Fang, W.; Yang, Y. W. A triple-stimuli responsive hormone delivery system equipped with pillararene magnetic nanovalves. Mater. Chem. Front. 2019 , 3 , 103−110..

Yan, H.; Wang, J.; He, X.; Yu, D.; Qiu, Y.; Liao, Y.; Xie, X. A quadruple-stimuli responsive supramolecular hydrogel constructed from a poly(acrylic acid) derivative and β-cyclodextrin dimer. Soft Matter 2024 , 20 , 5343−5350..

Chen, Y.; Li, H.; Zhang, Y.; Li, Z.; Yang, D. Eu 3+ -directed supramolecular metallogels with reversible quadruple-stimuli response behaviors. Small 2024 , 20 , 2309542..

Yang, J.; Dai, D.; Lou, X.; Ma, L.; Wang, B.; Yang, Y.-W. Supramolecular nanomaterials based on hollow mesoporous drug carriers and macrocycle-capped CuS nanogates for synergistic chemo-photothermal therapy. Theranostics 2020 , 10 , 615−629..

Shang, J.; Theato, P. Smart composite hydrogel with pH-, ionic strength- and temperature-induced actuation. Soft Matter 2018 , 14 , 8401−8407..

Huang, X.; Jiang, X.; Yang, Q.; Chu, Y.; Zhang, G.; Yang, B.; Zhuo, R. Triple-stimuli (pH/thermo/reduction) sensitive copolymers for intracellular drug delivery. J. Mater. Chem. B 2013 , 1 , 1860−1868..

Xu, W.; Qian, J.; Hou, G.; Wang, Y.; Wang, J.; Sun, T.; Ji, L.; Suo, A.; Yao, Y. A dual-targeted hyaluronic acid-gold nanorod platform with triple-stimuli responsiveness for photodynamic/photothermal therapy of breast cancer. Acta Bio. 2019 , 83 , 400−413..

Zhang, X.; Gao, J.; Zhao, X.; Liu, Z.; Liu, Z.; Wang, K.; Li, G.; Jiang, J. Hyperbranched polymer micelles with triple-stimuli backbone-breakable iminoboronate ester linkages. Chinese Chem. Lett. 2020 , 31 , 1822−1826..

Gao, W.; Bigham, A.; Ghomi, M.; Zarrabi, A.; Rabiee, N.; Saeb, M. R.; Nuri Ertas, Y.; Goel, A.; Sharifi, E.; Ashrafizadeh, M.; Sethi, G.; Tambuwala, M. M.; Wang, Y.; Ghaffarlou, M.; Jiao, T. Micelle-engineered nanoplatforms for precision oncology. Chem. Eng. J. 2024 , 495 , 153438..

Mei, G.; Su, Z.; Liu, N.; Qu, J.; Liu, X.; Qian, D.; Zhou, X.; Liu, Z. Robust artificial spider silk via synergistic cross-linking of slide-ring and covalent bonds. Macromolecules 2025 , 58 , 10738−10751..

Li, J.; Mei, G.; Fang, S.; Liu, X.; Liu, S.; Liu, Y.; Yang, Z.; Han, X.; Wang, M.; Xiao, Y.; Chang, W.; Guo, W.; Zhao, W.; Zhang, G.; Zhang, Z.; Li, C.; Zhang, M.; Bai, J.; Zhou, X.; Baughman, R. H.; Liu, Z. Creating nanoknot-like domains for robust artificial spider silk towards high twistocaloric performance. Adv. Mater. 2026 , 38 , e16934..

Li, Z.; Zhu, Y.-L.; Niu, W.; Yang, X.; Jiang, Z.; Lu, Z. -Y.; Liu, X.; Sun, J. Healable and recyclable elastomers with record-high mechanical robustness, unprecedented crack tolerance, and superhigh elastic restorability. Adv. Mater. 2021 , 33 , 2101498..

McCune, J. A.; Mommer, S.; Parkins, C. C.; Scherman, O. A. Design principles for aqueous interactive materials: lessons from small molecules and stimuli-responsive systems. Adv. Mater. 2020 , 32 , 1906890..

He, W.; Wang, M.; Mei, G.; Liu, S.; Khan, A. Q.; Li, C.; Feng, D.; Su, Z.; Bao, L.; Wang, G.; Liu, E.; Zhu, Y.; Bai, J.; Zhu, M.; Zhou, X.; Liu, Z. Establishing superfine nanofibrils for robust polyelectrolyte artificial spider silk and powerful artificial muscles. Nat. Commun. 2024 , 15 , 3485..

Li, Y.; Schreiber, S.; Yang, H.; Liu, M.; Little, J. M.; Cao, W.; Luo, Y.; Bao, Y.; Shih, C. J.; Bai, H.; Chen, P. Y. From molecules to machines: a multiscale roadmap to intelligent, multifunctional soft robotics. Chem. Rev. 2025 , 125 , 8123−8245..

Kumar, N.; Singh, S.; Sharma, P.; Kumar, B.; Kumar, A. Single-, dual-, and multi-stimuli-responsive nanogels for biomedical applications. Gels 2024 , 10 , 61..

Wojtecki, R. J.; Meador, M. A.; Rowan, S. J. Using the dynamic bond to access macroscopically responsive structurally dynamic polymers. Nat. Mater. 2011 , 10 , 14−27..

Rice, A. M.; Martin, C. R.; Galitskiy, V. A.; Berseneva, A. A.; Leith, G. A.; Shustova, N. B. Photophysics modulation in photoswitchable metal-organic frameworks. Chem. Rev. 2020 , 120 , 8790−8813..

Zhu, S.; Wang, S.; Huang, Y.; Tang, Q.; Fu, T.; Su, R.; Fan, C.; Xia, S.; Lee, P. S.; Lin, Y. Bioinspired structural hydrogels with highly ordered hierarchical orientations by flow-induced alignment of nanofibrils. Nat. Commun. 2024 , 15 , 118..

Wang, L.; Li, Q. Photochromism into nanosystems: towardss lighting up the future nanoworld. Chem. Soc. Rev. 2018 , 47 , 1044−1097..

Nguyen, T. H. L.; Gigant, N.; Joseph, D. Advances in direct metal-catalyzed functionalization of azobenzenes. ACS Catal. 2018 , 8 , 1546−1579..

Jian, H.; Wang, W.; Yao, Y.; Yang, Y.; Huang, Y.; Huang, H.; Yang, S. Cold drawing of azobenzene incorporated poly(urethane urea)s for heat, humidity and light responsiveness. Polymer 2026 , 343 , 129449..

Tian, J.; Zhou, Z.; Miao, X.; Wang, S.; Ming, Y.; Nie, Y.; Ma, Y.; Li, Z. Supertough, resilient, and healable thermoplastic poly(urethane urea) elastomers by densepacking of hydrogen-bonding arrays. Adv. Funct. Mater. 2026 , 36 , e04882..

Wang, L.; Guo, L.; Zhang, K.; Xia, Y.; Hao, J.; Wang, X. Development of tough thermoplastic elastomers by leveraging rigid–flexible supramolecular segment interplays. Angew. Chem. Int. Ed. 2023 , 62 , e202301762..

Wang, X.; Xu, J.; Zhang, Y.; Wang, T.; Wang, Q.; Li, S.; Yang, Z.; Zhang, X. A stretchable, mechanically robust polymer exhibiting shape-memory-assisted self-healing and clustering-triggered emission. Nat. Commun. 2023 , 14 , 4712..

Bandara, H. M. D.; Burdette, S. C. Photoisomerization in different classes of azobenzene. Chem. Soc. Rev. 2012 , 41 , 1809−1825..

Gelebart, A. H.; Jan Mulder, D.; Varga, M.; Konya, A.; Vantomme, G.; Meijer, E. W.; Selinger, R. L. B.; Broer, D. J. Making waves in a photoactive polymer film. Nature 2017 , 546 , 632−636..

Hartley, G. S. The cis -form of azobenzene. Nature 1937 , 140 , 281−281..

Rau, H.; Lueddecke, E. On the rotation-inversion controversy on photoisomerization of azobenzenes. Experimental proof of inversion. J. Am. Chem. Soc. 1982 , 104 , 1616−1620..

Verpaalen, R. C. P.; Varghese, S.; Froyen, A.; Pilz da Cunha, M.; Pouderoijen, M. J.; Severn, J. R.; Bhatti, M. R.; Peijs, T.; Bastiaansen, C. W. M.; Debije, M. G.; Engels, T. A. P.; Schenning, A. P. H. J. Fast, light-responsive, metal-like polymer actuators generating high stresses at low strain. Matter 2020 , 2 , 1522−1534..

Bhatti, M. R. A.; Bilotti, E.; Zhang, H.; Bastiaansen, C. W. M.; Peijs, T. Photo-thermal actuation of ultra-drawn high-density polyethylene. Polymer 2020 , 207 , 122897..

Varghese, S.; Fredrich, S.; Vantomme, G.; Prabhu, S. R.; Teyssandier, J.; De Feyter, S.; Severn, J.; Bastiaansen, C. W. M.; Schenning, A. P. H. J. Epitaxial growth of light-responsive azobenzene molecular crystal actuators on oriented polyethylene films. J. Mater. Chem. C. 2020 , 8 , 694−699..

Liu, Z.; Huang, H.; Yin, P.; Zhang, C.; Yang, S. Dynamics of hydrogen-bonded polymer complexes of poly(ether oxide) and poly(acrylic acid): time-humidity-temperature equivalence. Polymer 2025 , 320 , 128080..

Huang, H.; Liu, Z.; Jian, H.; Yao, Y.; Tan, W.; Yang, S. Alginate/chitosan complex fibers reinforcement and their mechanical transition continuum with water uptake increasing. Macromol. Rapid Commun. 2025 , 46 , 2400735..

Wang, W.; Jian, H.; Huang, H.; Feng, F.; Meng, Q.; Li, Y.; Chen, G.; Yang, S. Structure, humidity adaptivity, and elasticity of hydrogen-bonded complexes formed by self-assembly of a triblock copolymer and a homopolymer. Polym. Chem. 2024 , 15 , 4710−4720..

Huang, H.; Liu, Z.; Jian, H.; Yao, Y.; Xue, B.; Yang, S. Humidity-adaptive behaviors of alginate/chitosan complex fiber. ACS Appl. Polym. Mater. 2024 , 6 , 4634−4641..

C. Zhang, W. Wang, H. Huang, Z. Liu, S. Yang. Effect of humidity on mechanical behavior of polymer hydrogen-bonding complex fibers. Acta Polymerica Sinica (in Chinese), 2023 , 54 , 1772−1783..

Views

Downloads

CSCD

Alert me when the article has been cited

Submit

Tools

Publicity Resources

Stimuli-responsive Perovskite Hybrid Films towards Multi-mode and Dual-key Multi-level Information Encryption

Direct Observation of Early-Stage Polymer Crystallization Driven by Surface Wrinkling and Compressive Stress in Thin Films

Chain Flexibility and Connectivity: The Uniqueness of Polymer Crystallization

Melting and Annealing Peak Temperatures of Poly(butylene succinate) on the Same Hoffman-Weeks Plot Parallel to Tm=Tc Line

Durable Anti-fogging and Abrasion-resistant Coatings Based on Polyoxometalates-Hydrophilic Resin Composites with Enhanced Cohesion and Adhesion

Related Author

Gang Zou

Hong-Li Zhang

Yi-Fan Xie

Xiang-Xiang Xu

Di Wang

Jia-He Li

Ze-Yu Feng

Cong-Yang Ye

Related Institution

State Key Laboratory of Precision and Intelligent Chemistry, Department of Polymer Science and Engineering, School of Chemistry and Materials Science, University of Science and Technology of China

State Key Laboratory of Polymer Physics and Chemistry, Changchun Institute of Applied Chemistry, Graduate University of Chinese Academy of Sciences, Chinese Academy of Sciences

Heinz Maier-Leibnitz-Zentrum (MLZ), Technical University of Munich, Lichtenbergstr. 1, Garching

Technical University of Munich, TUM School of Natural Sciences, Department of Physics, Chair for Functional Materials, James-Franck-Str. 1, Garching

Department of Fibre and Polymer Technology, KTH Royal Institute of Technology, Teknikringen 56–58, Stockholm SE

⁰