A facile approach toward scalable fabrication of reversible shape-memory polymers with bonded elastomer microphases as internal stress provider
Abstract
The present communication reports a novel strategy to fabricate reversible shape-memory polymer that operates without the aid of external force on the basis of a two-phase structure design. The proof-of-concept material, crosslinked styrene-butadiene-styrene block copolymer (SBS, dispersed phase)/polycaprolactone-based polyurethane (PU, continuous phase) blend, possesses a closely connected microphase separation structure. That is, SBS phases are chemically bonded to crosslinked PU by means of a single crosslinking agent and two-step crosslinking process for increasing integrity of the system. Miscibility between components in the blend is no longer critical by taking advantage of the reactive blending technique. It is found that a suitable programming leads to compressed SBS, which serves as internal expansion stress provider as a result. The desired two-way shape-memory effect is realized by the joint action of the temperature-induced reversible opposite directional deformabilities of the crystalline phase of PU and compressed SBS, accompanying melting and orientated recrystallization of the former. Owing to the broadness of material selection and manufacturing convenience, the proposed approach opens an avenue toward mass production and application of the smart polymer.
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The two-stage cross-linking method has been used to fabricate stress-free two-way SMPs.
“The two-stage cross-linking method has been used to fabricate stress-free two-way SMPs, i.e., class (ii); e.g., in [136-138].”
From Two-Way and Multiple-Way Shape Memory Polymers for Soft Robotics: An Overview (2020) · cites this paper as [138]
Cites
Light-induced shape-memory polymers
Lendlein, A., Jiang, H., Jünger, O., & Langer, R. (2005) · Nature · doi:10.1038/nature03496 · Cited by 2,006 · see citing works
Review of progress in shape-memory polymers
Liu, C., Qin, H., & Mather, P. T. (2007) · Journal of Materials Chemistry · doi:10.1039/b615954k · Cited by 1,942 · see citing works
Zhao, Q., Qi, H. J., & Xie, T. (2015) · Progress in Polymer Science · doi:10.1016/j.progpolymsci.2015.04.001 · Cited by 1,409 · see citing works
Hu, J., Zhu, Y., Huang, H., & Lu, J. (2012) · Progress in Polymer Science · doi:10.1016/j.progpolymsci.2012.06.001 · Cited by 1,279 · see citing works
Photomechanics of Liquid‐Crystalline Elastomers and Other Polymers
Ikeda, T., Mamiya, J., & Yu, Y. (2007) · Angewandte Chemie International Edition · doi:10.1002/anie.200602372 · Cited by 1,022 · see citing works
Shape memory polymers: Past, present and future developments
Hager, M. D., Bode, S., Weber, C., & Schubert, U. S. (2015) · Progress in Polymer Science · doi:10.1016/j.progpolymsci.2015.04.002 · Cited by 950 · see citing works
Mohr, R., Kratz, K., Weigel, T., Lucka-Gabor, M., Moneke, M., & Lendlein, A. (2006) · Proceedings of the National Academy of Sciences · doi:10.1073/pnas.0600079103 · Cited by 819 · see citing works
Liquid crystal elastomers with mechanical properties of a muscle
Thomsen, D. L., Keller, P., Naciri, J., Pink, R., Jeon, H., Shenoy, D., & Ratna, B. R. (2001) · Macromolecules · doi:10.1021/ma001639q · Cited by 689 · see citing works
Two-Way Reversible Shape Memory in a Semicrystalline Network
Chung, T., Romo-Uribe, A., & Mather, P. T. (2008) · Macromolecules · doi:10.1021/ma071517z · Cited by 531 · see citing works
Reversible bidirectional shape-memory polymers
Behl, M., Kratz, K., Zotzmann, J., Nöchel, U., & Lendlein, A. (2013) · Advanced Materials · doi:10.1002/adma.201300880 · Cited by 496 · see citing works
Poly(ε-caprolactone) Polyurethane and Its Shape-Memory Property
Ping, P., Wang, W., Chen, X., & Jing, X. (2005) · Biomacromolecules · doi:10.1021/bm049477j · Cited by 354 · see citing works
Self-citationBioinspired mechanically adaptive polymer nanocomposites with water-activated shape-memory effect
Mendez, J., Annamalai, P. K., Eichhorn, S. J., Rusli, R., Rowan, S. J., Foster, E. J., & Weder, C. (2011) · Macromolecules · doi:10.1021/ma201502k · Cited by 319 · see citing works
Temperature-memory polymer actuators
Behl, M., Kratz, K., Noechel, U., Sauter, T., & Lendlein, A. (2013) · Proceedings of the National Academy of Sciences · doi:10.1073/pnas.1301895110 · Cited by 313 · see citing works
Semi-crystalline two-way shape memory elastomer
Li, J., Rodgers, W. R., & Xie, T. (2011) · Polymer · doi:10.1016/j.polymer.2011.09.030 · Cited by 220 · see citing works
Polyurethane ionomers having shape memory effects
Kim, B. K., Lee, S. Y., Lee, J. S., Baek, S. H., Choi, Y. J., Lee, J. O., & Xu, M. (1998) · Polymer · doi:10.1016/s0032-3861(97)00616-2 · Cited by 215 · see citing works
Shapeshifting: Reversible shape memory in semicrystalline elastomers
Zhou, J., Turner, S. A., Brosnan, S. M., Li, Q., Carrillo, J.-M. Y., Nykypanchuk, D., Gang, O., Ashby, V. S., Dobrynin, A. V., & Sheiko, S. S. (2014) · Macromolecules · doi:10.1021/ma4023185 · Cited by 209 · see citing works
Combined one-way and two-way shape memory in a glass-forming nematic network
Qin, H., & Mather, P. T. (2009) · Macromolecules · doi:10.1021/ma8022926 · Cited by 179 · see citing works
Chen, E.-C., & Wu, T. (2007) · Polymer Degradation and Stability · doi:10.1016/j.polymdegradstab.2007.02.019 · Cited by 178 · see citing works
Two-way shape memory effect in polymer laminates
Chen, S., Hu, J., Zhuo, H., & Zhu, Y. (2008) · Materials Letters · doi:10.1016/j.matlet.2008.05.073 · Cited by 158 · see citing works
Two-way shape memory polymer with “switch–spring” composition by interpenetrating polymer network
Wu, Y., Hu, J., Han, J., Zhu, Y., Huang, H., Li, J., & Tang, B. (2014) · J. Mater. Chem. A · doi:10.1039/c4ta03640a · Cited by 144 · see citing works
Ji, F. L., Hu, J. L., Li, T. C., & Wong, Y. W. (2007) · Polymer · doi:10.1016/j.polymer.2007.06.032 · Cited by 137 · see citing works
Properties and mechanism of two-way shape memory polyurethane composites
Chen, S., Hu, J., & Zhuo, H. (2010) · Composites Science and Technology · doi:10.1016/j.compscitech.2010.01.017 · Cited by 134 · see citing works
Shape actuation via internal stress-induced crystallization of dual-cure networks
Meng, Y., Jiang, J., & Anthamatten, M. (2015) · ACS Macro Letters · doi:10.1021/mz500773v · Cited by 134 · see citing works
Pandini, S., Baldi, F., Paderni, K., Messori, M., Toselli, M., Pilati, F., Gianoncelli, A., Brisotto, M., Bontempi, E., & Riccò, T. (2013) · Polymer · doi:10.1016/j.polymer.2013.06.016 · Cited by 122 · see citing works
A tough shape memory polymer with triple shape memory and two-way shape memory properties
Bai, Y., Zhang, X., Wang, Q., & Wang, T. (2014) · Journal of Materials Chemistry A · doi:10.1039/c3ta15117d · Cited by 115 · see citing works
Two‐Way Shape Changes of a Shape‐Memory Poly(ester urethane)
Bothe, M., & Pretsch, T. (2012) · Macromolecular Chemistry and Physics · doi:10.1002/macp.201200096 · Cited by 92 · see citing works
Baker, R. M., Henderson, J. H., & Mather, P. T. (2013) · Journal of Materials Chemistry B · doi:10.1039/c3tb20810a · Cited by 92 · see citing works
Crystallization under Strain and Resultant Orientation of Poly(ε-caprolactone) in Miscible Blends
Zhao, Y., Keroack, D., & Prud'homme, R. E. (1999) · Macromolecules · doi:10.1021/ma981416o · Cited by 75 · see citing works
Effects of carbon black nanoparticles on two-way reversible shape memory in crosslinked polyethylene
Ma, L., Zhao, J., Wang, X., Chen, M., Liang, Y., Wang, Z., Yu, Z., & Hedden, R. C. (2014) · Polymer · doi:10.1016/j.polymer.2014.11.036 · Cited by 71 · see citing works
Two-way shape memory behavior of shape memory polyurethanes with a bias load
Hong, S. J., Yu, W., & Youk, J. H. (2010) · Smart Materials and Structures · doi:10.1088/0964-1726/19/3/035022 · Cited by 69 · see citing works
Thermo-responsive two-way shape changeable polymeric laminate
Tamagawa, H. (2010) · Materials Letters · doi:10.1016/j.matlet.2009.12.053 · Cited by 56 · see citing works
Electroactive two‐way shape memory polymer laminates
Chen, S., Yang, S.-X., Li, Z., Xu, S., Yuan, H., Chen, S., & Ge, Z. (2014) · Polymer Composites · doi:10.1002/pc.22958 · Cited by 40 · see citing works
In situtemperature tunable pores of shape memory polyurethane membranes
Ahn, J.-S., Yu, W., Youk, J. H., & Ryu, H. Y. (2011) · Smart Materials and Structures · doi:10.1088/0964-1726/20/10/105024 · Cited by 32 · see citing works
Flagged first, then by citations
Cited by
Sorted by citations
Thermally-induced two-way shape memory polymers: Mechanisms, structures, and applications
Zare, M., Prabhakaran, M. P., Parvin, N., & Ramakrishna, S. (2019) · Chemical Engineering Journal · doi:10.1016/j.cej.2019.05.167 · Cited by 330 · see citing works
Advanced functional polymer materials
Wang, K., Amin, K., An, Z., Cai, Z., Chen, H., Chen, H., Dong, Y., Feng, X., Fu, W., Gu, J., et al. (2020) · Materials Chemistry Frontiers · doi:10.1039/d0qm00025f · Cited by 245 · see citing works
Self-citationMultiple and two-way reversible shape memory polymers: Design strategies and applications
Wang, K., Jia, Y.-G., Zhao, C., & Zhu, X. X. (2019) · Progress in Materials Science · doi:10.1016/j.pmatsci.2019.100572 · Cited by 208 · see citing works
Two-Way and Multiple-Way Shape Memory Polymers for Soft Robotics: An Overview
Scalet, G. (2020) · Actuators · doi:10.3390/act9010010 · Cited by 209 · see citing works
Wang, X., He, Y., Liu, Y., & Leng, J. (2022) · Materials Science and Engineering R Reports · doi:10.1016/j.mser.2022.100702 · Cited by 137 · see citing works
Fan, L. F., Rong, M. Z., Zhang, M. Q., & Chen, X. (2018) · ACS Applied Materials & Interfaces · doi:10.1021/acsami.8b15636 · Cited by 138 · see citing works
Self-citationSelf-healable functional polymers and polymer-based composites
Zhang, Z. P., Rong, M. Z., & Zhang, M. Q. (2023) · Progress in Polymer Science · doi:10.1016/j.progpolymsci.2023.101724 · Cited by 127 · see citing works
Self-citationShape-Memory Polymeric Artificial Muscles: Mechanisms, Applications and Challenges
Chen, Y., Chen, C., Rehman, H. U., Xu, Z., Li, H., Liu, H., & Hedenqvist, M. S. (2020) · Molecules · doi:10.3390/molecules25184246 · Cited by 98 · see citing works
Fan, L. F., Rong, M. Z., Zhang, M. Q., & Chen, X. (2018) · Journal of Materials Chemistry A · doi:10.1039/c8ta05751f · Cited by 95 · see citing works
Self-citationHuang, J., Cao, L., Yuan, D., & Chen, Y. (2018) · ACS Sustainable Chemistry & Engineering · doi:10.1021/acssuschemeng.8b05025 · Cited by 94 · see citing works
Enyan, M., Zhang, B., Amu‐Darko, J. N. O., Issaka, E., Otoo, S. L., & Agyemang, M. F. (2024) · Journal of Thermoplastic Composite Materials · doi:10.1177/08927057241248028 · Cited by 75 · see citing works
Qi, X., Pan, C., Zhang, L., & Yue, D. (2023) · ACS Applied Materials & Interfaces · doi:10.1021/acsami.2c19782 · Cited by 74 · see citing works
Zare, M., Davoodi, P., & Ramakrishna, S. (2021) · Nanomaterials · doi:10.3390/nano11040933 · Cited by 71 · see citing works
Towards high performance and durable soft tactile actuators
Tan, M., Wang, H., Gao, D., Huang, P.-W., & Lee, P. S. (2024) · Chemical Society Reviews · doi:10.1039/d3cs01017a · Cited by 69 · see citing works
Du, L., Xu, Z., Huang, C.-L., Zhao, F.-Y., Fan, C., Dai, J., Yang, K., & Wang, Y. (2019) · Applied Materials Today · doi:10.1016/j.apmt.2019.100463 · Cited by 59 · see citing works
Zhou, J., Yue, H., Huang, M., Hao, C., He, S., Liu, H., Liu, W., Zhu, C., Dong, X., & Wang, D. (2021) · ACS Applied Materials & Interfaces · doi:10.1021/acsami.1c13057 · Cited by 51 · see citing works
Inverardi, N., Toselli, M., Scalet, G., Messori, M., Auricchio, F., & Pandini, S. (2022) · Macromolecules · doi:10.1021/acs.macromol.2c01064 · Cited by 50 · see citing works
Fan, L. F., Rong, M. Z., Zhang, M. Q., & Chen, X. (2018) · Macromolecular Rapid Communications · doi:10.1002/marc.201700714 · Cited by 50 · see citing works
Self-citationExternal Stress-Free Reversible Multiple Shape Memory Polymers
Huang, Y. N., Fan, L. F., Rong, M. Z., Zhang, M. Q., & Gao, Y. (2019) · ACS Applied Materials & Interfaces · doi:10.1021/acsami.9b10052 · Cited by 45 · see citing works
Self-citationDong, K., Chen, Z., Momo, Z. Y., Jiani, W., Xuan, C., Yu, X., & Xueliang, X. (2019) · Smart Materials and Structures · doi:10.1088/1361-665x/ab5e6d · Cited by 44 · see citing works
Fan, L. F., Huang, Y. N., Rong, M. Z., Zhang, M. Q., & Chen, X. (2019) · ACS Macro Letters · doi:10.1021/acsmacrolett.9b00467 · Cited by 39 · see citing works
Self-citationShape memory polymer-based thermal-responsive circuit switches
Jia, J., Wang, J., & Wang, Y. (2023) · Journal of Materials Chemistry C · doi:10.1039/d3tc00848g · Cited by 35 · see citing works
Han, J., Lai, S., & Chiu, Y. T. (2018) · Polymers for Advanced Technologies · doi:10.1002/pat.4309 · Cited by 34 · see citing works
Styrene‐butadiene‐styrene ‐based shape memory polymers: Evolution and the current state of art
Basak, S., & Bandyopadhyay, A. (2022) · Polymers for Advanced Technologies · doi:10.1002/pat.5682 · Cited by 34 · see citing works
Wang, Z., Zhou, J., Liang, H., Ye, S., Zou, J., & Yang, H. (2020) · Progress in Organic Coatings · doi:10.1016/j.porgcoat.2020.105943 · Cited by 32 · see citing works
Lai, S., & Guo, G.-L. (2019) · Polymer Testing · doi:10.1016/j.polymertesting.2019.05.008 · Cited by 31 · see citing works
Yuan, S. J., Peng, Z. Q., Rong, M. Z., & Zhang, M. Q. (2022) · Materials Chemistry Frontiers · doi:10.1039/d2qm00090c · Cited by 29 · see citing works
Self-citationXu, C., Cui, R., Chen, Y., & Ding, J. (2019) · Composites Part B Engineering · doi:10.1016/j.compositesb.2019.107532 · Cited by 27 · see citing works
High-performance fibrous artificial muscle based on reversible shape memory UHMWPE
Li, Y., Min, L., Xin, J. H., Wang, L. H., Wu, Q. H., Fan, L. F., Gan, F., & Yu, H. (2022) · Journal of Materials Research and Technology · doi:10.1016/j.jmrt.2022.07.045 · Cited by 24 · see citing works
Self-citationWang, T., Liu, Y., Zhao, J., Zhang, H., & Zhang, Z. (2020) · Smart Materials and Structures · doi:10.1088/1361-665x/ab7f40 · Cited by 23 · see citing works
Yu, Y. Y., Xiang, H., Fan, L. F., & Zhang, M. Q. (2025) · Polymer science & technology. · doi:10.1021/polymscitech.4c00035 · Cited by 23 · see citing works
Self-citationHuang, Y., Dang, G., Zhu, M., Fan, L. F., Rong, M. Z., & Zhang, M. (2022) · Applied Materials Today · doi:10.1016/j.apmt.2022.101709 · Cited by 22 · see citing works
Self-citationRen, S., & Feng, J. (2020) · Journal of Materials Chemistry C · doi:10.1039/d0tc00086h · Cited by 20 · see citing works
Lai, S., Jiang, S.-Y. F., Chou, H.-C., Lin, T.-Y., Wei, Y.-E., & Yu, B. (2021) · Polymer Testing · doi:10.1016/j.polymertesting.2021.107333 · Cited by 19 · see citing works
Electrothermally activated soft materials: Mechanisms, methods and applications
Long, C.-Y., Wang, R., Wang, Y., Lan, H.-B., Zhu, X.-Y., & Zhang, Y.-F. (2024) · Progress in Materials Science · doi:10.1016/j.pmatsci.2024.101406 · Cited by 19 · see citing works
Fan, L. F., Huang, Y. N., Rong, M. Z., & Zhang, M. Q. (2020) · eXPRESS Polymer Letters · doi:10.3144/expresspolymlett.2020.26 · Cited by 18 · see citing works
Self-citationReversible Stepless Multiple Shape Memory Polymer Comprising Amorphous Region as Switching Phase
Li, Y., Tang, H. H., Luo, Y. C., Huang, Y.-C., Zhu, M., Zhang, Y. M., Luo, M. J., Fan, L. F., Gan, F., Ma, C. P., et al. (2025) · Advanced Functional Materials · doi:10.1002/adfm.202500230 · Cited by 14 · see citing works
Self-citationRen, S., & Feng, J. (2023) · Advanced Materials Technologies · doi:10.1002/admt.202300029 · Cited by 14 · see citing works
Lai, S., & You, P.-Y. (2018) · Macromolecular Research · doi:10.1007/s13233-018-6134-9 · Cited by 14 · see citing works
Stepless shape morphing polymer
Min, L., Zhu, M., Lu, H., Li, Y., Fan, L. F., Zhang, M., & Minzhi, R. (2022) · SmartMat · doi:10.1002/smm2.1134 · Cited by 12 · see citing works
Self-citationLai, S., Chen, Y., & Yu, B. (2021) · Journal of Applied Polymer Science · doi:10.1002/app.51238 · Cited by 12 · see citing works
Guo, Q., Zhang, Y., Ruan, H., Sun, H., Wang, T., Wang, Q., & Wang, C. (2023) · Macromolecular Rapid Communications · doi:10.1002/marc.202300534 · Cited by 9 · see citing works
Lai, S., Lin, T.-Y., & Huang, G.-L. (2023) · Journal of Polymer Research · doi:10.1007/s10965-022-03420-9 · Cited by 8 · see citing works
Lai, S., Guo, G.-L., Xie, Y.-C., Chen, J., Xu, D.-Y., Wei, Y.-E., & Cao, Z.-R. (2020) · Journal of Polymer Research · doi:10.1007/s10965-020-02256-5 · Cited by 6 · see citing works
Harnessing length and height changes in thermoresponsive programmable materials
Chalissery, D., Rümmler, T., Ziervogel, F., Eberl, C., & Pretsch, T. (2023) · Programmable Materials · doi:10.1017/pma.2023.9 · Cited by 2 · see citing works
Luo, Y. C., Dang, G. Q., Tang, H. H., Luo, M. J., Zhang, Y. M., Liu, Y., Chen, K., Zhu, M., Fan, L. F., Wu, Q. H., et al. (2025) · ACS Applied Materials & Interfaces · doi:10.1021/acsami.5c12725 · Cited by 1 · see citing works
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Jia, J., & Wang, Y. (2025) · Macromolecules · doi:10.1021/acs.macromol.5c00683
- Authors
- Fan, L. F., Rong, M. Z., Zhang, M. Q., & Chen, X. D.
- Affiliations
- Sun Yat-sen University (CN)
- Key Laboratory for Polymeric Composite and Functional Materials of Ministry of Education GD HPPC Lab School of Chemistry Sun Yat‐sen University Guangzhou 510275 China
- Corresponding author
- Rong, Min Zhi
- Zhang, Ming Qiu
- Venue
- Macromolecular Rapid Communications
- Publisher
- Wiley
- Published
- 2017-06-19
- Volume
- 38
- Issue
- 16
- ISSN
- 1022-1336 (ISSN-L)
- 1521-3927
- OpenAlex
- W2624923551
- Cited by
- 47
- References
- 33
- Citations by year
- 2025: 4 · 2024: 3 · 2023: 7 · 2022: 7 · 2021: 4 · 2020: 8 · 2019: 8 · 2018: 6
- FWCI
- 3.44
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- Macromolecular Rapid Communications (publishedVersion)
- PubMed (publishedVersion)
- Funders
- National Natural Science Foundation of China (51333008, 51673219)
- Topics
- Physical Sciences › Materials Science › Polymers and Plastics › Polymer composites and self-healing
- Physical Sciences › Engineering › Mechanical Engineering › Advanced Materials and Mechanics
- Physical Sciences › Materials Science › Polymers and Plastics › Polymer crystallization and properties
- Keywords
- shape memory polymers, internal stress, styrene-butadiene-styrene block copolymer, reactive blending, crosslinked elastomers, programming, recrystallization, stimuli-responsive polymers, scalable fabrication
- MeSH terms
- Chemistry Techniques, Analytical, Polymers, Polyurethanes, Styrenes, Temperature, Elastomers, Mechanical Phenomena
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