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Cold-induced shape memory hydrogels for strong and programmable artificial muscles

基于冷致形状记忆水凝胶的超强可编程人工肌肉

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Abstract

Thermo-responsive shape memory hydrogels generally achieve shape fixation at low temperatures, and shape recovery at high temperatures. However, these hydro-gels usually suffer from poor mechanical properties. Herein, we present a unique poly(acrylic acid)/calcium acetate shape memory hydrogel with cold-induced shape recovery performances as ultrastrong artificial muscles. Since the acetate groups could form aggregate at high temperatures and thus induce the association of the hydrogel network, the hydrogel can be fixed into a temporary shape upon heating and recover to its original shape in a cold environment. Moreover, a programmable shape recovery process is realized by adjusting the shape fixing time. In addition, the unique shape memory process enables the application demonstration as bio-inspired artificial muscles with an ultrahigh work density of 45.2 kJ m−3, higher than that of biological muscles (∼8 kJ m−3).

摘要

热致响应形状记忆水凝胶通常在低温时固定临时形状, 升高温度回复至初始形状. 然而, 水凝胶高含水量的特点导致其较弱的力学性能, 限制了其广泛应用. 本文介绍了一种具有独特的冷致形状回复功能的聚丙烯酸/乙酸钙水凝胶, 由于乙酸基团在高温下形成聚集体, 进而会导致聚丙烯酸网络的疏水聚集和硬化, 因而水凝胶的临时形状可在70°C时固定, 并在20°C的低温环境回复至初始形状. 同时, 通过调控形状固定时间可以实现分步形状恢复. 这种形状记忆水凝胶可用作人工肌肉, 其做功能力高达45.2 kJ m−3, 远超过一般动物肌肉的做功能力(∼8 kJ m−3).

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References

  1. Zhao Q, Qi HJ, Xie T. Recent progress in shape memory polymer: New behavior, enabling materials, and mechanistic understanding. Prog Polym Sci, 2015, 49–50: 79–120

    Article  Google Scholar 

  2. Lendlein A, Gould OEC. Reprogrammable recovery and actuation behaviour of shape-memory polymers. Nat Rev Mater, 2019, 4: 116–133

    Article  Google Scholar 

  3. Wang K, Jia YG, Zhao C, et al. Multiple and two-way reversible shape memory polymers: Design strategies and applications. Prog Mater Sci, 2019, 105: 100572

    Article  CAS  Google Scholar 

  4. Zhang D, Zhang J, Jian Y, et al. Multi-field synergy manipulating soft polymeric hydrogel transformers. Adv Intelligent Syst, 2021, 3: 2000208

    Article  Google Scholar 

  5. Zhuo S, Zhao Z, Xie Z, et al. Complex multiphase organohydrogels with programmable mechanics toward adaptive soft-matter machines. Sci Adv, 2020, 6: 1464

    Article  Google Scholar 

  6. Zhu CN, Bai T, Wang H, et al. Dual-encryption in a shape-memory hydrogel with tunable fluorescence and reconfigurable architecture. Adv Mater, 2021, 33: 2102023

    Article  CAS  Google Scholar 

  7. Xie T. Tunable polymer multi-shape memory effect. Nature, 2010, 464: 267–270

    Article  CAS  Google Scholar 

  8. Julich-Gruner KK, Löwenberg C, Neffe AT, et al. Recent trends in the chemistry of shape-memory polymers. Macromol Chem Phys, 2013, 214: 527–536

    Article  CAS  Google Scholar 

  9. Xu W, Zhang R, Liu W, et al. A multiscale investigation on the mechanism of shape recovery for IPDI to PPDI hard segment substitution in polyurethane. Macromolecules, 2016, 49: 5931–5944

    Article  CAS  Google Scholar 

  10. Xu XQ, He Y, Liu H, et al. Polydiacetylene-polyurethane crisscross elastomer as an intrinsic shape memory conductive polymer. ACS Macro Lett, 2019, 8: 409–413

    Article  CAS  Google Scholar 

  11. Osada Y, Matsuda A. Shape memory in hydrogels. Nature, 1995, 376: 219

    Article  CAS  Google Scholar 

  12. Lei H, Dong L, Li Y, et al. Stretchable hydrogels with low hysteresis and anti-fatigue fracture based on polyprotein cross-linkers. Nat Commun, 2020, 11: 4032

    Article  CAS  Google Scholar 

  13. Kempaiah R, Nie Z. From nature to synthetic systems: Shape transformation in soft materials. J Mater Chem B, 2014, 2: 2357–2368

    Article  CAS  Google Scholar 

  14. Liu T, Wang F, Wu Q, et al. Fluorescent, electrically responsive and ultratough self-healing hydrogels via bioinspired all-in-one hierarchical micelles. Mater Horiz, 2021, 8: 3096–3104

    Article  CAS  Google Scholar 

  15. Xu H, Shi FK, Liu XY, et al. How can multi-bond network hydrogels dissipate energy more effectively: An investigation on the relationship between network structure and properties. Soft Matter, 2020, 16: 4407–4413

    Article  CAS  Google Scholar 

  16. Dou Y, Wang ZP, He W, et al. Artificial spider silk from ion-doped and twisted core-sheath hydrogel fibres. Nat Commun, 2019, 10: 5293

    Article  Google Scholar 

  17. Li X, He L, Li Y, et al. Healable, degradable, and conductive MXene nanocomposite hydrogel for multifunctional epidermal sensors. ACS Nano, 2021, 15: 7765–7773

    Article  CAS  Google Scholar 

  18. Zhang S, Li Y, Zhang H, et al. Bioinspired conductive hydrogel with ultrahigh toughness and stable antiswelling properties for articular cartilage replacement. ACS Mater Lett, 2021, 3: 807–814

    Article  CAS  Google Scholar 

  19. Li X, Wang Z, Li W, et al. Superstrong water-based supramolecular adhesives derived from poly(vinyl alcohol)/poly(acrylic acid) complexes. ACS Mater Lett, 2021, 3: 875–882

    Article  CAS  Google Scholar 

  20. Ju G, Cheng M, Guo F, et al. Elasticity-dependent fast underwater adhesion demonstrated by macroscopic supramolecular assembly. Angew Chem Int Ed, 2018, 57: 8963–8967

    Article  CAS  Google Scholar 

  21. Zhu J, Chen GY, Yu L, et al. Mechanically strong and highly stiff supramolecular polymer composites repairable at ambient conditions. CCS Chem, 2020, 2: 280–292

    Article  CAS  Google Scholar 

  22. Li P, Xia Y, Hao J, et al. Transient healability of metallosupramolecular polymer networks mediated by kinetic control of competing chemical reactions. Macromolecules, 2020, 53: 2856–2863

    Article  CAS  Google Scholar 

  23. Le X, Lu W, Zheng J, et al. Stretchable supramolecular hydrogels with triple shape memory effect. Chem Sci, 2016, 7: 6715–6720

    Article  CAS  Google Scholar 

  24. Li P, Wang Z, Lin X, et al. Muscle-inspired ion-sensitive hydrogels with highly tunable mechanical performance for versatile industrial applications. Sci China Mater, 2022, 65: 229–236

    Article  CAS  Google Scholar 

  25. Xu L, Qiu D. Reversible switching of polymeric gel structure and property by solvent exchange. Sci China Mater, 2022, 65: 547–552

    Article  CAS  Google Scholar 

  26. Xie M, Wu C, Chen C, et al. Photo-adaptable shape memory hydrogels based on orthogonal supramolecular interactions. Polym Chem, 2019, 10: 4852–4858

    Article  CAS  Google Scholar 

  27. Jia YG, Jin J, Liu S, et al. Self-healing hydrogels of low molecular weight poly(vinyl alcohol) assembled by host-guest recognition. Biomacromolecules, 2018, 19: 626–632

    Article  CAS  Google Scholar 

  28. Xiao H, Lu W, Le X, et al. A multi-responsive hydrogel with a triple shape memory effect based on reversible switches. Chem Commun, 2016, 52: 13292–13295

    Article  CAS  Google Scholar 

  29. Hu X, Zhang D, Sheiko SS. Cooling-triggered shapeshifting hydrogels with multi-shape memory performance. Adv Mater, 2018, 30: 1707461

    Article  Google Scholar 

  30. Zhang Y, Desai MS, Wang T, et al. Elastin-based thermoresponsive shape-memory hydrogels. Biomacromolecules, 2020, 21: 1149–1156

    Article  CAS  Google Scholar 

  31. Nonoyama T, Lee YW, Ota K, et al. Instant thermal switching from soft hydrogel to rigid plastics inspired by thermophile proteins. Adv Mater, 2020, 32: 1905878

    Article  CAS  Google Scholar 

  32. Zhao C, Ma Z, Zhu XX. Rational design of thermoresponsive polymers in aqueous solutions: A thermodynamics map. Prog Polym Sci, 2019, 90: 269–291

    Article  CAS  Google Scholar 

  33. Kram R. Inexpensive load carrying by rhinoceros beetles. J Exp Biol, 1996, 199: 609–612

    Article  CAS  Google Scholar 

  34. Lumsden JS. XXXIV.—Solubilities of the calcium salts of the acids of the acetic series. J Chem Soc Trans, 1902, 81: 350–362

    Article  CAS  Google Scholar 

  35. Wang L, Jian Y, Le X, et al. Actuating and memorizing bilayer hydrogels for a self-deformed shape memory function. Chem Commun, 2018, 54: 1229–1232

    Article  CAS  Google Scholar 

  36. Xue P, Bisoyi HK, Chen Y, et al. Near-infrared light-driven shape-morphing of programmable anisotropic hydrogels enabled by MXene nanosheets. Angew Chem Int Ed, 2021, 60: 3390–3396

    Article  CAS  Google Scholar 

  37. Mirfakhrai T, Madden JDW, Baughman RH. Polymer artificial muscles. Mater Today, 2007, 10: 30–38

    Article  CAS  Google Scholar 

  38. Ma Y, Hua M, Wu S, et al. Bioinspired high-power-density strong contractile hydrogel by programmable elastic recoil. Sci Adv, 2020, 6: 2520

    Article  Google Scholar 

Download references

Acknowledgements

This work was supported by the National Natural Science Foundation of China (51873223 and 22075154) and the Natural Science Foundation of Zhejiang Province (LY19B040001).

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Authors

Contributions

Author contributions Hua L conducted most of the experiments and drafted the manuscript; Zhao C designed the experiments and drafted the manuscript; Guan X helped with the synthesis of the hydrogel; Lu J conducted the rheology experiments; Zhang J initiated and guided the work and drafted the manuscript. All authors contributed to the discussion and preparation of the manuscript.

Corresponding author

Correspondence to Jiawei Zhang  (张佳玮).

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Conflict of interest The authors declare that they have no conflict of interest.

Additional information

Supplementary information Experimental details and supporting data are available in the online version of the paper.

Luqin Hua received her BSc degree from Ningbo University in 2020. She is now a master candidate at Ningbo University under the supervision of Prof. Chuanzhuang Zhao. Her research interest focuses on shape memory hydrogels and their applications.

Chuanzhuang Zhao received his PhD degree in polymer chemistry and physics from Nankai University in China in 2010. After postdoctoral training at the Institute of Chemistry, Chinese Academy of Sciences, he joined Ningbo University in 2013, and now he is an associate professor. His current research involves the synthetic chemistry and physical chemistry of stimuli-responsive polymers.

Jiawei Zhang received her PhD degree in polymer chemistry and physics from Nankai University in China in 2010, during which she had research training at the University of Montreal (2007–2009, Canada). After postdoctoral training at Tsinghua University, China, she joined Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences in 2013, and now she is a professor of Tiangong University. Her research interest includes smart polymeric hydrogel actuators and shape memory hydrogels.

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Hua, L., Zhao, C., Guan, X. et al. Cold-induced shape memory hydrogels for strong and programmable artificial muscles. Sci. China Mater. 65, 2274–2280 (2022). https://doi.org/10.1007/s40843-021-1971-9

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  • DOI: https://doi.org/10.1007/s40843-021-1971-9

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