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Cited by 288Hydrogels: synthesis, properties, applicationsAdvanced Materials and MechanicsAdvanced Sensor and Energy Harvesting Materials

Stretchable hydrogels with low hysteresis and anti-fatigue fracture based on polyprotein cross-linkers

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Lei, Hai, Dong, Liang, Li, Ying, Zhang, Junsheng, Chen, Huiyan, Wu, Junhua, Zhang, Yu, Fan, Qiyang +5 more·2020·Nature Communications
DOI 10.1038/s41467-020-17877-zPMC PMC7423981
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Abstract

Hydrogel-based devices are widely used as flexible electronics, biosensors, soft robots, and intelligent human-machine interfaces. In these applications, high stretchability, low hysteresis, and anti-fatigue fracture are essential but can be rarely met in the same hydrogels simultaneously. Here, we demonstrate a hydrogel design using tandem-repeat proteins as the cross-linkers and random coiled polymers as the percolating network. Such a design allows the polyprotein cross-linkers only to experience considerable forces at the fracture zone and unfold to prevent crack propagation. Thus, we are able to decouple the hysteresis-toughness correlation and create hydrogels of high stretchability (~1100%), low hysteresis (< 5%), and high fracture toughness (~900 J m −2 ). Moreover, the hydrogels show a high fatigue threshold of ~126 J m −2 and can undergo 5000 load-unload cycles up to 500% strain without noticeable mechanical changes. Our study provides a general route to decouple network elasticity and local mechanical response in synthetic hydrogels.

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  • Synthetic hydrogels (PEG, PVA, PHEMA, PAM) with enhanced mechanical deformability and controlled structure and degradation can be used in sensors, actuators, soft robots, and wastewater treatment.

    “synthetic hydrogels with enhanced mechanical deformability and controlled structure and degradation, such as polyethylene glycol (PEG), polyvinyl alcohol (PVA), poly(2-hydroxyethyl methacrylate) (PHEMA) and polyacrylamide (PAM), can be used in sensors, actuators, soft robots, and wastewater treatment”

    From Functionalized Hydrogel-Based Wearable Gas and Humidity Sensors. (2023) · cites this paper as [101]

    The Discussion (page not specified) reports highly stretchable engineered hydrogels and identifies sensors, actuators, and soft robotics as potential applications. The Results describe PEG- and polyacrylamide-based hydrogels, but the cited passages do not support the inclusion of PVA or PHEMA, controlled degradation, or wastewater treatment. (LLM, conf=0.87)

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Research works printed but not linked: 45

  1. [1]Ducrot E Chen Y Bulters M Sijbesma RP Creton C Toughening elastomers with sacrificial bonds and watching them break Science 2014 344 186 189 24723609
  2. [3]Minev IR Biomaterials. Electronic dura mater for long-term multimodal neural interfaces Science 2015 347 159 163 25574019
  3. [4]Park S Self-powered ultra-flexible electronics via nano-grating-patterned organic photovoltaics Nature 2018 561 516 521 30258137
  4. [5]Wang J Zhang F Tsang WP Wan C Wu C Fabrication of injectable high strength hydrogel based on 4-arm star PEG for cartilage tissue engineering Biomaterials 2017 120 11 21 28024231
  5. [6]Ooi HW Hafeez S van Blitterswijk CA Moroni L Baker MB Hydrogels that listen to cells: a review of cell-responsive strategies in biomaterial design for tissue regeneration Mater. Horiz. 2017 4 1020 1040
  6. [7]Li J Mooney DJ Designing hydrogels for controlled drug delivery Nat. Rev. Mater. 2016 1 16071 29657852 PMC5898614
  7. [9]Sun JY Highly stretchable and tough hydrogels Nature 2012 489 133 136 22955625 PMC3642868
  8. [10]Guo M Tough stimuli-responsive supramolecular hydrogels with hydrogen-bonding network junctions J. Am. Chem. Soc. 2014 136 6969 6977 24803288
  9. [11]Yu W Tuning of the dynamics of metal ion crosslinked hydrogels by network structures Soft Matter 2019 15 4423 4427 31106324
  10. [13]Wang Z Stretchable materials of high toughness and low hysteresis Proc. Natl Acad. Sci. USA 2019 116 5967 5972 30850517 PMC6442615
  11. [15]Bai R Yang J Morelle XP Yang C Suo Z Fatigue fracture of self-recovery hydrogels ACS Macro Lett. 2018 7 312 317 35632906
  12. [16]Lin S Anti-fatigue-fracture hydrogels Sci. Adv. 2019 5 eaau8528 30746464 PMC6357728
  13. [17]Vatankhah-Varnosfaderani M Chameleon-like elastomers with molecularly encoded strain-adaptive stiffening and coloration Science 2018 359 1509 1513 29599240
  14. [18]Lin S Liu J Liu X Zhao X Muscle-like fatigue-resistant hydrogels by mechanical training Proc. Natl Acad. Sci. USA 2019 116 10244 10249 31068458 PMC6535018
  15. [19]Simha NK Carlson CS Lewis JL Evaluation of fracture toughness of cartilage by micropenetration J. Matt. Sci. Mater. Med. 2004 15 631 639 15386973
  16. [20]Broedersz CP Storm C MacKintosh FC Nonlinear elasticity of composite networks of stiff biopolymers with flexible linkers Phys. Rev. Lett. 2008 101 118103 18851336
  17. [21]Li H Reverse engineering of the giant muscle protein titin Nature 2002 418 998 1002 12198551
  18. [23]Fang J Forced protein unfolding leads to highly elastic and tough protein hydrogels Nat. Commun. 2013 4 2974 24352111 PMC3983047
  19. [24]Wu J Rationally designed synthetic protein hydrogels with predictable mechanical properties Nat. Commun. 2018 9 620 29434258 PMC5809592
  20. [25]Lv S Designed biomaterials to mimic the mechanical properties of muscles Nature 2010 465 69 73 20445626
  21. [26]Lee HP Gu L Mooney DJ Levenston ME Chaudhuri O Mechanical confinement regulates cartilage matrix formation by chondrocytes Nat. Mater. 2017 16 1243 1251 28967913 PMC5701824
  22. [27]Kollmannsberger, P., Bidan, C. M., Dunlop, J. W. C., Fratzl, P. & Vogel, V. Tensile forces drive a reversible fibroblast-to-myofibroblast transition during tissue growth in engineered clefts. Sci. Adv. 4, eaao4881 (2018). PMC5771696 29349300
  23. [28]Saxena M EGFR and HER2 activate rigidity sensing only on rigid matrices Nat. Mater. 2017 16 775 781 28459445 PMC5920513
  24. [29]Oria R Force loading explains spatial sensing of ligands by cells Nature 2017 552 219 224 29211717
  25. [30]Huang G Functional and biomimetic materials for engineering of the three-dimensional cell microenvironment Chem. Rev. 2017 117 12764 12850 28991456 PMC6494624
  26. [32]Petridou NI Spiro Z Heisenberg CP Multiscale force sensing in development Nat. Cell Biol. 2017 19 581 588 28561050
  27. [33]Latorre E Active superelasticity in three-dimensional epithelia of controlled shape Nature 2018 563 203 208 30401836 PMC6520229
  28. [34]Brangwynne CP Microtubules can bear enhanced compressive loads in living cells because of lateral reinforcement J. Cell Biol. 2006 173 733 741 16754957 PMC2063890
  29. [35]van Doorn JM Lageschaar L Sprakel J van der Gucht J Criticality and mechanical enhancement in composite fiber networks Phys. Rev. E 2017 95 042503 28505721
  30. [36]Das M MacKintosh FC Poisson’s ratio in composite elastic media with rigid rods Phys. Rev. Lett. 2010 105 138102 21230814
  31. [37]Huisman EM Heussinger C Storm C Barkema GT Semiflexible filamentous composites Phys. Rev. Lett. 2010 105 118101 20867610
  32. [38]Das M MacKintosh FC Mechanics of soft composites of rods in elastic gels Phys. Rev. E. 2011 84 061906 22304115
  33. [40]Cao Y Li H Polyprotein of GB1 is an ideal artificial elastomeric protein Nat. Mater. 2007 6 109 114 17237787
  34. [42]Hussain AF Heppenstall PA Kampmeier F Meinhold-Heerlein I Barth S One-step site-specific antibody fragment auto-conjugation using SNAP-tag technology Nat. Protoc. 2019 14 3101 3125 31605098
  35. [43]Caliari SR Burdick JA A practical guide to hydrogels for cell culture Nat. Methods 2016 13 405 414 27123816 PMC5800304
  36. [45]Zhang W Fracture toughness and fatigue threshold of tough hydrogels ACS Macro Lett. 2019 8 17 23 35619405
  37. [46]Sun TL Physical hydrogels composed of polyampholytes demonstrate high toughness and viscoelasticity Nat. Mater. 2013 12 932 937 23892784
  38. [47]Liu J Biomimetic supramolecular polymer networks exhibiting both toughness and self-recovery Adv. Mater. 2017 29 1604951 28092128
  39. [48]Wang Z Stretchable materials of high toughness and low hysteresis Proc. Natl Acad. Sci. USA 2019 116 5967 5972 30850517 PMC6442615
  40. [50]Xie J Qin M Cao Y Wang W Mechanistic insight of photo-induced aggregation of chicken egg white lysozyme: the interplay between hydrophobic interactions and formation of intermolecular disulfide bonds Proteins 2011 79 2505 2516 21661057
  41. [51]Schonbrunn E Eschenburg S Luger K Kabsch W Amrhein N Structural basis for the interaction of the fluorescence probe 8-anilino-1-naphthalene sulfonate (ANS) with the antibiotic target MurA Proc. Natl Acad. Sci. USA 2000 97 6345 6349 10823915 PMC18605
  42. [52]Zhang E Bai R Morelle XP Suo Z Fatigue fracture of nearly elastic hydrogels Soft Matter 2018 14 3563 3571 29682668
  43. [53]Wagner B Tharmann R Haase I Fischer M Bausch AR Cytoskeletal polymer networks: the molecular structure of cross-linkers determines macroscopic properties Proc. Natl Acad. Sci. USA. 2006 103 13974 13978 16963567 PMC1599898
  44. [54]Lake GJ Thomas AG Strength of highly elastic Mater. Proc. R. Soc. Lond. Ser. A Math. Phhys. Sci. 1967 300 108 119
  45. [56]Akagi Y Sakurai H Gong JP Chung UI Sakai T Fracture energy of polymer gels with controlled network structures J. Chem. Phys. 2013 139 144905 24116644

Cited by

Sorted by citations

Authors
Lei, H., Dong, L., Li, Y., Zhang, J., Chen, H., Wu, J., Zhang, Y., Fan, Q., Xue, B., Qin, M., Chen, B., Cao, Y., & Wang, W.
Affiliations
  • Collaborative Innovation Center of Advanced Microstructures (CN)
  • Nanjing University of Information Science and Technology (CN)
  • Nanjing University (CN)
  • Zhejiang University (CN)
Corresponding author
Cao, Yi
ORCID
Venue
Nature Communications
Publisher
Springer Science and Business Media LLC
Published
2020-08-12
Volume
11
Issue
1
Pages
4032-4032
ISSN
2041-1723 (ISSN-L)
DOI
10.1038/s41467-020-17877-z
PMC
PMC7423981
OpenAlex
W3048822132
Cited by
288
References
3
Citations by year
2026: 45 · 2025: 60 · 2024: 66 · 2023: 52 · 2022: 34 · 2021: 29 · 2020: 2
FWCI
9.77
Type
journal article
Language
en
Open access
Licence
Locations
  • Nature Communications (publishedVersion, cc-by)
  • PubMed Central (publishedVersion, cc-by)
  • PubMed (publishedVersion)
  • RePEc: Research Papers in Economics (submittedVersion)
  • DOAJ (DOAJ: Directory of Open Access Journals) (submittedVersion, cc-by-sa)
Funders
  • National Natural Science Foundation of China (21774057, 11934008, 020414380080, 11804147, 11974174, 11674153, 11804148)
  • Government of Jiangsu Province
  • Tianjin University
  • Natural Science Foundation of Jiangsu Province (BK20180320, BK20180335)
  • State Key Laboratory of Precision Measurement Technology and Instruments
  • Fundamental Research Funds for the Central Universities (020414380080, 020414380148)
Topics
  • Life Sciences › Biochemistry, Genetics and Molecular Biology › Molecular Medicine › Hydrogels: synthesis, properties, applications
  • Physical Sciences › Engineering › Mechanical Engineering › Advanced Materials and Mechanics
  • Physical Sciences › Engineering › Biomedical Engineering › Advanced Sensor and Energy Harvesting Materials
Keywords
stretchable hydrogels, tandem repeat proteins, random coil polymers, percolation network, hysteresis, fatigue resistance, fracture toughness, crack propagation, protein unfolding, network elasticity
MeSH terms
Polyacrylamides, Acrylic Resins, Cross-Linking Reagents, Fluorescence, Stress, Mechanical, Hydrogels, Polyproteins, Mechanical Phenomena

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