ACS Publications. Most Trusted. Most Cited. Most Read

OR SEARCH CITATIONS

My Activity
Publications
CONTENT TYPES

Figure 1Loading Img
Download Hi-Res ImageDownload to MS-PowerPointCite This:ACS Appl. Polym. Mater. 2020, 2, 9, 4127-4139
RETURN TO ISSUEPREVArticleNEXT

Tuning the Self-Healing Response of Poly(dimethylsiloxane)-Based Elastomers

  • Diana Döhler*
    Diana Döhler
    Macromolecular Chemistry, Division of Technical and Macromolecular Chemistry, Institute of Chemistry, Faculty of Natural Sciences II (Chemistry, Physics and Mathematics), Martin Luther University Halle-Wittenberg, von-Danckelmann-Platz 4, Halle D-06120, Germany
    Department of Chemical Engineering, Stanford University, 443 Via Ortega, Stanford, California 94305, United States
    *(D.D.) Email: [email protected]
    More by Diana Döhler
    Orcidhttp://orcid.org/0000-0003-4996-1892
  • , 
  • Jiheong Kang
    Jiheong Kang
    Department of Chemical Engineering, Stanford University, 443 Via Ortega, Stanford, California 94305, United States
    Department of Materials Science and Engineering, Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-ro, Yuseong-gu, Daejeon 34141, Republic of Korea
    More by Jiheong Kang
  • , 
  • Chris Brittain Cooper
    Chris Brittain Cooper
    Department of Chemical Engineering, Stanford University, 443 Via Ortega, Stanford, California 94305, United States
    More by Chris Brittain Cooper
  • , 
  • Jeffrey B.-H. Tok
    Jeffrey B.-H. Tok
    Department of Chemical Engineering, Stanford University, 443 Via Ortega, Stanford, California 94305, United States
    More by Jeffrey B.-H. Tok
  • , 
  • Harald Rupp
    Harald Rupp
    Macromolecular Chemistry, Division of Technical and Macromolecular Chemistry, Institute of Chemistry, Faculty of Natural Sciences II (Chemistry, Physics and Mathematics), Martin Luther University Halle-Wittenberg, von-Danckelmann-Platz 4, Halle D-06120, Germany
    More by Harald Rupp
    Orcidhttp://orcid.org/0000-0002-3309-706X
  • , 
  • Wolfgang H. Binder
    Wolfgang H. Binder
    Macromolecular Chemistry, Division of Technical and Macromolecular Chemistry, Institute of Chemistry, Faculty of Natural Sciences II (Chemistry, Physics and Mathematics), Martin Luther University Halle-Wittenberg, von-Danckelmann-Platz 4, Halle D-06120, Germany
    More by Wolfgang H. Binder
    Orcidhttp://orcid.org/0000-0003-3834-5445
  • , and 
  • Zhenan Bao*
    Zhenan Bao
    Department of Chemical Engineering, Stanford University, 443 Via Ortega, Stanford, California 94305, United States
    *(Z.B.) Email: [email protected]
    More by Zhenan Bao
    Orcidhttp://orcid.org/0000-0002-0972-1715
Cite this: ACS Appl. Polym. Mater. 2020, 2, 9, 4127–4139
Publication Date (Web):August 3, 2020
https://doi.org/10.1021/acsapm.0c00755
Copyright © 2020 American Chemical Society
Request reuse permissions

    Article Views

    4366

    Altmetric

    -

    Citations

    38
    LEARN ABOUT THESE METRICS
    Read OnlinePDF (3 MB)
    Get e-Alerts
    Supporting Info (1)»
    SUBJECTS:

    Abstract

    Abstract Image

    We present a comprehensive investigation of mechanical properties of supramolecular polymer networks with rationally developed multistrength hydrogen-bonding interactions. Self-healing poly(dimethylsiloxane) (PDMS)-based elastomers with varying elasticity, fracture toughness, and the ability to dissipate strain energy through the reversible breakage and re-formation of the supramolecular interactions were obtained. By changing the ratio between isophorone diisocyanate (IU), 4,4′-methylenebis(cyclohexyl isocyanate) (MCU), and 4,4′-methylenebis(phenyl isocyanate) (MPU) and by varying the molecular weight of the PDMS precursor, we obtained a library of poly(urea)s to study the interplay of mechanical performance and self-healability. The Young’s moduli of the presented materials ranged between 0.4 and 13 MPa and increased with decreasing molecular weight of the PDMS precursor and increasing content of MCU or MPU units related to the formation of stronger hydrogen-bonding interactions. By exchanging MPU against MCU units, we achieved an optimum balance between mechanical properties and self-healing performance, and by the additional reduction of the molecular weight of the precursor polymer, a minimum recovery of 80% in stress within 12 h at room temperature was observed. Selected poly(urea)s could be processed via 3D printing by the conventional extrusion method, obtaining dimensionally stable and freestanding objects.

    KEYWORDS:

    Supporting Information

    ARTICLE SECTIONS
    Jump To

    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsapm.0c00755.

    • Materials and instrumentation; Synthesis of PDMS-based elastomers using two diisocyanates: reaction scheme and material details; 1H NMR spectra of PDMS-3-IU1.0, PDMS-3-MPU0.4-IU0.6, PDMS-3-MCU1.0, PDMS-5-IU1.0, and PDMS-5-MCU1.0; SEC traces of the PDMS-3-MPU and the PDMS-3-MCU series; IR spectra of PDMS-3-IU1.0, PDMS-3-MPU0.4-IU0.6, PDMS-3-MCU1.0, PDMS-3-MPU1.0, PDMS-5-IU1.0, and PDMS-5-MCU1.0; ESI-ToF mass spectrum of PDMS-3-MCU0.2-IU0.8; thermal characterization, Young’s moduli and stress–strain-curves; self-healing efficiencies; cyclic stress–strain curves of PDMS-3-MPU0.4-IU0.6 and PDMS-3-MCU1.0; rheology investigations; viscosity vs shear rate investigations of PDMS-3-IU1.0 and PDMS-3-MPU0.4-IU0.6 (PDF)

    Terms & Conditions

    Most electronic Supporting Information files are available without a subscription to ACS Web Editions. Such files may be downloaded by article for research use (if there is a public use license linked to the relevant article, that license may permit other uses). Permission may be obtained from ACS for other uses through requests via the RightsLink permission system: http://pubs.acs.org/page/copyright/permissions.html.

    Cited By

    This article is cited by 38 publications.

    1. Lucile Fauvre, Etienne Fleury, François Ganachaud, Daniel Portinha. Extra-Soft Self-Healable Supramolecular Silicone Elastomers from Bis-Amide-PDMS Multiblock Copolymers Prepared by Aza-Michael Reaction. ACS Applied Polymer Materials 2023, 5 (2) , 1229-1240. https://doi.org/10.1021/acsapm.2c01746
    2. Alejandra Durand-Silva, Sachini D. Perera, Ashele K. Remy, Hao-Che Peng, James A. Hargrove, Zackery D. Ferneyhough, Paola M. Lopez Landaverde, Allison L. Stelling, Ronald A. Smaldone. Infrared Spectroscopic and Mechanical Analysis of Supramolecular Self-Healing in 3D Printable Urea Photoresins. ACS Applied Polymer Materials 2022, 4 (12) , 8825-8832. https://doi.org/10.1021/acsapm.2c01233
    3. Christopher B. Cooper, Zhenan Bao. Using Periodic Dynamic Polymers to Form Supramolecular Nanostructures. Accounts of Materials Research 2022, 3 (9) , 948-959. https://doi.org/10.1021/accountsmr.2c00101
    4. Nan Wang, Xingwei Feng, Jingke Pei, Qinke Cui, Yuanjie Li, Hongyi Liu, Xinxing Zhang. Biobased Reversible Cross-Linking Enables Self-Healing and Reprocessing of Epoxy Resins. ACS Sustainable Chemistry & Engineering 2022, 10 (11) , 3604-3613. https://doi.org/10.1021/acssuschemeng.1c08378
    5. Shengping Dai, Meng Li, Hao Yan, Hao Zhu, Hongwei Hu, Yixing Zhang, Guanggui Cheng, Ningyi Yuan, Jianning Ding. Self-Healing Silicone Elastomer with Stable and High Adhesion in Harsh Environments. Langmuir 2021, 37 (46) , 13696-13702. https://doi.org/10.1021/acs.langmuir.1c02356
    6. Yue Han, Yongqing Bai, Jiali Bian, Xiuping Guo, Bin Liu, Zhaofeng Wang. Polydimethylsiloxane-Based Mechanoluminescent Occlusal Splint with the Visualization of Occlusal Force. ACS Applied Polymer Materials 2021, 3 (10) , 5180-5187. https://doi.org/10.1021/acsapm.1c00917
    7. Christian Andersen, Libor Zverina, Koosha Ehtiati, Esben Thormann, Hanne Mordhorst, Sünje J. Pamp, Niels J. Madsen, Anders E. Daugaard. Antimicrobial PDMS Surfaces Prepared through Fast and Oxygen-Tolerant SI-SARA-ATRP, Using Na2SO3 as a Reducing Agent. ACS Omega 2021, 6 (22) , 14551-14558. https://doi.org/10.1021/acsomega.1c01611
    8. Christopher B. Cooper, Jiheong Kang, Yikai Yin, Zhiao Yu, Hung-Chin Wu, Shayla Nikzad, Yuto Ochiai, Hongping Yan, Wei Cai, Zhenan Bao. Multivalent Assembly of Flexible Polymer Chains into Supramolecular Nanofibers. Journal of the American Chemical Society 2020, 142 (39) , 16814-16824. https://doi.org/10.1021/jacs.0c07651
    9. Chen-Chu Hsu, Livy Laysandra, Yu-Cheng Chiu, Wei-Ren Liu. Pivotal role of Boron-doped graphene quantum dots in stretchable and Self-Healable red emission nanocomposite Film: One step advance for white light emitting diodes application. Chemical Engineering Journal 2023, 473 , 145469. https://doi.org/10.1016/j.cej.2023.145469
    10. Yingqiao Ma, Chong‐an Di, Daoben Zhu. Advances in Organic Thermoelectric Devices for Multiple Applications. Advanced Physics Research 2023, 4 https://doi.org/10.1002/apxr.202300027
    11. Yuhang Zhang, Lu Bai, Zhirui Xu, Siyuan Chen, Junping Zheng. A Robust, Thermally Stable, and Efficiently Reprocessable Poly(dimethylsiloxane) Elastomers Based on Activated Dynamic Silyl Ether Linkages by Neighboring Groups. Macromolecular Chemistry and Physics 2023, 224 (15) https://doi.org/10.1002/macp.202300076
    12. Bingrui Li, Sirui Ge, Sheng Zhao, Kunyue Xing, Alexei P. Sokolov, Peng-Fei Cao, Tomonori Saito. Puncture-resistant self-healing polymers with multi-cycle adhesion and rapid healability. Materials Horizons 2023, 10 (8) , 2868-2875. https://doi.org/10.1039/D3MH00481C
    13. Christopher B. Cooper, Samuel E. Root, Lukas Michalek, Shuai Wu, Jian-Cheng Lai, Muhammad Khatib, Solomon T. Oyakhire, Renee Zhao, Jian Qin, Zhenan Bao. Autonomous alignment and healing in multilayer soft electronics using immiscible dynamic polymers. Science 2023, 380 (6648) , 935-941. https://doi.org/10.1126/science.adh0619
    14. Changxu Sun, Zhe Cheng, Jj Abu-Halimah, Bozhi Tian. Perspectives on tissue-like bioelectronics for neural modulation. iScience 2023, 26 (5) , 106715. https://doi.org/10.1016/j.isci.2023.106715
    15. Anja Marinow, Zviadi Katcharava, Wolfgang H. Binder. Self-Healing Polymer Electrolytes for Next-Generation Lithium Batteries. Polymers 2023, 15 (5) , 1145. https://doi.org/10.3390/polym15051145
    16. Jing Yang, Xin Zhou, Xiaomu Wen, Gazi Hao, Lei Xiao, Guangpu Zhang, Wei Jiang. Molecular Engineering of Binder for Improving the Mechanical Properties and Recyclability of Energetic Composites. Nanomaterials 2023, 13 (6) , 1087. https://doi.org/10.3390/nano13061087
    17. Jing Yang, Xin Zhou, Junqing Yang, Jiaoyang Chen, Zhe Sun, Yuhang Cheng, Lin Yang, Hui Wang, Guangpu Zhang, Jiajun Fu, Wei Jiang. A microscale regulation strategy for strong, tough, and efficiently self-healing energetic adhesives. Chemical Engineering Journal 2023, 451 , 138810. https://doi.org/10.1016/j.cej.2022.138810
    18. Yue Zhao, Ziling Jiang, Wei Wang, Danfeng Zhi, Fengjiao Zhang, Chong‐an Di. Organic Thermoelectric Devices. 2022, 237-273. https://doi.org/10.1002/9783527835492.ch8
    19. M. Hyder, A.D. O'Donnell, A.M. Chippindale, I.M. German, J.L. Harries, O. Shebanova, I.W. Hamley, W. Hayes. Tailoring viscoelastic properties of dynamic supramolecular poly(butadiene)-based elastomers. Materials Today Chemistry 2022, 26 , 101008. https://doi.org/10.1016/j.mtchem.2022.101008
    20. In Ho Kim, Subi Choi, Jieun Lee, Jiyoung Jung, Jinwook Yeo, Jun Tae Kim, Seunghwa Ryu, Suk-kyun Ahn, Jiheong Kang, Philippe Poulin, Sang Ouk Kim. Human-muscle-inspired single fibre actuator with reversible percolation. Nature Nanotechnology 2022, 17 (11) , 1198-1205. https://doi.org/10.1038/s41565-022-01220-2
    21. Jun Xu, Lei Zhu, Yongjia Nie, Yuan Li, Shicheng Wei, Xu Chen, Wenpeng Zhao, Shouke Yan. Advances and Challenges of Self-Healing Elastomers: A Mini Review. Materials 2022, 15 (17) , 5993. https://doi.org/10.3390/ma15175993
    22. Chuanhui Gao, Yiliang Gao, Sikai Wang, Yajie Dong, Yumin Wu, Yuetao Liu, Chuanxing Wang. Self-healing unsaturated polyester sensor based on multiple hydrogen bonds. European Polymer Journal 2022, 175 , 111301. https://doi.org/10.1016/j.eurpolymj.2022.111301
    23. Balaji Krishnakumar, Andrea Pucci, Prakash P. Wadgaonkar, Indresh Kumar, Wolfgang H. Binder, Sravendra Rana. Vitrimers based on bio-derived chemicals: Overview and future prospects. Chemical Engineering Journal 2022, 433 , 133261. https://doi.org/10.1016/j.cej.2021.133261
    24. Di Zhao, Jing Yang, Xinle Tian, Jinzhu Wei, Qianrui Li, Yige Wang. Self-healing metallo-supramolecular polymers showing luminescence off/on switching based on lanthanide ions and terpyridine moieties. Chemical Engineering Journal 2022, 434 , 134806. https://doi.org/10.1016/j.cej.2022.134806
    25. Siyang Wang, Dmitriy Davydovich, Marek W. Urban. Shape Memory‐Induced Self‐Healable Polymers. 2022, 1-19. https://doi.org/10.1002/9783527815562.mme0052
    26. Yuehui Wang, Zhimin Zhou, Sixing Li, Han Zheng, Jiaxin Lu, Shuyue Wang, Jiahao Zhang, Ke Wang, Kaiwen Lin. Near-Infrared-Light-Assisted Self-Healing Graphene-Thermopolyurethane Composite Films. Polymers 2022, 14 (6) , 1183. https://doi.org/10.3390/polym14061183
    27. Gaurav Balakrishnan, Jiwoo Song, Chenchen Mou, Christopher J. Bettinger. Recent Progress in Materials Chemistry to Advance Flexible Bioelectronics in Medicine. Advanced Materials 2022, 34 (10) https://doi.org/10.1002/adma.202106787
    28. Debabrata Ganguly, Santanu Chattopadhyay. Plastics in Self-Healing Applications. 2022, 259-272. https://doi.org/10.1016/B978-0-12-820352-1.00134-6
    29. Di Zhao, Jing Yang, Yige Wang, Huanrong Li. Luminescent self-healing materials constructed via coordination between lanthanide ions and phenanthroline-tethered to polymer chain. Dyes and Pigments 2022, 197 , 109864. https://doi.org/10.1016/j.dyepig.2021.109864
    30. Yogeenth Kumaresan, Nivasan Yogeswaran, Luigi G. Occhipinti, Ravinder Dahiya. Stretchable Systems. 2021https://doi.org/10.1017/9781108882330
    31. Seonghyeon Jeong, Anders E. Daugaard, Anne Ladegaard L. Skov, , , . Autonomously self-healing dielectric elastomer actuators from thermoplastic polydimethylsiloxane elastomer. 2021, 42. https://doi.org/10.1117/12.2576864
    32. Yue Zhao, Liyao Liu, Fengjiao Zhang, Chong‐an Di, Daoben Zhu. Advances in organic thermoelectric materials and devices for smart applications. SmartMat 2021, 2 (4) , 426-445. https://doi.org/10.1002/smm2.1034
    33. Harald Rupp, Wolfgang H. Binder. 3D Printing of Solvent-Free Supramolecular Polymers. Frontiers in Chemistry 2021, 9 https://doi.org/10.3389/fchem.2021.771974
    34. Tianwen Yu, Yifei Shan, Zhixi Li, Xiaoxiao Wang, Huanan Cui, Kun Yang, Yongyan Cui. Application of a super-stretched self-healing elastomer based on methyl vinyl silicone rubber for wearable electronic sensors. Polymer Chemistry 2021, 12 (42) , 6145-6153. https://doi.org/10.1039/D1PY01089A
    35. Jin Hu, Ruhan Yang, Li Zhang, Ying Chen, Xinxin Sheng, Xinya Zhang. Robust, transparent, and self-healable polyurethane elastomer via dynamic crosslinking of phenol-carbamate bonds. Polymer 2021, 222 , 123674. https://doi.org/10.1016/j.polymer.2021.123674
    36. Weiyang Yang, Yan Gong, Wen Li. A Review: Electrode and Packaging Materials for Neurophysiology Recording Implants. Frontiers in Bioengineering and Biotechnology 2021, 8 https://doi.org/10.3389/fbioe.2020.622923
    37. Di Zhao, Jing Yang, Qianrui Li, Xinle Tian, Jinzhu Wei, Yige Wang. Self-Healing Metallo-Supramolecular Polymers Showing Luminescence Off/On Switching Based on Lanthanide Ions and Terpyridine Moieties. SSRN Electronic Journal 2021, 13 https://doi.org/10.2139/ssrn.3989389
    38. Gulzhian I. Dzhardimalieva, Bal C. Yadav, Sarkyt E. Kudaibergenov, Igor E. Uflyand. Basic Approaches to the Design of Intrinsic Self-Healing Polymers for Triboelectric Nanogenerators. Polymers 2020, 12 (11) , 2594. https://doi.org/10.3390/polym12112594
    Download PDF

    Pair your accounts.

    Export articles to Mendeley

    Get article recommendations from ACS based on references in your Mendeley library.

    Pair your accounts.

    Export articles to Mendeley

    Get article recommendations from ACS based on references in your Mendeley library.

    You’ve supercharged your research process with ACS and Mendeley!

    STEP 1:
    Click to create an ACS ID

    Please note: If you switch to a different device, you may be asked to login again with only your ACS ID.

    Please note: If you switch to a different device, you may be asked to login again with only your ACS ID.

    Please note: If you switch to a different device, you may be asked to login again with only your ACS ID.

    MENDELEY PAIRING EXPIRED
    Your Mendeley pairing has expired. Please reconnect