Mechano-responsive hydrogen-bonding array of thermoplastic polyurethane elastomer captures both strength and self-healing

Eom, Youngho; Kim, Seon-Mi; Lee, Minkyung; Jeon, Hyeonyeol; Hwang, Sung Yeon; Park, Jeyoung; Oh, Dongyeop X.

doi:10.21203/rs.3.rs-38016/v1

Cited by 8 publications

(7 citation statements)

References 63 publications

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“…However, as shown in Figure b, the peak of CO moved to a longer wavenumber anomalously, owing to strong hydrogen bonding leading to a shift to a longer wave number. According to the carbonyl stretching region of the infrared spectrum, a reasonable semiquantitative hydrogen-bonded carbonyl groups could be obtained by curve fitting and integrating to get the area of the region to account for the different absorptivity coefficient ratio. , The absorption peaks of the carbonyl region (1600–1700 cm –1 ) in the infrared spectrum for PU were obtained from curve fitting. In Figures c,d and S2b–f, the carbonyl stretching region of the infrared spectrum of SMPU is shown.…”

Section: Resultsmentioning

confidence: 99%

Shape Memory Supramolecular Polyurea with Adjustable Toughness and Ultrahigh Energy Density

Leng

2022

ACS Appl. Polym. Mater.

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As typical stimulus-responsive materials, shape memory polymers (SMPs) have potential for many advanced applications owing to their controllable and programmable shape-changing properties. However, the combination of high toughness and tailorable strength remains a challenge to overcome for SMPs. Here, we engineered meticulously a supramolecular structure with quadruple and double hydrogen bonding arrays to achieve shape memory polyurea elastomers with adjustable strength and toughness. The polyurea with a supramolecular structure had the highest tensile strength of 47 MPa and ultrahigh toughness up to 256 MJ m −3 . Meanwhile, the polyurea was also adjustable to a small tensile strength of 0.87 MPa matching the tensile strength of biological soft tissue (≈1 MPa). The reversible hydrogen bonding arrays endowed polyurea with a shape memory effect as well as excellent selfhealing properties. More importantly, the prestretched polyurea could raise a 500 g weight, which is over 3968 times its own mass, up to 18 mm, because of a high energy density of 75 MJ m −3 , which was higher than the energy density of most SMPs (generally <1 MJ m −3 ).

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Section: Resultsmentioning

confidence: 99%

Shape Memory Supramolecular Polyurea with Adjustable Toughness and Ultrahigh Energy Density

Leng

2022

ACS Appl. Polym. Mater.

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“…The interaction between the charged ammonium group and the other [EMI][TFSI] ion pair also affected the segmental relaxation behaviors of 92-AAHA and 90-DAHA in the ionoconductors. The rheological difference was evaluated by calculating the relaxation time (λ) using the following equation 39 :…”

Section: Resultsmentioning

confidence: 99%

Ion-cluster-mediated ultrafast self-healable ionoconductors for reconfigurable electronics

et al. 2022

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Implementing self-healing capabilities in a deformable platform is one of the critical challenges for achieving future wearable electronics with high durability and reliability. Conventional systems are mostly based on polymeric materials, so their self-healing usually proceeds at elevated temperatures to promote chain flexibility and reduce healing time. Here, we propose an ion-cluster-driven self-healable ionoconductor composed of rationally designed copolymers and ionic liquids. After complete cleavage, the ionoconductor can be repaired with high efficiency (∼90.3%) within 1 min even at 25 °C, which is mainly attributed to the dynamic formation of ion clusters between the charged moieties in copolymers and ionic liquids. By taking advantages of the superior self-healing performance, stretchability (∼1130%), non-volatility (over 6 months), and ability to be easily shaped as desired through cutting and re-assembly protocol, reconfigurable, deformable light-emitting electroluminescent displays are successfully demonstrated as promising electronic platforms for future applications.

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“…In the strain-softening regime, stress is relieved by the conformational rearrangement of the chains, leading to a strain-induced ordering in the network. The increase in the number of hydrogen bonds at moderate strain reflects this increased ordering because the enhanced alignment of the polyurethane chains facilitates hydrogen-bond formation between urethane groups (this behavior is similar to strain-induced crystallization in natural rubber 18,19,21,22 ). At higher strain, the finite extensibility of the chains leads to an upturn of the stress-strain curve.…”

mentioning

confidence: 93%

Rheo-2DIR spectroscopy reveals strain-induced hydrogen-bond redistribution in polyurethane

Giubertoni

Hilbers

Groen

et al. 2022

Preprint

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The remarkable elastic properties of polymers are ultimately due to their molecular structure, but the relation between the macroscopic and molecular properties is often difficult to establish, in particular for (bio)polymers that contain hydrogen bonds, which can easily rearrange upon mechanical deformation. Here we show that two-dimensional infrared spectroscopy on polymer films in a miniature stress tester sheds new light on how the hydrogen-bond structure of a polymer is related to its visco-elastic response. We study thermoplastic polyurethane, a block copolymer consisting of hard segments of hydrogen-bonded urethane groups embedded in a soft matrix of polyether chains. The conventional infrared spectrum shows that upon deformation, the number of hydrogen bonds increases, a process that is largely reversible. However, the 2DIR spectrum reveals that the distribution hydrogen-bond strengths becomes slightly narrower after a deformation cycle, due to the disruption of weak hydrogen bonds, an effect that could explain the strain-cycle induced softening (Mullins effect) of polyurethane. These results show how rheo-2DIR spectroscopy can bridge the gap between the molecular structure and the macroscopic elastic properties of (bio)polymers.

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Mechano-responsive hydrogen-bonding array of thermoplastic polyurethane elastomer captures both strength and self-healing

Cited by 8 publications

References 63 publications

Shape Memory Supramolecular Polyurea with Adjustable Toughness and Ultrahigh Energy Density

Shape Memory Supramolecular Polyurea with Adjustable Toughness and Ultrahigh Energy Density

Ion-cluster-mediated ultrafast self-healable ionoconductors for reconfigurable electronics

Rheo-2DIR spectroscopy reveals strain-induced hydrogen-bond redistribution in polyurethane

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