Force-mediated molecule release from double network hydrogels

Jayathilaka, Pavithra Bhakthi; Molley, Thomas G.; Huang, Yuwan; Islam, Shariful; Buche, Michael R.; Silberstein, Meredith N.; Kruzic, Jamie J.; Kilian, Kristopher A.

doi:10.1039/d1cc02726c

Cited by 15 publications

(13 citation statements)

References 44 publications

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“… (a) Double network hydrogels can withstand large deformation. (b) Calcium crosslinked alginate as sacrifice network can provide water gel dissipation energy [170]. (c) Schematic diagram of brown algae adhesive system.…”

Section: Fundamental Design Principles Of Natural Polymer‐based Adhes...mentioning

confidence: 99%

“…It is assumed that stress appears at the crack tip; it does not destroy the polymer chain at the crack tip but destroys the relatively weak bonds in the bulk matrix (such as sacrificial bonds), thereby preserving the chain integrity. The dispassion energy blocks significant crack propagation at the interface as well as within the gel itself (Figure 4a) [170]; the resultant product is malleable and can withstand large deformations through the Irwin-Orowan mechanism. In general, the molar concentration of the former is generally 20-30 times higher than that of the previous one, and there may be cross-linking between them [171,172].…”

Section: Balance Of Cohesion and Adhesionmentioning

confidence: 99%

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Natural polymer‐based adhesive hydrogel for biomedical applications

Long

Xie

2022

Biosurface and Biotribology

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Hydrogel is a polymer network system that can form a hydrophilic three‐dimensional network structure through different cross‐linking methods. In recent years, hydrogels have received considerable attention due to their good biocompatibility and biodegradability by introducing different cross‐linking mechanisms and functional components. Compared with synthetic hydrogels, natural polymer‐based hydrogels have low biotoxicity, high cell affinity, and great potential for biomedical fields; however, their mechanical properties and tissue adhesion capabilities have been unable to meet clinical requirements. In recent years, many efforts have been made to solve these issues. In this review, the recent progress in the field of natural polymer‐based adhesive hydrogels is highlighted. The authors first introduce the general design principles for the natural polymer‐based adhesive hydrogels being used as excellent tissue adhesives and the challenges associated with their design. Next, their usages in biomedical applications are summarised, such as wound healing, haemostasis, nerve repair, bone tissue repair, cartilage tissue repair, electronic devices, and other tissue repairs. Finally, the potential challenges of natural polymer‐based adhesive hydrogels are presented.

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Section: Fundamental Design Principles Of Natural Polymer‐based Adhes...mentioning

confidence: 99%

Section: Balance Of Cohesion and Adhesionmentioning

confidence: 99%

Natural polymer‐based adhesive hydrogel for biomedical applications

Long

Xie

2022

Biosurface and Biotribology

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“…Though the particularities may differ, the harmonic potential is the most common way of rendering the rigid links of the FJC model flexible [6][7][8][9][10][11][12][13][14][15][16][17][18][19][20][21][22][23][24][26][27][28][29][30][31]. The full asymptotic, reduced asymptotic, and exact (see the Appendix) approaches of obtaining the EFJC single-chain mechanical response γ(η) are plotted in Fig.…”

Section: Harmonic Link Potentialmentioning

confidence: 99%

“…The reduced asymptotic approach tends to be inaccurate for moderate κ, but quickly becomes accurate for large κ. Above κ = 100, the difference between all three approaches vanishes, where the reduced asymptotic approach could be used in place of the exact approach for expediency since κ is often larger than 100 when modeling experiments [5,11,12,24]. The nondimensional single-chain mechanical response γ(η) for the log-squared-FJC model, using the full asymptotic (dotted), reduced asymptotic (dashed), and quadrature (solid) approaches, for varying κ = ε.…”

Section: Harmonic Link Potentialmentioning

confidence: 99%

“…Additional terms can be included to obtain an improved approximation for harmonic potentials [7,22], enabling better accuracy at lower link stiffnesses and therefore more robust modeling [6,23]. This simplest approach can be gener-alized for anharmonic link potentials in order to capture the mechanical response up until the chain breaks, which is useful for large-deformation polymer network constitutive models [5,24]. An alternative approach has been developed by Mao et al [25], where a constructed free energy function is minimized with respect to link length in order to obtain an effective link length, and subsequently, the single-chain mechanical response.…”

Section: Introductionmentioning

confidence: 99%

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On freely-jointed chain models with flexible links

Buche,

Silberstein,

Grutzik

2022

Preprint

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Analytical relations for the mechanical response of single polymer chains are valuable for modeling purposes, on both the molecular and continuum scale. These relations can be obtained using statistical thermodynamics and an idealized single-chain model, such as the freely-jointed chain model. In order to include bond stretching, the rigid links in the freely-jointed chain model can be made flexible, but this almost always renders the model analytically intractable. Here, an asymptotically-correct statistical thermodynamic theory is used to develop analytic approximations for the single-chain mechanical response of this model. The accuracy of these approximations is demonstrated using several link potential energy functions. This approach can be applied to other single-chain models, and to molecular stretching in general.

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Release of Molecular Cargo from Polymer Systems by Mechanochemistry

Küng

Göstl

Schmidt

2022

Chemistry A European J

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The design and manipulation of (multi)functional materials at the nanoscale holds the promise of fuelling tomorrow's major technological advances. In the realm of macromolecular nanosystems, the incorporation of force‐responsive groups, so called mechanophores, has resulted in unprecedented access to responsive behaviours and enabled sophisticated functions of the resulting structures and advanced materials. Among the diverse force‐activated motifs, the on‐demand release or activation of compounds, such as catalysts, drugs, or monomers for self‐healing, are sought‐after since they enable triggering pristine small molecule function from macromolecular frameworks. Here, we highlight examples of molecular cargo release systems from polymer‐based architectures in solution by means of sonochemical activation by ultrasound (ultrasound‐induced mechanochemistry). Important design concepts of these advanced materials are discussed, as well as their syntheses and applications.

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Force-mediated molecule release from double network hydrogels

Abstract: The incorporation of mechanosensitive linkages into polymers has led to materials that display dynamic functional behavior in response to force. However, mechanophores have predominantly been integrated into bulk thermoplastics, while...

Cited by 15 publications

References 44 publications

Natural polymer‐based adhesive hydrogel for biomedical applications

Natural polymer‐based adhesive hydrogel for biomedical applications

On freely-jointed chain models with flexible links

Release of Molecular Cargo from Polymer Systems by Mechanochemistry

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