Self‐Healing Gelatin Hydrogels Cross‐Linked by Combining Multiple Hydrogen Bonding and Ionic Coordination

Zhang, Guangzhao; Lv, Lei; Deng, Yonghong; Wang, Chaoyang

doi:10.1002/marc.201700018

Cited by 80 publications

(50 citation statements)

References 51 publications

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“…The cross‐over point of G′ and G″ curves which referred to the sol–gel transition was observed at 54 °C. Comparing with chelation‐crosslinked gelatin‐UPy‐Fe hydrogels whose sol–gel occurred at 34 °C, the present oxidation‐crosslinked hydrogel exhibited a higher temperature durability. When the temperature further increased, G′ was lower than G″, which may imply the gradual destruction of the 3D network in this hydrogel.…”

Section: Resultsmentioning

confidence: 99%

Tannin‐Tethered Gelatin Hydrogels with Considerable Self‐Healing and Adhesive Performances

Zhao

Long

et al. 2019

Macro Materials & Eng

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wearable devices, [4] soft electronics, [5,6] battery binders, [7][8][9] etc. Among these versatile materials, self-healing hydrogels, which can recover their original properties through autonomous healing after suffering from damages, exhibit an enormous potential in the fields of wound closure, [10,11] scaffolds for tissue engineering, [12,13] drug/cell delivery devices, [14][15][16] and so on.In nature, marine mussels can tightly attach to almost all surfaces by secreting mussel adhesive proteins (MAPs). [17] In addition, the adhesion property of MAPs is attributed to the presence of a special catechol-containing amino acid compound, 3,4-dihydroxyphenylalanine (DOPA). [18] The catechol groups of DOPA are easy oxidized to quinones in alkaline condition [1] and subsequently react with nucleophiles such as amines and thiols to form the 3D net structure of hydrogel via Schiff's base and Michael addition reactions. [19] Additionally, the catechol moieties endow DOPA with the capability to complex with various metal ions in order to produce coordination-crosslinked hydrogels. Owing to the versatility of DOPA, it has been coupled through various reactions to numerous macromolecules, including chitosan, [20] gelatin, [19] and polyethylene glycol (PEG). [21] This has allowed to fabricate mussel-inspired materials with self-healing and adhesive properties. The high price and potential neurotransmission effect of DOPA limit its commercial applications, however, and consequently the search of alternatives to DOPA is necessary. [22] Tannic acid (TA), a plant-derived polyphenolic compound, consists of a glucose core and ester-linked peripheral gallol groups (three adjacent hydroxyls attached to benzene). [23] With these functional groups, TA is capable to precipitate proteins (collagen and gelatin) by multi-point hydrogen bond and hydrophobic interactions. [24] The two adjacent phenolic hydroxyls of gallols in TA can also chelate metal ions (e.g., Fe 3+ , Al 3+ , Cr 3+ ) in the form of oxygen anion to form stable pentacyclic complexes. Although the third phenol hydroxyl is not involved in the formation of these pentacyclic structures, it can encourage the dissociation of the other two adjacent OH groups and accelerate the coordination reaction promoting its stability. [25] In addition, TA presents a good antioxidant capacity. The gallols of TA are oxidized to form quinones that further undergo nucleophilic Hydrogels Hydrogels, especially the ones with self-recovery and adhesive performances, have attracted more and more attention owing to their wide practical potential in the biomedical field involving cell delivery, wound filling, and tissue engineering. Tannic acid (TA), a nature-derived gallol-rich polyphenol, exhibits not only unique chelating properties with transition metal cations but also desirable anti-oxidation properties and strong bonding capability to proteins and gelatin. Thus, taking advantage of the versatility of TA, a one-pot method is proposed herein to produce TA-modified gelatin hydrogels with the aid ...

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Section: Resultsmentioning

confidence: 99%

Tannin‐Tethered Gelatin Hydrogels with Considerable Self‐Healing and Adhesive Performances

Zhao

Long

et al. 2019

Macro Materials & Eng

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“…[31,32] Comparing with single or double hydrogen bonding, the ureido-pyrimidinone (UPy) unit which was first reported by the Meijer' group, can form more stable quadruplehydrogen-bonded dimers with an ultrahigh association constant of 6 × 10 7 m −1 and superior bonding energy of 44 kJ mol −1 in chloroform, making it one of the most promising candidates as supramolecular building blocks for constructing the fast selfhealing materials with high healing efficiency. [33][34][35][36][37][38][39][40] Herein, through covalently integrating a small amount of UPy moieties with a linear polymer poly(acrylic acid) (PAA), we report a new supramolecular polymer which can serve as self-healable binder for high-performance silicon nanoparticle (SiNP) anodes. The supramolecular polymer offers strong adhesion strength with SiNP, which can withstand large volume expansion and release the internal stress of SiNP during repeated lithiation/delithiation process.…”

Section: Introductionmentioning

confidence: 99%

A Quadruple‐Hydrogen‐Bonded Supramolecular Binder for High‐Performance Silicon Anodes in Lithium‐Ion Batteries

Zhang

Yang

Chen

et al. 2018

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With extremely high specific capacity, silicon has attracted enormous interest as a promising anode material for next-generation lithium-ion batteries. However, silicon suffers from a large volume variation during charge/discharge cycles, which leads to the pulverization of the silicon and subsequent separation from the conductive additives, eventually resulting in rapid capacity fading and poor cycle life. Here, it is shown that the utilization of a self-healable supramolecular polymer, which is facilely synthesized by copolymerization of tert-butyl acrylate and an ureido-pyrimidinone monomer followed by hydrolysis, can greatly reduce the side effects caused by the volume variation of silicon particles. The obtained polymer is demonstrated to have an excellent self-healing ability due to its quadruple-hydrogen-bonding dynamic interaction. An electrode using this self-healing supramolecular polymer as binder exhibits an initial discharge capacity as high as 4194 mAh g and a Coulombic efficiency of 86.4%, and maintains a high capacity of 2638 mAh g after 110 cycles, revealing significant improvement of the electrochemical performance in comparison with that of Si anodes using conventional binders. The supramolecular binder can be further applicable for silicon/carbon anodes and therefore this supramolecular strategy may increase the choice of amendable binders to improve the cycle life and energy density of high-capacity Li-ion batteries.

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“…For example, reversible addition-fragmentation chain transfer polymerization (RAFT) was employed to prepare UPy-contained multi-block supramolecular materials [24][25][26][27][28][29]. In addition, UPy moieties could be grafted onto the polymeric backbone to obtain dynamic hydrogen-bonding cross-linked materials [30][31][32][33]. The UPy group has been commonly modified to the end of a small molecule [34] or polymers [35][36][37][38] in order to prepare a supramolecular cross-linking dynamic network.…”

Section: Introductionmentioning

confidence: 99%

A robust self-healing polyurethane elastomer: From H-bonds and stacking interactions to well-defined microphase morphology

Fan

Huang

et al. 2019

Sci. China Mater.

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Self-healing materials have attracted considerable attention because of their improved safety, lifetime, energy efficiency and environmental impact. Supramolecular interactions have been extensively considered in the field of self-healing materials due to their excellent reversibility and sensitive responsiveness to environmental stimuli. However, development of a polymeric material with good mechanical performance as well as self-healing capacity is very challenging. In this study, we report a robust self-healing polyurethane (PU) elastomer polypropylene glycol-2-amino-5-(2hydroxyethyl)-6-methylpyrimidin-4-ol (PPG-mUPy) by integrating ureidopyrimidone (UPy) motifs with a PPG segment with a well-defined architecture and microphase morphology. To balance the self-healing capacity and mechanical performance, a thermal-triggered switch of H-bonding is introduced. The quadruple H-bonded UPy dimeric moieties in the backbone induce phase separation to form a hard domain as well as enable further aggregation into microcrystals by virtue of the stacking interactions, which are stable in ambient temperature. This feature endows the PU with high mechanical strength. Meanwhile, a high healing efficiency can be realized, when the reversibility of the H-bond was unlocked from the stacking at higher temperature. An optimized sample PPG 1000-mUPy 50% with a good balance of mechanical performance (20.62 MPa of tensile strength) and healing efficiency (93% in tensile strength) was achieved. This strategy will provide a new idea for developing robust self-healing polymers.

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Self‐Healing Gelatin Hydrogels Cross‐Linked by Combining Multiple Hydrogen Bonding and Ionic Coordination

Cited by 80 publications

References 51 publications

Tannin‐Tethered Gelatin Hydrogels with Considerable Self‐Healing and Adhesive Performances

Tannin‐Tethered Gelatin Hydrogels with Considerable Self‐Healing and Adhesive Performances

A Quadruple‐Hydrogen‐Bonded Supramolecular Binder for High‐Performance Silicon Anodes in Lithium‐Ion Batteries

A robust self-healing polyurethane elastomer: From H-bonds and stacking interactions to well-defined microphase morphology

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