pH‐Based Regulation of Hydrogel Mechanical Properties Through Mussel‐Inspired Chemistry and Processing

Barrett, Devin G.; Fullenkamp, Dominic E; He, Linghui; Holten‐Andersen, Niels; Lee, Ka Yee C.; Messersmith, Phillip B.

doi:10.1002/adfm.201201922

Cited by 228 publications

(263 citation statements)

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“…Integrating chemical insights with higher length scale structure and architecture as well as time scales is likely to provide the best opportunities for improved adhesion technology. So far, there are few initiatives in this direction (Barrett et al, 2012;Menyo et al, 2015;Zhao et al, 2016).…”

Section: Resultsmentioning

confidence: 99%

“…(2) some proportion of the Dopa adsorbs to form bidentate complexes with the surface; (3) owing to trace O 2 or Fe 3+ present, unadsorbed Dopa undergoes a one-or two-electron oxidation to Dopa-quinone (Barrett et al, 2012), which has poor surface bonding properties; to decrease Dopa-quinone's tendency to undergo oxidation, mussels have evolved two rescue pathways: (4) Dopa-quinones tautomerize to dehydroDopa, or (5) thiolates in Mfp-6 donate electrons to restore Dopa from quinone.…”

Section: Redoxmentioning

confidence: 99%

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Mussel adhesion – essential footwork

Waite

2017

Journal of Experimental Biology

527

744

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Robust adhesion to wet, salt-encrusted, corroded and slimy surfaces has been an essential adaptation in the life histories of sessile marine organisms for hundreds of millions of years, but it remains a major impasse for technology. Mussel adhesion has served as one of many model systems providing a fundamental understanding of what is required for attachment to wet surfaces. Most polymer engineers have focused on the use of 3,4-dihydroxyphenyl-L-alanine (Dopa), a peculiar but abundant catecholic amino acid in mussel adhesive proteins. The premise of this Review is that although Dopa does have the potential for diverse cohesive and adhesive interactions, these will be difficult to achieve in synthetic homologs without a deeper knowledge of mussel biology; that is, how, at different length and time scales, mussels regulate the reactivity of their adhesive proteins. To deposit adhesive proteins onto target surfaces, the mussel foot creates an insulated reaction chamber with extreme reaction conditions such as low pH, low ionic strength and high reducing poise. These conditions enable adhesive proteins to undergo controlled fluid-fluid phase separation, surface adsorption and spreading, microstructure formation and, finally, solidification.

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Section: Resultsmentioning

confidence: 99%

Section: Redoxmentioning

confidence: 99%

Mussel adhesion – essential footwork

Waite

2017

Journal of Experimental Biology

527

744

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“…Some physical hydrogels can undergo a sol-gel phase transition (SGPT) 7 as a response to external stimuli. 8,9 In contrast, the chemically cross-linked hydrogels are permanent networks formed through covalent bonds, enabling volume phase transitions (VPT) 10 when exposed to external physical or chemical stimuli, including temperature, 11,12 light, electric field, 13 ionic strength, 14 pH, 15 enzyme, 16 and biomolecules. As a result of these characteristics, hydrogels can be used as superabsorbents, 17,18 packaging materials, 19 soft lenses, 20 microfluidic devices, 21 catalyst supports, 22,23 biomedical materials, 24,25 and bioactuators 26 ( Fig.…”

Section: Introductionmentioning

confidence: 99%

Recent advances in clay mineral-containing nanocomposite hydrogels

et al. 2015

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Clay mineral-containing nanocomposite hydrogels have been proven to have exceptional composition, properties, and applications, and consequently have attracted a significant amount of research effort over the past few years. The objective of this paper is to summarize and evaluate scientific advances in clay mineral-containing nanocomposite hydrogels in terms of their specific preparation, formation mechanisms, properties, and applications, and to identify the prevailing challenges and future directions in the field. The state-of-the-art of existing technologies and insights into the exfoliation of layered clay minerals, in particular montmorillonite and LAPONITE s , are discussed first. The formation and structural characteristics of polymer/clay nanocomposite hydrogels made from in situ free radical polymerization, supramolecular assembly, and freezing-thawing cycles are then examined. Studies indicate that additional hydrogen bonding, electrostatic interactions, coordination bonds, hydrophobic interaction, and even covalent bonds could occur between the clay mineral nanoplatelets and polymer chains, thereby leading to the formation of unique three-dimensional networks. Accordingly, the hydrogels exhibit exceptional optical and mechanical properties, swelling-deswelling behavior, and stimuli-responsiveness, reflecting the remarkable effects of clay minerals. With the pivotal roles of clay minerals in clay mineral-containing nanocomposite hydrogels, the nanocomposite hydrogels possess great potential as superabsorbents, drug vehicles, tissue scaffolds, wound dressing, and biosensors. Future studies should lay emphasis on the formation mechanisms with in-depth insights into interfacial interactions, the tactical functionalization of clay minerals and polymers for desired properties, and expanding of their applications.

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“…9, 10 Chujo et al also employed the bipyridine chemistry to include polyoxazoline into the gel matrix. 11,12 Cu 2+ /carboxyl, 13 Fe 3+ /catechol, 14,15 and Ni 2+ /histidine interactions were also employed. 16,17 Self-healing is a very interesting and useful feature of metal-coordinated gels; broken gel pieces can seal together with a mild mechanical force.…”

mentioning

confidence: 99%

Self-healing metal-coordinated hydrogels using nucleotide ligands

et al. 2015

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A supramolecular gel formed by Zn 2+ coordination with adenosine monophosphate (AMP) is reported. The adenine base, the monophosphate, and Zn 2+ are all important for gel formation. Mechanically disrupted gels can re-form upon centrifugation; applications of this gel for guest molecule entrapment are explored.Supramolecular gels have received considerable attention in recent years both as intriguing examples of self-assembly and as a means of creating smart materials.1-5 These gels are formed by noncovalent interactions to assemble supramolecular networks that trap solvent. 6Among the various types of supramolecular gels, those crosslinked by metal coordination are particular interesting. A few types of ligands have been developed for this purpose. For example, Craig and coworkers reported organopalladium−pyridine coordination. 16,17 Self-healing is a very interesting and useful feature of metal-coordinated gels; broken gel pieces can seal together with a mild mechanical force.Most of previously reported gels have to use specially designed ligands (e.g. incorporating a segment of PEG chain in addition to the metal ligand) to facilitate solvent trapping and gelation. Few reports are based on pure small molecule ligands. We reason that small molecule ligands will allow a higher metal density and thus may display different properties.Adenine, a purine nucleobase, is an important ligand in supramolecular chemistry. Adenine and its derivatives can form many complexes by coordination (with metal ions) and hydrogen bonding (with organic molecules). [18][19][20] With metal ions, it may form metalorganic frameworks, 21 and nanoparticles. [22][23][24][25] Recently, the gelation of adenine with tricarboxylic acid compounds was reported based on hydrogen bonding and π-π stacking. 26,27 We are interested in exploring whether it is possible to achieve gelation by metal coordination with adenine derivatives. Guanine and its derivatives have been mixed with monovalent metal ions to form gels based on quadruplex formation. 28-31 However, little has been done on adenine derivatives. Nanoparticles are the most common products. [22][23][24][25] Compared to nanoparticles, hydrogels are more attractive materials for making stimuli-responsible materials. [32][33][34][35][36][37][38][39] In this work, we communicate such an example, its property in guest molecule encapsulation, and healing.Since most previous work focused on adenine nucleobase and nucleoside as ligands, we started with nucleotide coordination in this work. Zn 2+ was chosen as the metal because it is a good Lewis acid that can be coordinated by a diverse range of ligands. In addition, it is a relatively biocompatible metal with low toxicity. We first studied the reaction between Zn 2+ and three kinds of nucleotides (AMP, GMP and CMP). TMP was not included since thymine has very weak coordination ability at neutral pH. Zn 2+ was respectively titrated into the solutions of AMP, GMP and CMP, and the UV-vis extinction at 550 nm was recorded. Since none of the products are c...

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pH‐Based Regulation of Hydrogel Mechanical Properties Through Mussel‐Inspired Chemistry and Processing

Cited by 228 publications

References 55 publications

Mussel adhesion – essential footwork

Mussel adhesion – essential footwork

Recent advances in clay mineral-containing nanocomposite hydrogels

Self-healing metal-coordinated hydrogels using nucleotide ligands

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