Tuning the Interactions in Multiresponsive Complex Coacervate-Based Underwater Adhesives

Dompè, Marco; Cedano‐Serrano, Francisco J.; Vahdati, Mehdi; Sidoli, Ugo; Heckert, Olaf; Synytska, Alla; Hourdet, Dominique; Creton, Costantino; Gucht, Jasper van der; Kodger, Thomas E.; Kamperman, Marleen

doi:10.3390/ijms21010100

Cited by 18 publications

(24 citation statements)

References 51 publications

(88 reference statements)

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“…This is also reflected in an immediate change from transparency to an opaque color (Figure 9D) which is plausibly due to the formation of microscopic pockets of water. 37,40,49 In its hardened state, it has an adhesion energy of 3.5 J.m -2 similar to those of Dompé and coworkers (2-6.5 J.m -2 ) under the same experimental conditions. 37,40 However, it appears softer and less stretchable than the non-injectable 0.1 M coacervate.…”

Section: Adhesiveness In Physiological Conditionssupporting

confidence: 79%

“…37,40,49 In its hardened state, it has an adhesion energy of 3.5 J.m -2 similar to those of Dompé and coworkers (2-6.5 J.m -2 ) under the same experimental conditions. 37,40 However, it appears softer and less stretchable than the non-injectable 0.1 M coacervate. Although this further confirms that a salt switch is a promising strategy to reinforce coacervate-based underwater adhesives, there seems to be an upper limit to the final mechanical properties which can be achieved with this strategy.…”

Section: Adhesiveness In Physiological Conditionssupporting

confidence: 79%

“…6,32,33,40 Dompé and coworkers recently proposed a novel macromolecular design to compensate for the slow salt switch of liquid-like coacervates by incorporating thermoresponsive grafts onto the polyelectrolyte backbones with DPs above 1000. 37,40 This endowed the adhesive with a rapid initial hardening upon heating at body temperature, due to the formation of strong hydrophobic domains.…”

Section: Introductionmentioning

confidence: 99%

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Coacervate-Based Underwater Adhesives in Physiological Conditions

Vahdati

Cedano‐Serrano

Creton

et al. 2020

ACS Appl. Polym. Mater.

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Soft underwater adhesives which can function in physiological environments are in high demandfor biomedical applications. This study establishes a clear link between the composition and mechanical properties of complex coacervates from poly(2-acrylamido-2-methylpropane sulfonic acid) (PAMPS) and poly (N,N-[(dimethylamino) propyl]methacrylamide) (PMADAP) with degrees of polymerization (DP) close to 100. Choosing such low DPs offers several advantages including low water contents corresponding to strong mechanical properties while remaining in the unentangled regime to allow injectability at high salt concentrations. Most importantly, this strategy favors the occurrence of the salt-induced sol-gel transition near physiological concentrations, where these materials form sticky hydrogels due to their viscoelastic dissipative nature. The fluid-like coacervate prepared at 0.75 M NaCl behaves as a soft adhesive when injected in physiological conditions. This adhesive satisfies a nontrivial tradeoff between injectability and final mechanical properties. Alternatively, the gel-like coacervate prepared at 0.1 M NaCl offers an instant-stick solution in physiological conditions with a remarkable underwater adhesion energy of 65 J.m -2 without the need to a trigger or any form of postreinforcement. These coacervates mimic the behavior of soft adhesives in air and may be useful as biomedical adhesives.

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Section: Adhesiveness In Physiological Conditionssupporting

confidence: 79%

Section: Adhesiveness In Physiological Conditionssupporting

confidence: 79%

Section: Introductionmentioning

confidence: 99%

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Coacervate-Based Underwater Adhesives in Physiological Conditions

Vahdati

Cedano‐Serrano

Creton

et al. 2020

ACS Appl. Polym. Mater.

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“…Along those lines, several recent reports focused on the enhancement of underwater adhesion of complex coacervates by introducing short poly(N‐isopropylacrylamide) (PNIPAM) side chains on polyelectrolyte backbones. [ 18–20 ] These materials are injectable at room temperature, but form sticky hydrogels upon immersion in an aqueous medium above the transition temperature (also called lower critical solution temperature or LCST) of PNIPAM owing to both electrostatic and hydrophobic interactions. Meanwhile, Guo and co‐workers also reported the reversible formation of stable hydrogels upon heating aqueous solutions of graft copolymers designed either with a thermoresponsive PNIPAM backbone and hydrophilic poly( N , N ‐dimethylacrylamide) (PDMA) side chains or with the opposite topology, i.e., PDMA backbone with PNIPAM side‐chains.…”

Section: Figurementioning

confidence: 99%

“…This adhesive hydrogel is too soft for structural, industrial applications, but is already stronger than many similar adhesive hydrogels relying on weak physical interactions tested under experimentally comparable conditions. [ 18–20,43 ] This claim does not concern bioinspired systems taking advantage of stronger, and in most cases, irreversible interactions such as those based on catechol chemistry. [ 44,45 ] However, there are several instances of stronger underwater adhesives based on electrostatic interactions.…”

Section: Figurementioning

confidence: 99%

Thermally Triggered Injectable Underwater Adhesives

Vahdati

Ducouret

Creton

et al. 2020

Macromol. Rapid Commun.

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A novel bioinspired underwater adhesive based on the injectable aqueous solution of a graft copolymer with a thermoresponsive backbone is reported, which turns into a sticky hydrogel just below body temperature. With this topology, the collapse of the backbones upon the thermal transition leads to the formation of a percolating network of strong hydrophobic domains. Similar to pressure‐sensitive adhesives (PSAs), the hydrogel goes through fibrillation and extensive energy dissipation in large deformations, giving it an edge over conventional chemical hydrogels, which are typically elastic and inherently nonsticky. This capability comes from the hydrophobic nanoscaffold, which resists large deformations to minimize its contact with water. Since hydrophobic interactions are not weakened in water, the behavior of the hydrogel is maintained in aqueous medium. Chemistry‐insensitive adhesion of this hydrogel offers a major advantage over current injectable adhesives, which rely on in situ chemical crosslinking reactions with tissues.

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Bioinspired Underwater Adhesives

2021

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adhesive, causing plasticization, swelling, erosion, degradation, or hydrolysis of adhesives, which eventually leads to cohesive failure. [8,9] Therefore, the development of underwater adhesives remains a significant challenge.An efficient way of developing underwater adhesives is by taking inspiration from nature. For instance, sessile marine organisms such as mussels and sandcastle worms use L-3,4-dihydroxyphenylalanine (DOPA) to achieve permanent underwater adhesion, whereas aquatic creatures such as remora and clingfish use unique microstructures for temporary underwater attachment. [10][11][12][13] Inspired by these unique underwater adhesion strategies, significant progress has been made in the design and fabrication of novel underwater adhesives in the past decade.Previous reviews on underwater adhesion have mainly focused on the micromechanics and bonding mechanisms. Adhesives for soft and wet tissues and hydrogels have been discussed in other recent reviews. [1,[14][15][16] However, only a few have been devoted to bulk underwater adhesives. [10,12,13,[16][17][18][19][20] In this review, we summarize the currently reported adhesives that show macroscopic adhesion to mainly, but not limited to, solid surfaces under wet and underwater conditions. We provide an overview of the development and performance of underwater adhesives based on different bonding methods and mechanisms. In addition, we discuss the possible research directions and perspectives for underwater adhesives. Current Design Strategies for Underwater AdhesionThe keys to achieving wet adhesion are the breaking down of the hydration layer and interaction with the substrate surface, which can be designed at different length scales (Figure 1). [21][22][23] To achieve dehydration at the molecular level (∼nm), hydrophobic organic solvents, monomers, and polymers have been used to remove the hydration layer and facilitate surface wetting, especially for hydrophobic substrates. [24,25] The use of water-absorbing fillers, including inorganic substances and hydrophilic polymers, is an alternative strategy that is widely used for wet surfaces. [26][27][28] At a larger length scale (μm to mm), surface microstructures can promote water drainage to prevent permanent water trapping. [29] Accompanied by the dehydration process, the interfacial bonding of adhesives is achieved by the formation of covalent/ non-covalent bonds (∼nm), which highly depends on the interfacial chemistry between the adherend and the adhesive. [10] For Underwater adhesives are in high demand in both commercial and industrial sectors. Compared with adhesives used in dry (air) environments, adhesives used for wet or submerged surfaces in aqueous environments have specific challenges in development and performance. In this review, focus is on adhesives demonstrating macroscopic adhesion to wet/underwater substrates. The current strategies are first introduced for different types of underwater adhesives, and then an overview is provided of the development and performance of underwater ad...

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Tuning the Interactions in Multiresponsive Complex Coacervate-Based Underwater Adhesives

Cited by 18 publications

References 51 publications

Coacervate-Based Underwater Adhesives in Physiological Conditions

Coacervate-Based Underwater Adhesives in Physiological Conditions

Thermally Triggered Injectable Underwater Adhesives

Bioinspired Underwater Adhesives

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