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Wet Adhesion: New Chemistries, Models and Translation to Materials

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A special issue of International Journal of Molecular Sciences (ISSN 1422-0067). This special issue belongs to the section "Materials Science".

Deadline for manuscript submissions: closed (31 December 2019) | Viewed by 26968

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Prof. Dr. Marco d'Ischia

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Department of Chemical Sciences, University of Naples Federico II, Via Cintia 4, I-80126 Naples, Italy
Interests: structure, synthesis, physicochemical properties, and reactivity of melanins; polydopamine and related bioinspired functional materials for underwater surface functionalization and hybrid nanostructures for bioelectronics and biomedical applications; design, antioxidant properties, and reactivity of bioactive phenolic and quinone compounds; free radical oxidations and nature-inspired redox-active systems for biomedical and technological applications; chemistry and physicochemical properties of natural or bioinspired heterocyclic compounds; bioorganic chemistry of organic sulphur and selenium compounds; model reactions and transformation pathways of polycyclic aromatic hydrocarbons and derivatives of astrochemical relevance
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Dr. Julieta Paez

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Leibniz-Institut für Neue Materialien GmbH. Campus D2-2, D-66123 Saarbrücken, Germany
Interests: biomaterials; bioinspired chemistry and materials; tissue adhesives; adhesion under wet conditions; crosslinking; hydrogels; chemical reactions under physiological conditions; catechol chemistry; materials for 3D cell encapsulation; thiol-mediated coupling chemistries; bioinks for 3D bioprinting technologies

Dr. habil. Alla Synytska

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Department Polymer Interfaces, Leibniz-Institut für Polymerforschung Dresden e.V., Dresden, Germany
Interests: physical chemistry of polymers, colloids, and interfaces; design of soft and hybrid colloids with chemical and geometrical anisotropy; assembly; bioinspired design of soft polymer-based materials with tailored adhesion properties in complex environments (wet, icy); electrokinetic, wetting, and adhesion phenomena at soft interfaces; adhesion testing under water with AFM colloidal probe technique
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Special Issue Information

Dear Colleagues，

One of the fundamental challenges in materials science is the development of synthetic durable adhesives that perform under wet conditions. Despite the great progress achieved so far, most man-made adhesives deteriorate and ultimately fail in watery environments. Conversely, certain aquatic animals like mussels, sandcastle worms, and freshwater caddisfly larvae have long solved this challenge through evolution. These organisms show impressive underwater adhesion performance and, therefore, provide a source of inspiration for the development of new adhesive materials. Advancing the field of wet adhesives will certainly have a profound industrial and technological impact that spans from medicine, coating technologies, and materials for construction, to additive manufacturing.

In this Special Issue, we aim to bring together contributions from different research groups working in the field of underwater adhesion, within a multidisciplinary approach that combines fundamental chemistry and physics, materials science, and engineering. We are interested in contributions that elucidate the mechanisms of bio-adhesion, extract its main design principles as guidelines for development of synthetic adhesive materials, and promote their application to solve current and emerging challenges in aqueous adhesion.

Prof. Dr. Marco d'Ischia
Dr. Julieta Paez
Dr. habil. Alla Synytska
Guest Editors

Manuscript Submission Information

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Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. International Journal of Molecular Sciences is an international peer-reviewed open access semimonthly journal published by MDPI.

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Keywords

Hydrogels, coatings, and adhesives;
Bioinspired and biomimetic adhesives;
Structure/property/function relationships;
Catechol chemistry, complex coacervation;
Novel curing and polymerization mechanisms;
Novel solutions for industrial applications (adhesive processing, storage, etc.);
Biomedical applications;
Adhesion on demand;
Adhesives from renewable feedstock;
Novel characterization techniques of wet adhesive properties;
Biochemistry and processing of natural bioadhesives;
Theoretical and computational studies, modeling;
Multifunctional adhesive materials (self-healing, stimuli-responsive, cell-instructive, antifouling, antioxidant, printable, etc.);
Additive manufacturing and biofabrication.

Published Papers (7 papers)

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Research

16 pages, 3655 KiB

Open AccessArticle

Interpenetrating Hydrogel Networks Enhance Mechanical Stability, Rheological Properties, Release Behavior and Adhesiveness of Platelet-Rich Plasma

by Roberta Censi, Cristina Casadidio, Siyuan Deng, Maria Rosa Gigliobianco, Maria Giovanna Sabbieti, Dimitrios Agas, Fulvio Laus and Piera Di Martino

Int. J. Mol. Sci. 2020, 21(4), 1399; https://doi.org/10.3390/ijms21041399 - 19 Feb 2020

Cited by 18 | Viewed by 3892

Abstract

Platelet-rich plasma (PRP) has attracted much attention for the treatment of articular cartilage defects or wounds due to its intrinsic content of growth factors relevant for tissue repair. However, the short residence time of PRP in vivo, due to the action of lytic enzymes, its weak mechanical properties and the consequent short-term release of bioactive factors has restricted its application and efficacy. The present work aimed at designing new formulation strategies for PRP, based on the use of platelet concentrate (PC)-loaded hydrogels or interpenetrating polymer networks, directed at improving mechanical stability and sustaining the release of bioactive growth factors over a prolonged time-span. The interpenetrating hydrogels comprised two polymer networks interlaced on a molecular scale: (a) a first covalent network of thermosensitive and biodegradable vinyl sulfone bearing p(hydroxypropyl methacrylamide-lacate)-polyethylene glycol triblock copolymers, tandem cross-linked by thermal gelation and Michael addition when combined with thiolated hyaluronic acid, and (b) a second network composed of cross-linked fibrin. The PC-loaded hydrogels, instead, was formed only by network (a). All the designed and successfully synthesized formulations greatly increased the stability of PRP in vitro, leading to significant increase in degradation time and storage modulus of PRP gel. The resulting viscoelastic networks showed the ability to controllably release platelet derived growth factor and transforming growth factr β1, and to improve the tissue adhesiveness of PRP. The newly developed hydrogels show great potential for application in the field of wound healing, cartilage repair and beyond. Full article

(This article belongs to the Special Issue Wet Adhesion: New Chemistries, Models and Translation to Materials)

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23 pages, 25294 KiB

Open AccessArticle

Integrative Transcriptome and Proteome Analysis of the Tube Foot and Adhesive Secretions of the Sea Urchin Paracentrotus lividus

by Robert Pjeta, Herbert Lindner, Leopold Kremser, Willi Salvenmoser, Daniel Sobral, Peter Ladurner and Romana Santos

Int. J. Mol. Sci. 2020, 21(3), 946; https://doi.org/10.3390/ijms21030946 - 31 Jan 2020

Cited by 17 | Viewed by 4141

Abstract

Echinoderms, such as the rock-boring sea urchin Paracentrotus lividus, attach temporarily to surfaces during locomotion using their tube feet. They can attach firmly to any substrate and release from it within seconds through the secretion of unknown molecules. The composition of the adhesive, as well as the releasing secretion, remains largely unknown. This study re-analyzed a differential proteome dataset from Lebesgue et al. by mapping mass spectrometry-derived peptides to a P. lividus de novo transcriptome generated in this study. This resulted in a drastic increase in mapped proteins in comparison to the previous publication. The data were subsequently combined with a differential RNAseq approach to identify potential adhesion candidate genes. A gene expression analysis of 59 transcripts using whole mount in situ hybridization led to the identification of 16 transcripts potentially involved in bioadhesion. In the future these data could be useful for the production of synthetic reversible adhesives for industrial and medical purposes. Full article

(This article belongs to the Special Issue Wet Adhesion: New Chemistries, Models and Translation to Materials)

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22 pages, 8050 KiB

Open AccessArticle

Tuning the Interactions in Multiresponsive Complex Coacervate-Based Underwater Adhesives

by Marco Dompé, Francisco J. Cedano-Serrano, Mehdi Vahdati, Ugo Sidoli, Olaf Heckert, Alla Synytska, Dominique Hourdet, Costantino Creton, Jasper van der Gucht, Thomas Kodger and Marleen Kamperman

Int. J. Mol. Sci. 2020, 21(1), 100; https://doi.org/10.3390/ijms21010100 - 21 Dec 2019

Cited by 15 | Viewed by 4835

Abstract

In this work, we report the systematic investigation of a multiresponsive complex coacervate-based underwater adhesive, obtained by combining polyelectrolyte domains and thermoresponsive poly(N-isopropylacrylamide) (PNIPAM) units. This material exhibits a transition from liquid to solid but, differently from most reactive glues, is completely held together by non-covalent interactions, i.e., electrostatic and hydrophobic. Because the solidification results in a kinetically trapped morphology, the final mechanical properties strongly depend on the preparation conditions and on the surrounding environment. A systematic study is performed to assess the effect of ionic strength and of PNIPAM content on the thermal, rheological and adhesive properties. This study enables the optimization of polymer composition and environmental conditions for this underwater adhesive system. The best performance with a work of adhesion of 6.5 J/m² was found for the complex coacervates prepared at high ionic strength (0.75 M NaCl) and at an optimal PNIPAM content around 30% mol/mol. The high ionic strength enables injectability, while the hydrated PNIPAM domains provide additional dissipation, without softening the material so much that it becomes too weak to resist detaching stress. Full article

(This article belongs to the Special Issue Wet Adhesion: New Chemistries, Models and Translation to Materials)

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23 pages, 3453 KiB

Open AccessArticle

Thermo-Responsive Polymer Brushes with Side Graft Chains: Relationship Between Molecular Architecture and Underwater Adherence

by Ugo Sidoli, Hisaschi T. Tee, Ivan Raguzin, Jakob Mühldorfer, Frederik R. Wurm and Alla Synytska

Int. J. Mol. Sci. 2019, 20(24), 6295; https://doi.org/10.3390/ijms20246295 - 13 Dec 2019

Cited by 4 | Viewed by 3161

Abstract

During the last few decades, wet adhesives have been developed for applications in various fields. Nonetheless, key questions such as the most suitable polymer architecture as well as the most suitable chemical composition remain open. In this article, we investigate the underwater adhesion properties of novel responsive polymer brushes with side graft chain architecture prepared using “grafting through” approach on flat surfaces. The incorporation in the backbone of thermo-responsive poly(N-isopropylacrylamide) (PNIPAm) allowed us to obtain LCST behavior in the final layers. PNIPAm is co-polymerized with poly(methyl ethylene phosphate) (PMEP), a poloyphosphoester. The final materials are characterized studying the surface-grafted polymer as well as the polymer from the bulk solution, and pure PNIPAm brush is used as reference. PNIPAm-g-PMEP copolymers retain the responsive behavior of PNIPAm: when T > LCST, a clear switching of properties is observed. More specifically, all layers above the critical temperature show collapse of the chains, increased hydrophobicity and variation of the surface charge even if no ionizable groups are present. Secondly, effect of adhesion parameters such as debonding rate and contact time is studied. Thirdly, the reversibility of the adhesive properties is confirmed by performing adhesion cycles. Finally, the adhesive properties of the layers are studied below and above the LCST against hydrophilic and hydrophobic substrates. Full article

(This article belongs to the Special Issue Wet Adhesion: New Chemistries, Models and Translation to Materials)

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15 pages, 1995 KiB

Open AccessArticle

Thermoresponsive Catechol Based-Polyelectrolyte Complex Coatings for Controlled Release of Bortezomib

by Berthold Reis, David Vehlow, Tarik Rust, Dirk Kuckling and Martin Müller

Int. J. Mol. Sci. 2019, 20(23), 6081; https://doi.org/10.3390/ijms20236081 - 02 Dec 2019

Cited by 5 | Viewed by 3077

Abstract

To overcome the high relapse rate of multiple myeloma (MM), a drug delivery coating for functionalization of bone substitution materials (BSM) is reported based on adhesive, catechol-containing and stimuli-responsive polyelectrolyte complexes (PECs). This system is designed to deliver the MM drug bortezomib (BZM) directly to the anatomical site of action. To establish a gradual BZM release, the naturally occurring caffeic acid (CA) is coupled oxidatively to form poly(caffeic acid) (PCA), which is used as a polyanion for complexation. The catechol functionalities within the PCA are particularly suitable to form esters with the boronic acid group of the BZM, which are then cleaved in the body fluid to administer the drug. To achieve a more thorough control of the release, the thermoresponsive poly(N-isoproplyacrylamide-co-dimethylaminoethylmethacrylate) (P(NIPAM-co-DMAEMA)) was used as a polycation. Using turbidity measurements, it was proven that the lower critical solution temperature (LCST) character of this polymer was transferred to the PECs. Further special temperature dependent attenuated total reflection infrared spectroscopy (ATR-FTIR) showed that coatings formed by PEC immobilization exhibit a similar thermoresponsive performance. By loading the coatings with BZM and studying the release in a model system, via UV/Vis it was observed, that both aims, the retardation and the stimuli control of the release, were achieved. Full article

(This article belongs to the Special Issue Wet Adhesion: New Chemistries, Models and Translation to Materials)

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15 pages, 4651 KiB

Open AccessArticle

Variable Smear Layer and Adhesive Application: The Pursuit of Clinical Relevance in Bond Strength Testing

by Abu Faem Mohammad Almas Chowdhury, Rafiqul Islam, Arefin Alam, Mariko Matsumoto, Monica Yamauti, Ricardo Marins Carvalho and Hidehiko Sano

Int. J. Mol. Sci. 2019, 20(21), 5381; https://doi.org/10.3390/ijms20215381 - 29 Oct 2019

Cited by 18 | Viewed by 4710

Abstract

The removal or modification of smear layers that cover the dentin is critical to allow the penetration of adhesive molecules and to ensure a strong bond between resin and dentin. Aiming to establish a model for clinically-relevant dentin-bond testing, we evaluated the effects of smear layers created by abrasives having similar coarseness (180-grit SiC paper; fine-grit diamond bur) and application modes (single application; double application) on the microtensile bond strengths (µTBS) of two currently available universal adhesives (G-Premio Bond; Scotchbond Universal Adhesive) and a two-step self-etch adhesive (Clearfil Megabond 2). Sixty extracted human third molars were used for the μTBS test. Data were analyzed by three-way ANOVA and Tukey’s test (α = 0.05). Fracture modes were determined using stereomicroscopy. An additional 24 third molars were prepared for observation of the resin–dentin interface by TEM and adhesive-smear layer interaction by SEM. μTBS was significantly affected by the adhesives and their application modes (p < 0.001), implying that the double application of universal adhesives should be recommended to improve their performance. The effect of smear layers was not significant (p > 0.05), indicating that 180-grit SiC papers could be used to prepare dentin as a substitute for fine-grit diamond burs for dentin-bond testing in laboratory settings. Full article

(This article belongs to the Special Issue Wet Adhesion: New Chemistries, Models and Translation to Materials)

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10 pages, 1968 KiB

Open AccessArticle

Reaction-Based, Fluorescent Film Deposition from Dopamine and a Diamine-Tethered, Bis–Resorcinol Coupler

by Maria Laura Alfieri, Mariagrazia Iacomino, Alessandra Napolitano and Marco d’Ischia

Int. J. Mol. Sci. 2019, 20(18), 4532; https://doi.org/10.3390/ijms20184532 - 13 Sep 2019

Cited by 3 | Viewed by 2323

Abstract

The reaction-based deposition on various surfaces of an all-organic fluorescent coating is reported here, involving autoxidation of 2 mM dopamine in carbonate buffer at pH 9.0, in the presence of a 1 mM diamine–resorcinol coupler (Bis–Res) prepared from 2,4-dihydroxybenzaldehyde and hexamethylenediamine (HMDA). Spectral analysis of the films coupled with an LC-MS investigation of the yellow fluorescent mixture was compatible with the formation and deposition of HMDA-linked methanobenzofuroazocinone fluorophores. Both the emission properties and hydrophobicity of the film were abated in a reversible manner following exposure to acid vapors. These results provide an entry to efficient and practical fluorescent coating methodologies based on in situ generation and the deposition of wet adhesive, as well as fluorescent materials combining a strongly emitting fluorophore with the film-forming properties of long chain diamines. Full article

(This article belongs to the Special Issue Wet Adhesion: New Chemistries, Models and Translation to Materials)

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