Publications by authors named "Vincent Ball"

109 Publications

Dual role of tannic acid and pyrogallol incorporated in plaster of Paris: Morphology modification and release for antimicrobial properties.

Mater Sci Eng C Mater Biol Appl 2021 Aug 27;127:112209. Epub 2021 May 27.

Université de Strasbourg, Faculté de Chirurgie Dentaire, 8 rue Sainte Elisabeth, 67000 Strasbourg, France; Institut National de la Santé et de la Recherche Médicale, Unité Mixte de Recherche 1121, 11 rue Humann, 67085 Strasbourg Cedex, France. Electronic address:

The design of bioactive plasters is of major interest for the amelioration of dental and bone cements. In this article, a one pot and environmentally friendly strategy based on the addition of a cheap polyphenol-tannic acid (TA) or the main phenolic constituent of TA, namely pyrogallol (PY)- able to interact with calcium sulfate is proposed. Tannic acid and pyrogallol not only modify the morphology of the obtained plaster+TA/PY composites but a part of it is released and provides strong-up to twenty fold- antibacterial effect against Staphylococcus aureus. It is shown that the higher antibacterial efficiency of PY is related to a greater release compared to TA even if in solution the antibacterial effect of PY is lower than that of TA when reported on the basis of the molar concentration in PY units.
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http://dx.doi.org/10.1016/j.msec.2021.112209DOI Listing
August 2021

Insensitivity of dental pulp stem cells migration to substrate stiffness.

Biomaterials 2021 Jun 15;275:120969. Epub 2021 Jun 15.

Inserm UMR-S1121, Centre de Recherche en Biomédecine de Strasbourg (CRBS), 1 rue Eugène Boeckel, 67084, Strasbourg, France; Université de Strasbourg, Faculté de Chirurgie Dentaire, 8 rue Sainte Elisabeth, 67000, Strasbourg, France; Fédération de Médecine Translationnelle, Strasbourg, France. Electronic address:

Dental pulp stem cells (DPSCs) are a promising cell source for regeneration of dental pulp. Migration is a key event but influence of the microenvironment rigidity (5 kPa at the center of dental pulp to 20 GPa for the dentin) is largely unknown. Mechanical signals are transmitted from the extracellular matrix to the cytoskeleton, to the nuclei, and to the chromatin, potentially regulating gene expression. To identify the microenvironmental influence on migration, we analyzed motility on PDMS substrates with stiffness increasing from 1.5 kPa up to 2.5 MPa. We found that migration speed slightly increases as substrate stiffness decreases in correlation with decreasing focal adhesion size. Motility is relatively insensitive to substrate stiffness, even on a bi-rigidity PDMS substrate where DPSCs migrate without preferential direction. Migration is independent of both myosin II activity and YAP translocation after myosin II inhibition. Additionally, inhibition of Arp2/3 complex leads to significant speed decrease for all rigidities, suggesting contribution of the lamellipodia in the migration. Interestingly, the chromatin architecture remains stable after a 7-days exposure on the PDMS substrates for all rigidity. To design scaffold mimicking dental pulp environment, similar DPSCs migration for all rigidity, leaves field open to choose this mechanical parameter.
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http://dx.doi.org/10.1016/j.biomaterials.2021.120969DOI Listing
June 2021

Antibacterial and Bonding Properties of Universal Adhesive Dental Polymers Doped with Pyrogallol.

Polymers (Basel) 2021 May 11;13(10). Epub 2021 May 11.

Department of Endodontics, Faculty of Dental Medicine, Strasbourg University, 67000 Strasbourg, France.

This study investigated the antibacterial activity, bond strength to dentin (SBS), and ultra-morphology of the polymer-dentin interface of experimental adhesive systems doped with pyrogallol (PY), which is a ubiquitous phenolic moiety that is present in flavonoids and polyphenols. A universal adhesive containing 4-META and 10-MDP was used in this study. PY behaves as an antioxidant and anti-cancerogenic agent and it was incorporated into the adhesive at different concentrations (0.5 and 1 wt.%). The antibacterial activity and SBS were analyzed and the results were statistically analyzed. The ultra-morphology of the polymer-dentin interface was assessed using scanning electron microscopy (SEM). At 24 h, a lower antibacterial activity was observed for the control adhesive compared to those with 0.5% and 1% PY. No difference was seen in SBS between the three groups at 24 h. After 6 months, the SBS of the 0.5% PY adhesive was significantly lower than the other tested adhesives. The specimens created with 1% PY adhesive presented a higher bond strength at six months compared with that found at 24 h. No morphological differences were found at the polymer-dentin interfaces of the tested adhesives. Pyrogallol may be incorporated into modern universal adhesive systems to preserve the polymer-dentin bonding interface and confer a certain degree of antibacterial activity.
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http://dx.doi.org/10.3390/polym13101538DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8151108PMC
May 2021

Tannic acid speeds up the setting of mineral trioxide aggregate cements and improves its surface and bulk properties.

J Colloid Interface Sci 2021 May 8;589:318-326. Epub 2021 Jan 8.

Université de Strasbourg, Faculté de Chirurgie Dentaire, 8 rue Sainte Elisabeth, 67000 Strasbourg, France; Institut National de la Santé et de la Recherche Médicale, Unité Mixte de Recherche 1121, 11 rue Humann, 67085 Strasbourg Cedex, France. Electronic address:

Hypothesis: The setting time and mechanical properties of cements are a major technical concern for a long time in civil engineering. More recently those practical problems became a major concern for biomedical applications -in bone surgery and in dentistry- in particular concerning the setting time which should be minimized. The possibility to add organic additives to interact with the different constituting ions in cements constitutes a way to modify the setting kinetics. We made the assumption that a hydrolysable polyphenol like tannic acid could modify the setting time and the physical properties of Mineral Trioxide Aggregate (MTA).

Experiments: Tannic acid is added in variable proportions to the water used to set MTA. The formation of the hybrid organic-mineral cements is investigated using a combination of structural, chemical and mechanical methods. X-ray tomography was also used to investigate the changes in porosity and pore size distribution upon incorporation of tannic acid in MTA based cements. The hydrophilicity of the cements was evaluated by measuring the permeation kinetics of small water droplets.

Findings: We found that tannic acid allowed to reduce markedly the setting time of MTA based cements. The obtained cements have an increased hydrophilicity and display excellent resistance to compression. The number of pores but not the average pore size is also affected. The possible roles of tannic acid in modifying the cement properties are discussed.
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http://dx.doi.org/10.1016/j.jcis.2020.12.115DOI Listing
May 2021

Correlative Microscopy Insight on Electrodeposited Ultrathin Graphite Oxide Films.

J Phys Chem Lett 2020 Nov 14;11(21):9117-9122. Epub 2020 Oct 14.

Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), UMR 7504 CNRS-Université de Strasbourg, 23 rue du Loess, BP 43 Strasbourg Cedex 2, France.

Here, we present a correlative microscopic analysis of electrodeposited films from catechol solutions in aqueous electrolytes. The films were prepared in a miniaturized electrochemical cell and were analyzed by identical location transmission electron microscopy, scanning transmission X-ray microscopy, and atomic force microscopy. Thanks to this combined approach, we have shown that the electrodeposited films are constituted of ultrathin graphite oxide nanosheets. Detailed information about the electronic structure of the films was obtained by X-ray absorption near edge structure spectroscopy. These results show the large potential of soft electrochemical conditions for the bottom-up production of ultrathin graphite oxide nanosheet films via a one-pot green chemistry approach from simple organic building blocks.
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http://dx.doi.org/10.1021/acs.jpclett.0c02482DOI Listing
November 2020

Polyarginine Decorated Polydopamine Nanoparticles With Antimicrobial Properties for Functionalization of Hydrogels.

Front Bioeng Biotechnol 2020 18;8:982. Epub 2020 Aug 18.

Institut National de la Santé et de la Recherche Médicale, INSERM UMR 1121 "Biomaterials and Bioengineering", Strasbourg, France.

Polydopamine (PDA) nanoparticles are versatile structures that can be stabilized with proteins. In this study, we have demonstrated the feasibility of developing PDA/polypeptides complexes in the shape of nanoparticles. The polypeptide can also render the nanoparticle functional. Herein, we have developed antimicrobial nanoparticles with a narrow size distribution by decorating the polydopamine particles with a chain-length controlled antimicrobial agent Polyarginine (PAR). The obtained particles were 3.9 ± 1.7 nm in diameter and were not cytotoxic at 1:20 dilution and above. PAR-decorated nanoparticles have exhibited a strong antimicrobial activity against , one of the most common pathogen involved in implant infections. The minimum inhibitory concentration is 5 times less than the cytotoxicity levels. Then, PAR-decorated nanoparticles have been incorporated into gelatin hydrogels used as a model of tissue engineering scaffolds. These nanoparticles have given hydrogels strong antimicrobial properties without affecting their stability and biocompatibility while improving their mechanical properties (modulus of increased storage). Decorated polydopamine nanoparticles can be a versatile tool for the functionalization of hydrogels in regenerative medicine applications by providing bioactive properties.
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http://dx.doi.org/10.3389/fbioe.2020.00982DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7461895PMC
August 2020

A Clean and Tunable Mussel-Inspired Coating Technology by Enzymatic Deposition of Pseudo-Polydopamine (ψ-PDA) Thin Films from Tyramine.

Int J Mol Sci 2020 Jul 10;21(14). Epub 2020 Jul 10.

Department of Chemical Sciences, University of Naples Federico II, Via Cintia 21, 80126 Naples, Italy.

The tyrosinase-catalyzed oxidation of tyramine, leading to the deposition of pseudo-polydopamine (ψ-PDA) thin films, is disclosed herein as a superior technology for surface functionalization and coating at a neutral pH and at a low substrate concentration, compared to the standard autoxidative PDA coating protocols. Smooth ψ-PDA thin films of variable thickness up to 87 nm were obtained from 1 mM tyramine by varying tyrosinase concentrations (5-100 U/mL). Compared to the PDA films obtained by the similar enzymatic oxidation of 1 mM dopamine with tyrosinase (T-PDA), ψ-PDA displayed slower deposition kinetics, lower water contact angles in the range of 11°-28°, denoting higher hydrophilicity but similar UV-vis absorption profiles, as well as electrochemical properties and antioxidant activity. MALDI-MS analysis indicated for ψ-PDA a well defined pattern of peaks compatible with dopamine tetrameric structures degraded to a variable extent. The exposure to a tyramine solution of tyrosinase-loaded alginate spheres, or films deposited on glass or polyethylene, resulted in a rapid gel-confined ψ-PDA formation with no leakage or darkening of the solution, allowing the complete recovery and re-utilization of the unreacted tyramine. In contrast, an abundant PDA precipitation outside the gel was observed with dopamine under the same conditions. The ψ-PDA deposition by tyrosinase-catalyzed tyramine oxidation is thus proposed as a controllable and low-waste technology for selective surface functionalization and coating or for clean eumelanin particle production.
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http://dx.doi.org/10.3390/ijms21144873DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7402308PMC
July 2020

Clinical Presentation and Outcome of Patients With Spontaneous Coronary Artery Dissection Versus Atherosclerotic Coronary Plaque Dissection.

Crit Pathw Cardiol 2021 03;20(1):36-43

Department of Cardiovascular Medicine, Baystate Medical Center, Tufts University School of Medicine, Springfield, MA.

Background: Atherosclerotic coronary plaque dissection (ACPD) is one cause of acute coronary syndrome (ACS) caused by underlying atherosclerosis. Spontaneous coronary artery dissection (SCAD) occurs outside the setting of atherosclerosis among young women and individuals with few or no conventional atherosclerotic risk factors, and has emerged as an important cause of ACS, and sudden death. A comparison between ACPD and SCAD has not been previously addressed in the literature. Our study will compare ACPD and SCAD.

Methods: Patients with confirmed diagnosis of SCAD and ACPD were retrospectively identified from 30 centers in 4 Arab Gulf countries between January 2011 and December 2017. In-hospital (ventricular tachycardia/ventricular fibrillation, myocardial infarction (MI), percutaneous coronary intervention, dissection extension, cardiogenic shock, death, implantable cardioverter-defibrillator placement) and follow-up (MI, de novo SCAD, spontaneous superior mesenteric artery dissection, death) events were compared between them.

Results: Eighty-three cases of SCAD and 48 ACPD were compared. ACPD patients were more frequently male (91.67% vs. 49.40%, P < 0.001) and older (58.5 vs. 44, P < 0.001). Cardiovascular risk factors were more prevalent in patients with ACPD, including diabetes mellitus (60.4% vs. 25.3%), dyslipidemia (62.5% vs. 38.5%), and hypertension (62.5% vs. 31.3%), P < 0.001. Hospital presentation of ST-elevation MI was diagnosed in 48% of SCAD versus 27% of ACPD patients (P = 0.012). SCAD patients received medical-only treatment in 40% of cases and ACPD in 21% (P = 0.042). In-hospital and follow-up events were comparable in both groups (P = 0.25).

Conclusions: Despite a completely different pathophysiology of ACS between SCAD and ACPD, in-hospital and follow-up events were comparable.
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http://dx.doi.org/10.1097/HPC.0000000000000233DOI Listing
March 2021

Polyphenols in Dental Applications.

Bioengineering (Basel) 2020 Jul 7;7(3). Epub 2020 Jul 7.

Faculté de Chirurgie Dentaire, Université de Strasbourg, 8 rue Sainte Elisabeth, 67000 Strasbourg, France.

(1) Background: polyphenols are a broad class of molecules extracted from plants and have a large repertoire of biological activities. Biomimetic inspiration from the effects of tea or red wine on the surface of cups or glass lead to the emergence of versatile surface chemistry with polyphenols. Owing to their hydrogen bonding abilities, coordination chemistry with metallic cations and redox properties, polyphenols are able to interact, covalently or not, with a large repertoire of chemical moieties, and can hence be used to modify the surface chemistry of almost all classes of materials. (2) Methods: the use of polyphenols to modify the surface properties of dental materials, mostly enamel and dentin, to afford them with better adhesion to resins and improved biological properties, such as antimicrobial activity, started more than 20 years ago, but no general overview has been written to our knowledge. (3) Results: the present review is aimed to show that molecules from all the major classes of polyphenolics allow for low coast improvements of dental materials and engineering of dental tissues.
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http://dx.doi.org/10.3390/bioengineering7030072DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7552636PMC
July 2020

Effect of the Buffer on the Buildup and Stability of Tannic Acid/Collagen Multilayer Films Applied as Antibacterial Coatings.

ACS Appl Mater Interfaces 2020 May 6;12(20):22601-22612. Epub 2020 May 6.

Université de Strasbourg, CNRS, Institut Charles Sadron, UPR 22, 67034 Strasbourg Cedex 2, France.

The deposition of polyelectrolyte multilayers, obtained by the layer-by-layer (LbL) method, is a well-established technology to design biocompatible and antibacterial coatings aimed at preventing implant-associated infections. Several types of LbL films have been reported to exhibit antiadhesive and/or antibacterial (contact-killing or release-killing) properties governed not only by the incorporated compounds but also by their buildup conditions or their postbuildup treatments. Tannic acid (TA), a natural polyphenol, is known to inhibit the growth of several bacterial strains. In this work, we developed TA/collagen (TA/COL) LbL films built in acetate or citrate buffers at pH 4. Surprisingly, the used buffer impacts not only the physicochemical but also the antibacterial properties of the films. When incubated in physiological conditions, both types of TA/COL films released almost the same amount of TA depending on the last layer and showed an antibacterial effect against only for citrate-built films. Because of their granular topography, TA/COL citrate films exhibited an efficient release-killing effect with no cytotoxicity toward human gingival fibroblasts. Emphasis is put on a comprehensive evaluation of the physicochemical parameters driving the buildup and the antibacterial property of citrate films. Specifically, complexation strengths between TA and COL are different in the presence of the two buffers affecting the LbL deposition. This work constitutes an important step toward the use of polyphenols as an antibacterial agent when incorporated in LbL films.
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http://dx.doi.org/10.1021/acsami.0c04475DOI Listing
May 2020

Functionalization of PTFE Materials Using a Combination of Polydopamine and Platelet-Rich Fibrin.

J Surg Res 2020 07 13;251:254-261. Epub 2020 Mar 13.

Institut National de la Santé et de la Recherche Médicale, UMR_S 1121, Strasbourg, France.

Background: The diaphragm, which forms a physical barrier between the thoracic and the abdominal cavities, is also the major part of the respiratory system. Congenital diaphragmatic hernia (CDH) is a malformation of that partition muscle. Expanded polytetrafluoroethylene (e-PTFE), a synthetic nondegradable biomaterial, is currently used for the repair of diaphragm defects. Indeed, this hydrophobic biomaterial does not promote rapid and dense cell colonization. Surface modifications are needed to favor or even guide cellular responses.

Materials And Methods: In this context, we present here a practical and effective way of functionalization of the e-PTFE material. We investigated, by using electron microscopy, the coating with PRF (Platelet-Rich Fibrin) of PDA (Polydopamine) treated e-PTFE implant material.

Results: We demonstrate that this straightforward chemical functionalization with PDA increases the hydrophilicity of e-PTFE and thus improves tissue integration. Then, we demonstrated that whatever the contact time between PRF and e-PTFE and the centrifugation speed, the PDA coating on the e-PTFE biomaterial promotes further biological events like cell adhesion and spreading.

Conclusions: Our findings clearly show that this composite coating (chemically by using PDA + biologically by using PRF) method of e-PTFE is a simple, interesting and promising way to favor tissular integration of such biomaterials.
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http://dx.doi.org/10.1016/j.jss.2019.11.014DOI Listing
July 2020

Polydopamine as a stable and functional nanomaterial.

Colloids Surf B Biointerfaces 2020 Feb 14;186:110719. Epub 2019 Dec 14.

Université de Strasbourg, Faculté de Chirurgie Dentaire, 8 Rue Sainte Elisabeth, 67000, Strasbourg, France; Institut National de la Santé et de la Recherche Médicale, Unité mixte de recherche 1121, 11 Rue Humann, 67085, Strasbourg Cedex, France. Electronic address:

The mussel inspired chemistry of dopamine leading to versatile coatings on the surface of all kinds of materials in a one pot process was considered as the unique aspect of catecholamine for a long time. Only recently, research has been undertaken to valorize the simultaneous oxidation and colloid formation in dopamine solutions in the presence of an oxidant. This mini review summarizes the synthesis methods allowing to get controlled nanomaterials, either nanoparticles, hollow capsules or nanotubes and even chiral nanomaterials from dopamine solutions. Finally the applications of those nanomaterials will be described.
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http://dx.doi.org/10.1016/j.colsurfb.2019.110719DOI Listing
February 2020

Hofmeister Effects of Monovalent Sodium Salts in the Gelation Kinetics of Gelatin.

Authors:
Vincent Ball

J Phys Chem B 2019 10 30;123(40):8405-8410. Epub 2019 Sep 30.

Université de Strasbourg , Faculté de Chirurgie Dentaire , 8 rue Sainte Elisabeth , 67000 Strasbourg , France.

The gelation kinetics of gelatin depends on the presence of electrolytes, and the influence of cations with variable valency has been recently emphasized. However, acquired knowledge shows that the nature of anions has more influence on various properties of aqueous solutions than the nature of the cations. It is shown herein, using sodium salts of monovalent anions, that the gelation kinetics of gelatin is accelerated by the presence of highly kosmotropic anions like fluoride and strongly slowed, eventually inhibited, by the presence of chaotropic anions like thiocyanate and perchlorate. Overall the parameter characterizing the gelation kinetics, , is a linear function of the polarizability of the used salt in aqueous solution, which has been quantified independently by refractometry and using the Lorentz-Lorenz formula. It is also found that the same parameter characterizing the gelation kinetics is a linear function of the viscosity coefficient taken from the literature. The linear correlation coefficients are excellent in the case of halide anions (F, Cl, Br, I) but poorer when nonspherical anions like NO, SCN, and ClO are considered.
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http://dx.doi.org/10.1021/acs.jpcb.9b07615DOI Listing
October 2019

Astrochemistry and Astrobiology: Materials Sciencein Wonderland?

Int J Mol Sci 2019 Aug 21;20(17). Epub 2019 Aug 21.

Scuola Normale Superiore, Piazza dei Cavalieri 7, I-56126 Pisa, Italy.

Astrochemistry and astrobiology, the fascinating disciplines that strive to unravel the origin of life, have opened unprecedented and unpredicted vistas into exotic compounds as well as extreme or complex reaction conditions of potential relevance for a broad variety of applications. Representative, and so far little explored sources of inspiration include complex organic systems, such as polycyclic aromatic hydrocarbons (PAHs) and their derivatives; hydrogen cyanide (HCN) and formamide (HCONH) oligomers and polymers, like aminomalononitrile (AMN)-derived species; and exotic processes, such as solid-state photoreactions on mineral surfaces, phosphorylation by minerals, cold ice irradiation and proton bombardment, and thermal transformations in fumaroles. In addition, meteorites and minerals like forsterite, which dominate dust chemistry in the interstellar medium, may open new avenues for the discovery of innovative catalytic processes and unconventional methodologies. The aim of this review was to offer concise and inspiring, rather than comprehensive, examples of astrochemistry-related materials and systems that may be of relevance in areas such as surface functionalization, nanostructures, and hybrid material design, and for innovative technological solutions. The potential of computational methods to predict new properties from spectroscopic data and to assess plausible reaction pathways on both kinetic and thermodynamic grounds has also been highlighted.
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http://dx.doi.org/10.3390/ijms20174079DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6747172PMC
August 2019

Polydopamine Functionalization: A Smart and Efficient Way to Improve Host Responses to e-PTFE Implants.

Front Chem 2019 9;7:482. Epub 2019 Jul 9.

Institut National de la Santé et de la Recherche Médicale, UMR_S 1121, Strasbourg, France.

Among the different materials used as protheses for the treatment of Congenital Diaphragmatic Hernia, expanded polytetrafluoroethylene (e-PTFE) plays a leading role owing to its mechanical properties as explained in the first part of this review. However, this material is poorly cell adhesive, which is expected for its contact on the abdominal face, but should display specific tissue adhesion on its thoracic exposed faced. A side specific functionalization method is hence required. The deposition of a nanosized polydopamine film on PTFE is known to be possible but immersion of the e-PTFE membrane in an aerated dopamine solution leads to a functionalization not only on both faces of the membrane but also in its porous volume. The fact that polydopamine also forms at the water/air interface has allowed to transfer a polydopamine film on only one face of the e-PTFE membrane. The deposition method and applications of such Janus like membranes are reviewed in the second part of the review.
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http://dx.doi.org/10.3389/fchem.2019.00482DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6629787PMC
July 2019

Deposition of Aminomalononitrile-Based Films: Kinetics, Chemistry, and Morphology.

Langmuir 2019 07 17;35(30):9896-9903. Epub 2019 Jul 17.

Faculté de Chirurgie Dentaire , Université de Strasbourg , 8 Rue Sainte Elizabeth , 67000 Strasbourg , France.

In the last few years, the development of versatile coating chemistries has become a hot topic in surface science after the discovery that catecholamines can lead to conformal coatings upon oxidation from aqueous solutions. Recently, it was found that aminomalononitrile (AMN), a molecule implicated in the appearance of life on earth, is an excellent prototype of novel material-independent surface functionalizing agents leading to conformal and biocompatible coatings in a simple and direct chemical process from aqueous solutions. So far, very little insight has been gained regarding the mechanisms underlying coating deposition. In this paper, we show that the chemical evolution of AMN film deposition under slightly basic conditions is different in solution and on silica. Thereon, the coating proceeds via a nucleation process followed by further deposition of islands which evolve to produce nitrogen-rich superhydrophilic fibrillar structures. Additionally, we show that AMN-based material can form films at the air-solution interface from unshaken solutions. These results open new vistas into the chemistry of HCN-derived species of potential relevance in materials science.
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http://dx.doi.org/10.1021/acs.langmuir.9b01497DOI Listing
July 2019

Hexamethylenediamine-Mediated Polydopamine Film Deposition: Inhibition by Resorcinol as a Strategy for Mapping Quinone Targeting Mechanisms.

Front Chem 2019 5;7:407. Epub 2019 Jun 5.

Department of Chemical Sciences, University of Naples Federico II, Naples, Italy.

Hexamethylenediamine (HMDA) and other long chain aliphatic diamines can induce substrate-independent polymer film deposition from dopamine and several other catechols substrates at relatively low concentrations, however the mechanism of the diamine-promoted effect has remained little understood. Herein, we report data indicating that: (a) film deposition from 1 mM HMDA and dopamine is not affected by chemical oxidation with periodate but is markedly inhibited by resorcinol, which also prevents PDA film formation at 10 mM monomer concentration in the absence of HMDA; (b) N-acetylation of HMDA completely inhibits the effect on PDA film formation; (c) HMDA enables surface functionalization with 1 mM 5,6-dihydroxyindole (DHI) polymerization at pH 9.0 in a resorcinol-inhibitable manner. Structural investigation of the polymers produced from dopamine and DHI in the presence of HMDA using solid state C and N NMR and MALDI-MS suggested formation of covalent cross linked structures. It is concluded that HMDA enhances polydopamine adhesion by acting both on dopamine quinone and downstream, e.g., via covalent coupling with DHI. These results provide new insights into the mechanisms of PDA adhesion and disclose resorcinol as a new potent tool for targeting/mapping quinone intermediates and for controlling polymer growth.
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http://dx.doi.org/10.3389/fchem.2019.00407DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6560077PMC
June 2019

Enzymatically Active Polydopamine @ Alkaline Phosphatase Nanoparticles Produced by NaIO Oxidation of Dopamine.

Biomimetics (Basel) 2018 Nov 12;3(4). Epub 2018 Nov 12.

Institut National de la Santé et de la Recherche Médicale, Unité Mixte de Recherche 1121, 11 rue Humann, CEDEX, 67085 Strasbourg, France.

Polydopamine (PDA) deposition, obtained from the oxidation of dopamine and other catecholamines, is a universal way to coat all known materials with a conformal coating which can subsequently be functionalized at will. The structural analogies between polydopamine and eumelanin, the black-brown pigment of the skin, were incited to produce stable polydopamine nanoparticles in solution, instead of amorphous precipitates obtained from the oxidation of dopamine. Herein, we demonstrate that size-controlled and colloidally stable PDA-based nanoparticles can be obtained in acidic conditions, where spontaneous auto-oxidation of dopamine is suppressed, using sodium periodate as the oxidant and a protein, like alkaline phosphatase (ALP), as a templating agent. The size of the [email protected] nanoparticles depends on the dopamine/enzyme ratio and the obtained particles display enzymatic activity of alkaline phosphatase, with an activity extending up to two weeks after particle synthesis. The [email protected] nanoparticles can be engineered in polyelectrolyte multilayered films to potentially design model biosensors.
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http://dx.doi.org/10.3390/biomimetics3040036DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6352692PMC
November 2018

Ultra-slow diffusion of hexacyanoferrate anions in poly(diallyldimethyl ammonium chloride)-poly(acrylic acid sodium salt) multilayer films.

J Colloid Interface Sci 2019 Mar 19;539:306-314. Epub 2018 Dec 19.

Centre National de la Recherche Scientifique (CNRS). Laboratoire Interdisciplinaire des Environnements Continentaux (LIEC), UMR 7360, Vandoeuvre-lès-Nancy F54501, France; Université de Lorraine. LIEC, UMR 7360, Vandoeuvre-lès-Nancy F-54501, France.

Polyelectrolyte multilayer (PEM) films display either a linear or an exponential increase of their thickness with increasing the number of polycation/polyanion deposition cycles. Each of these growth regimes is further associated with a specific mode of internal PEM charge compensation: either intrinsic in the case of linearly growing films, or extrinsic for exponentially growing films with incorporation of small ions from the neighbouring electrolyte solution. In this report, we investigate by electrochemistry the charge compensation mechanism operational for poly(diallyldimethyl ammonium chloride)-poly(acrylic acid sodium salt) (PDAMAC-PAA) films recently found to be out-of-equilibrium immediately after the deposition process despite of their exponential growth mode. It is found here that these films are defined by a negative Donnan potential drop (ca. -160 mV), thus evidencing an extrinsic charge compensation process, and most importantly, by a remarkably slow kinetics for loading of hexacyanoferrate anions, a very unusual property for PEMs with exponential growth. Depending on the film thickness, the diffusion coefficient of the redox probe in the film is found to be of the order of 10 - 10 cm s, i.e. about 8 to 10 orders of magnitude less than that typically measured in aqueous solution. This results in a steady state filling of e.g. a 2.8 µm thick PEM film with the redox probe that is achieved after more than 40 h, a feature in line with the typical 4 to 5 days relaxation timescale of the film structure previously determined by atomic force microscopy and Raman micro-spectroscopy analyses.
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http://dx.doi.org/10.1016/j.jcis.2018.12.073DOI Listing
March 2019

Polydopamine/Transferrin Hybrid Nanoparticles for Targeted Cell-Killing.

Nanomaterials (Basel) 2018 Dec 17;8(12). Epub 2018 Dec 17.

Adolphe Merkle Institute, University of Fribourg, Chemin des Verdiers 4, 1700 Fribourg, Switzerland.

Polydopamine can form biocompatible particles that convert light into heat. Recently, a protocol has been optimized to synthesize polydopamine/protein hybrid nanoparticles that retain the biological function of proteins, and combine it with the stimuli-induced heat generation of polydopamine. We have utilized this novel system to form polydopamine particles, containing transferrin (PDA/Tf). Mouse melanoma cells, which strongly express the transferrin receptor, were exposed to PDA/Tf nanoparticles (NPs) and, subsequently, were irradiated with a UV laser. The cell death rate was monitored in real-time. When irradiated, the melanoma cells exposed to PDA/Tf NPs underwent apoptosis, faster than the control cells, pointing towards the ability of PDA/Tf to mediate UV-light-induced cell death. The system was also validated in an organotypic, 3D-printed tumor spheroid model, comprising mouse melanoma cells, and the exposure and subsequent irradiation with UV-light, yielded similar results to the 2D cell culture. The process of apoptosis was found to be targeted and mediated by the lysosomal membrane permeabilization. Therefore, the herein presented polydopamine/protein NPs constitute a versatile and stable system for cancer cell-targeting and photothermal apoptosis induction.
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http://dx.doi.org/10.3390/nano8121065DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6315732PMC
December 2018

Uniform trend in layer-by-layer deposition of heteropolytungstates.

J Colloid Interface Sci 2019 Jan 27;533:771-778. Epub 2018 Aug 27.

Jacobs University, Department of Life Sciences and Chemistry, Campus Ring 1, 28759 Bremen, Germany. Electronic address:

Hypothesis: The layer-by-layer deposition of films including polyoxometalates (POMs) results in a very interesting range of applications in various fields such as electrochemical devices and as photochromic coatings. However, the fundamental knowledge of the parameters responsible for tuning the properties of the film (i.e. relation between the structure and composition of the POM and the properties of the final film) is still lacking.

Experiments: The current work establishes the relationship between the film thickness, the quantity of POM incorporated in each layer and the electrochemical response of the (PAH-POM) coatings, where PAH is poly(allylamine hydrochloride).

Findings: The results presented in this work show that the film thickness, composition and electrochemical activity scale proportionally with the number of W atoms in a series of heteropolytungstates ranging from 5 to 48 (PW, PW, PVW, PW, PW, PW). The obtained results allow us to establish a method to predict the behavior as well as the properties of the film based on the nature of the POM used.
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http://dx.doi.org/10.1016/j.jcis.2018.08.085DOI Listing
January 2019

Polydopamine Nanomaterials: Recent Advances in Synthesis Methods and Applications.

Authors:
Vincent Ball

Front Bioeng Biotechnol 2018 17;6:109. Epub 2018 Aug 17.

Faculté de Chirurgie Dentaire, Université de Strasbourg, Strasbourg, France.

Polydopamine (PDA), the final oxidation product of dopamine or other catecholamines, attracted much attention as versatile coatings that can be used to cover the surface of almost all materials with a conformal layer of adjustable thickness ranging from a few to about 100 nm. These PDA layers can be subsequently modified with molecules carrying nucleophilic groups or with metallic nanoparticles from solutions containing metallic cations. However, during the deposition of PDA film on the surfaces, the reaction products that are simultaneously obtained from the oxidation of catecholamines in solution precipitate. Hence, some recent effort has been devoted to produce PDA in the form of nanoparticles. The aim of this short review is to give a comprehensive description of the synthesis methods yielding of PDA nanoparticles in the absence or in the presence of templating agents (polymers, polyelectrolytes, surfactants, proteins, and even some small organic molecules). We will also describe the use of thin PDA layers to coat already synthesized nanoparticles or nanotubes. Finally, several first applications of the obtained PDA nanoparticles will be described.
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http://dx.doi.org/10.3389/fbioe.2018.00109DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6108306PMC
August 2018

Mimicking the Chemistry of Natural Eumelanin Synthesis: The KE Sequence in Polypeptides and in Proteins Allows for a Specific Control of Nanosized Functional Polydopamine Formation.

Biomacromolecules 2018 09 15;19(9):3693-3704. Epub 2018 Aug 15.

Université de Strasbourg , Faculté de Chirurgie Dentaire , 8 rue Sainte Elisabeth , 67000 Strasbourg France.

The oxidation of dopamine and of other catecholamines leads to the formation of conformal films on the surface of all known materials and to the formation of a precipitate in solution. In some cases, it has been shown that the addition of additives in the dopamine solution, like certain surfactants or polymers, polyelectrolytes, and certain proteins, allows to get polydopamine nanoparticles of controlled size and the concomitant decrease, in an additive/dopamine dependent manner, in film formation on the surface of the reaction beaker. However, the mechanism behind this controlled oxidation and self-assembly of catecholamines is not known. In this article, it is shown that a specific diad of amino acids in proteins, namely KE, allows for specific control in the oxidation-self-assembly of dopamine to obtain [email protected] core-shell nanoparticles which are biocompatible. The interactions between dopamine and the adjacent KE amino acids potentially responsible for the size control of polydopamine aggregates was investigated by molecular dynamics simulations. The obtained core-shell nanoparticles display the biological activity of the protein used to control the self-assembly of PDA. The photon to heat conversion ability of PDA is conserved in the [email protected] particles.
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http://dx.doi.org/10.1021/acs.biomac.8b00818DOI Listing
September 2018

Polyphenols at interfaces.

Adv Colloid Interface Sci 2018 Jul 7;257:31-41. Epub 2018 Jun 7.

Université de Strasbourg, INSERM, UMR_S 1121 Biomatériaux et bioingénierie, FMTS, 11 rue Humann, 67085 Strasbourg, Cedex, France.

Polyphenols are important molecules in living organisms, particularly in plants, where they serve as protectants against predators. They are also of fundamental importance in pharmacology for their antioxidant and antibacterial activities. Since a few years polyphenols are also used in surface functionalization mimicking the tannin deposition observed when tea or red wine are in contact with the surface of cups or glasses respectively. The interaction of polyphenols with proteins to yield colloids and of polyphenol with surfaces will be reviewed in this article to provide an overview of such particles and surface functionalization methods in modern surface science. Particular emphasis will be given to biological applications of polyphenols at interfaces.
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http://dx.doi.org/10.1016/j.cis.2018.06.001DOI Listing
July 2018

Polymer-free electrospinning of tannic acid and cross-linking in water for hybrid supramolecular nanofibres.

Nanoscale 2018 May;10(19):9164-9173

Institut National de la Santé et de la Recherche Médicale, Unité mixte de Recherche 1121, 11 rue Humann, 67085 Strasbourg Cedex, France.

Electrospinning is the process of choice allowing the preparation of nanofibrous materials from a solution usually based on a high molar mass polymer. The solution must bring enough chain entanglements to avoid any breaking or Rayleigh instability of the electrospun jet resulting thus in the deposition of a continuous and regular solid nanofibre. It has been however shown that some few non-polymeric molecules can be electrospun without using a carrier polymer. We demonstrate here the case of tannic acid. Indeed, it was possible to electrospin this molecule solubilised in a mixture of water and ethanol as well as in pure water. Rheology, dynamic light scattering and cryo-TEM highlight the formation of tannic acid aggregates in solution. Above a critical concentration, these aggregates form a supramolecular interconnected network strong enough to allow the electrospinning of a continuous and regular nanofibre. The resulting nanoweb is mechanically stable and can be handled and wrapped. Furthermore, as opposed to the other small molecules for which polymer-free electrospinning was also demonstrated, tannic acid nanowebs can be efficiently cross-linked in water either by oxidative reaction with sodium periodate or, most interestingly, with FeIII by a combination of oxidative reaction and the formation of coordination complexes. The proposed electrospinning and cross-linking strategy is easy, of low cost, and scalable and uses non-toxic solvents as well as biocompatible and biofunctional molecules. Furthermore, thanks to the chelation capacity of tannic acid having the ability to coordinate with a wide variety of metals, hybrid smart nanowebs can be envisaged for diverse applications such as biomedical, catalysis as well as environment.
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http://dx.doi.org/10.1039/c8nr01067fDOI Listing
May 2018

Multilayered films made from tannic acid and alkaline phosphatasewith enzymatic activity and electrochemical behavior.

J Colloid Interface Sci 2018 Feb 27;512:722-729. Epub 2017 Oct 27.

Institut National de la Santé et de la Recherche Médicale, Unité mixte de recherche 1121, Faculté de Médecine, 11 rue Humann, 67085 Strasbourg, France; Université de Strasbourg, Faculté de Chirurgie Dentaire, 8 rue Sainte Elisabeth, 67000 Strasbourg, France. Electronic address:

Layer-by-layer-deposition of enzymes and polyphenols, like tannic acid may provide a reservoir of antioxidant and antibacterial molecules of controlled thickness and degradability with an additional activity due to the presence of the enzyme. The layer-by-layer deposition of films made from tannic acid and alkaline phosphatase is shown to yield an exponential growth with the number of deposited layer pairs. The films display the electrochemical behavior of tannic acid and the enzymatic activity of alkaline phosphatase. However, it is shown that only the enzyme close to the film-solution interface is active and follows the Michaelis-Menten mechanism. Similarly, only tannic acid close to the electrode-film interface can be oxidized. The enzymatic activity is almost completely lost when the multilayer film is treated with sodium periodate which oxidizes tannic acid even if the solubilized enzyme is not affected by the oxidant. This shows that the formation of covalent bonds between alkaline phosphatase and tannic acid is deleterious for its conformation and activity.
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http://dx.doi.org/10.1016/j.jcis.2017.10.101DOI Listing
February 2018

Structural Basis of Polydopamine Film Formation: Probing 5,6-Dihydroxyindole-Based Eumelanin Type Units and the Porphyrin Issue.

ACS Appl Mater Interfaces 2018 Mar 29;10(9):7670-7680. Epub 2017 Sep 29.

Université de Strasbourg , Faculté de Chirurgie Dentaire , 8 rue Sainte Elisabeth , 67000 Strasbourg , France.

The role of 5,6-dihydroxyindole (DHI)-based oligomers, including porphyrin-like tetramers, in polydopamine (PDA) film formation was addressed by a comparative structural investigation against model polymers from DHI and its 2,7'-dimer. MALDI-MS data showed that (a) PDA is structurally different from DHI melanin and does not contain species compatible with DHI-based oligomers as primary building blocks; (b) PDA films and precipitate display a single main peak at m/ z 402 in common; (c) no species matching the range of m/ z values expected for cyclic porphyrin-type tetramers was detected in DHI melanin produced in the presence or in the absence of folic acid (FA) as templating agent, nor by oxidation of the 2,7'-dimer of DHI as putative precursor. N NMR resonances and Raman spectra predicted by extensive DFT calculations on porphyrin-type structures at various oxidation levels did not match spectral data for PDA or DHI melanin. Notably, unlike PDA, which gave structurally homogeneous films on quartz on atomic force microscopy (AFM) and micro-Raman spectroscopy, DHI melanin did not form any adhesive deposit after as long as 24 h. It is concluded that PDA film deposition involves structural components unrelated to DHI-based oligomers or porphyrin-type tetramers, which, on mechanism-based analysis, may arise by quinone-amine conjugation leading to polycyclic systems with extensive chain breakdown.
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http://dx.doi.org/10.1021/acsami.7b09662DOI Listing
March 2018

Boric Acid as an Efficient Agent for the Control of Polydopamine Self-Assembly and Surface Properties.

ACS Appl Mater Interfaces 2018 Mar 15;10(9):7574-7580. Epub 2017 Sep 15.

Institut National de la Santé et de la Recherche Médicale, Unité Mixte de Recherche 1121 , 11 rue Humann , 67085 Strasbourg Cedex , France.

The deposition of polydopamine (PDA) films on surfaces, a versatile deposition method with respect to the nature of the used substrate, is unfortunately accompanied by deposition of insoluble precipitates in solution after a prolonged oxidation time of dopamine solutions. Therefore, there is evident interest to find methods able to stop the deposition of PDA on surfaces and to simultaneously control the self-assembly of PDA in solution to get stable colloidal aggregates. In addition to proposed methods relying on the use of polymers like poly(vinyl alcohol) and proteins like human serum albumin, we show herein that boric acid is an efficient adjuvant that is simultaneously able to stop the self-assembly of PDA in solution as well as on surfaces and to change the adhesive properties of the resulting PDA coatings.
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http://dx.doi.org/10.1021/acsami.7b08356DOI Listing
March 2018

Composite Materials and Films Based on Melanins, Polydopamine, and Other Catecholamine-Based Materials.

Authors:
Vincent Ball

Biomimetics (Basel) 2017 Jul 6;2(3). Epub 2017 Jul 6.

Faculté de Chirurgie Dentaire, Université de Strasbourg, 8 rue Sainte Elisabeth, 67000 Strasbourg, France.

Polydopamine (PDA) is related to eumelanins in its composition and structure. These pigments allow the design, inspired by natural materials, of composite nanoparticles and films for applications in the field of energy conversion and the design of biomaterials. This short review summarizes the main advances in the design of PDA-based composites with inorganic and organic materials.
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http://dx.doi.org/10.3390/biomimetics2030012DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6352683PMC
July 2017

Polydopamine Coating To Stabilize a Free-Standing Lipid Bilayer for Channel Sensing.

Langmuir 2017 07 11;33(29):7256-7262. Epub 2017 Jul 11.

Jacobs University Bremen , Campus Ring 1, D-28759 Bremen, Germany.

An appropriate method to study the function of membrane channels is to insert them into free-standing lipid bilayers and to record the ion conductance across the membrane. The insulating property of a free-standing lipid bilayer versus the single-channel conductivity provides sufficient sensitivity to detect minor changes in the pathway of ions along the channel. A potential application is to use membrane channels as label-free sensors for molecules, with DNA sequencing as its most prominent application. However, the inherent instability of free-standing bilayers limits broader use as a biosensor. Here we report on a possible stabilization of free-standing lipid bilayers using polydopamine deposition from dopamine-containing solutions in the presence of an oxidant. This stabilization treatment can be initiated after protein reconstitution and is compatible with most reconstitution protocols.
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http://dx.doi.org/10.1021/acs.langmuir.7b01959DOI Listing
July 2017