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Silicate-Phenolic Networks: Coordination-Mediated Deposition of Bioinspired Tannic Acid Coatings.

ABSTRACT: Surface modification with polyphenolic molecules has been pursued in biomedical materials owing to their antioxidant, anti-inflammatory, and antimicrobial characteristics. Recently, the use of silicic acid (Si_aq ) as a mediator for efficient surface deposition of tannic acid (TA) was reported, but the postulated Si-TA polymeric networks were not characterized. Herein, we present unambiguous evidence for silicate-TA networks that involve Si-O-C motifs by using solid-state NMR spectroscopy, further supported by XPS and ToF-SIMS. By using QCM-D we demonstrate the advantages of Si_aq , compared to using transition-metal ions, to improve the coating efficiency under mildly acidic conditions. The presented homogenous coating buildup and validated applicability in inorganic buffers broadens the use of TA for surface modifications in technological and biomedical applications.

SUBMITTER: Weber F

PROVIDER: S-EPMC6772174 | biostudies-literature | 2019 Jul

REPOSITORIES: biostudies-literature

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Silicate-Phenolic Networks: Coordination-Mediated Deposition of Bioinspired Tannic Acid Coatings.

Weber Florian F Liao Wei-Chih WC Barrantes Alejandro A Edén Mattias M Tiainen Hanna H

Chemistry (Weinheim an der Bergstrasse, Germany) 20190701 42

Surface modification with polyphenolic molecules has been pursued in biomedical materials owing to their antioxidant, anti-inflammatory, and antimicrobial characteristics. Recently, the use of silicic acid (Si<sub>aq</sub> ) as a mediator for efficient surface deposition of tannic acid (TA) was reported, but the postulated Si-TA polymeric networks were not characterized. Herein, we present unambiguous evidence for silicate-TA networks that involve Si-O-C motifs by using solid-state NMR spectrosc ...[more]

PMID: 31132189

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Project description:Infection is the major cause of morbidity after breast implant surgery. Biodegradable medical-grade polycaprolactone (mPCL) scaffolds designed and rooted in evidence-based research offer a promising alternative to overcome the limitations of routinely used silicone implants for breast reconstruction. Nevertheless, as with any implant, biodegradable scaffolds are susceptible to bacterial infection too, especially as bacteria can rapidly colonize the biomaterial surface and form biofilms. Biofilm-related infections are notoriously challenging to treat and can lead to chronic infection and persisting inflammation of surrounding tissue. To date, no clinical solution that allows to efficiently prevent bacterial infection while promoting correct implant integration, has been developed. In this study, we demonstrated for the first time, to our knowledge that the physical immobilization of 1 and 5% human serum albumin (HSA) onto the surface of 3D printed macro- and microporous mPCL scaffolds, resulted in a reduction of Staphylococcus aureus colonization by 71.7 ± 13.6% and 54.3 ± 12.8%, respectively. Notably, when treatment of scaffolds with HSA was followed by tannic acid (TA) crosslinking/stabilization, uniform and stable coatings with improved antibacterial activity were obtained. The HSA/TA-coated scaffolds were shown to be stable when incubated at physiological conditions in cell culture media for 7 days. Moreover, they were capable of inhibiting the growth of S. aureus and Pseudomonas aeruginosa, two most commonly found bacteria in breast implant infections. Most importantly, 1%HSA/10%TA- and 5%HSA/1%TA-coated scaffolds were able to reduce S. aureus colonization on the mPCL surface, by 99.8 ± 0.1% and 98.8 ± 0.6%, respectively, in comparison to the non-coated control specimens. This system offers a new biomaterial strategy to effectively translate the prevention of biofilm-related infections on implant surfaces without relying on the use of prophylactic antibiotic treatment.

Project description:The purpose of this study was to comparatively investigate the behavior of silicate and sol-silicate coatings non-modified or modified with an organosilane on wood and on wood pre-coated with silica-mineralized primers. Adhesion strength, morphology, and water permeability and related damages were studied to evaluate the possibility of utilizing such inorganic-based coating systems for durable protection of wood without or with relatively cheap and water-borne primers. Potassium silicate and potassium methylsiliconate aqueous solutions and a colloidal silica were used for the preparation of the coatings. The white coating paints were brushed on beech wood substrates at a rate of 220 g·m-2. The coatings exhibited good coverage ability. The pull-off adhesion strength values appeared to be related to pH following a polynomial law. The adhesion strength for the silicate coatings were adequate (above 3 MPa and up to 5 MPa) for wood, whereas the values for the sol-silicates were too low for practical applications. The adhesion values were in general higher for the samples cured in a climate room (23 ± 3 °C and 75 ± 2% relative humidity) than the samples cured in the ambient atmosphere of the laboratory (23 ± 3 °C and 25 ± 5% relative humidity). The presence of microdefects (cracks, holes) was revealed in the coating layers by optical and scanning electron microscopy. The surface roughness parameters assessed by confocal scanning laser microscopy were dependent on the magnification applied for their measurement. The arithmetic average roughness Sa was between 5 µm and 10 µm at magnification 5× and between 2.5 μm and 10 µm at magnification 20×. The maximum peak-to-valley height Sz confirmed the presence of open pores emerging through the coatings. The open pores constitute free pathways for water ingress through the coatings, and could explain the high water absorption of the coatings including the methysiliconate-containing silicate coating and despite the relatively high water contact angle and low wettability exhibited by this sample. The post-application of a hydrophobizing solution containing hexadecyltrimethoxysilane and dimethyloctadecyl[3-(trimethoxysilyl)propyl]ammonium chloride considerably reduced the water permeability, while application of nanosilica-containing organic primers increased the adhesion for the coatings. Silicate coatings with adhesion great enough and resistance against water damages can be generated on wood even without a primer using low silica-to-alkali ratio binders and an organosilane additive. The sol-silicate coatings appear to be applicable only with a primer. The improvement of the paint formulations to control the formation of microcracks and open pores could be useful to reduce the liquid water permeability and increase durability. Otherwise, the application of a hydrophobizing treatment can be used for this purpose.

Dataset Information

Silicate-Phenolic Networks: Coordination-Mediated Deposition of Bioinspired Tannic Acid Coatings.

Publications

Silicate-Phenolic Networks: Coordination-Mediated Deposition of Bioinspired Tannic Acid Coatings.

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