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Organic-Inorganic Hybrid Planarization and Water Vapor Barrier Coatings on Cellulose Nanofibrils Substrates.

ABSTRACT: Cellulose nanofibrils (CNF) can be produced in the form of thin, transparent and flexible films. However, the permeability of such materials to oxygen and water vapor is very sensitive to moisture, which limits their potential for a variety of packaging and encapsulation applications. Diffusion barrier coatings were thus developed to reduce the access of water molecules to enzymatically pre-treated and carboxymethylated CNF substrates. The coatings were based on UV curable organic-inorganic hybrids with epoxy, tetraethylorthosilicate (TEOS) and 3-glycidoxypropyltrimethylenesilane (GPTS) precursors and additional vapor formed SiN_x layers. A total of 14 monolayer and multilayer coatings with various thickness and hybrid composition were produced and analyzed. The water vapor transmission rate (WVTR) of the bilayer epoxy/CNF film was two times lower compared to that of uncoated CNF film. This was partly due to the water vapor permeability of the epoxy, a factor of two times lower than CNF. The epoxy coating improved the transparency of CNF, however it did not properly wet to the CNF surfaces and the interfacial adhesion was low. In contrast hybrid epoxy-silica coatings led to high adhesion levels owing to the formation of covalent interactions through condensation reactions with the OH-terminated CNF surface. The barrier and optical performance of hybrid coated CNF substrates was similar to that of CNF coated with pure epoxy. In addition, the hybrid coatings provided an excellent planarization effect, with roughness close to 1 nm, one to two orders of magnitude lower than that of the CNF substrates. The WVTR and oxygen transmission rate values of the hybrid coated CNF laminates were in the range 5-10 g/m²/day (at 38°C and 50% RH) and 3-6 cm³/m²/day/bar (at 23°C and 70% RH), respectively, which matches food and pharmaceutical packaging requirements. The permeability to water vapor of the hybrid coatings was moreover found to decrease with increasing the TEOS/GPTS ratio up to 30 wt% and then increase at higher ratio, and to be much lower for thinner coatings due to further UV-induced silanol condensation and faster evaporation of byproducts. The addition of a single 150 nm thick SiN_x layer on the hybrid coated CNF improved its water vapor barrier performance by more than 680 times, with WVTR below the 0.02 g/m²/day detection limit.

SUBMITTER: Karasu F

PROVIDER: S-EPMC6262297 | biostudies-literature | 2018

REPOSITORIES: biostudies-literature

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Organic-Inorganic Hybrid Planarization and Water Vapor Barrier Coatings on Cellulose Nanofibrils Substrates.

Karasu Feyza F Müller Luca L Ridaoui Hassan H Ibn ElHaj Mohammed M Flodberg Göran G Aulin Christian C Axrup Lars L Leterrier Yves Y

Frontiers in chemistry 20181121

Cellulose nanofibrils (CNF) can be produced in the form of thin, transparent and flexible films. However, the permeability of such materials to oxygen and water vapor is very sensitive to moisture, which limits their potential for a variety of packaging and encapsulation applications. Diffusion barrier coatings were thus developed to reduce the access of water molecules to enzymatically pre-treated and carboxymethylated CNF substrates. The coatings were based on UV curable organic-inorganic hybr ...[more]

PMID: 30525026

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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

Organic-Inorganic Hybrid Planarization and Water Vapor Barrier Coatings on Cellulose Nanofibrils Substrates.

Publications

Organic-Inorganic Hybrid Planarization and Water Vapor Barrier Coatings on Cellulose Nanofibrils Substrates.

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