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Cellulose nanofibril-based coatings of woven cotton fabrics for improved inkjet printing with a potential in e-textile manufacturing Oleksandr Nechyporchuk, Junchun Yu, Vincent A. Nierstrasz, and Romain Bordes ACS Sustainable Chem. Eng., Just Accepted Manuscript • Publication Date (Web): 05 May 2017 Downloaded from http://pubs.acs.org on May 6, 2017

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Cellulose nanofibril-based coatings of woven cotton

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fabrics for improved inkjet printing with a potential

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in e-textile manufacturing

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Oleksandr Nechyporchuk,*,† Junchun Yu,§ Vincent Nierstrasz,§ Romain Bordes*,†

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Textile Materials Technology, Department of Textile Technology, Faculty of Textiles, Engineering and Business, University of Borås, SE-501 90 Borås, Sweden

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* Corresponding authors. E-mails: [email protected]; [email protected].

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Abstract: The roughness of woven fabrics strongly limits print quality, which is particularly critical in

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printing of conductive circuits on fabrics. This work demonstrates the use of wood-derived cellulose nanofibrils

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Keywords: cellulose nanofibrils, nanofibrillated cellulose, nanocellulose, fabric coating,

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inkjet printing, smart textiles, electronic textiles (e-textiles)

Department of Chemistry and Chemical Engineering, Applied Surface Chemistry, Chalmers University of Technology, SE-412 96 Gothenburg, Sweden

(CNFs) mixed with a plasticizer as coatings of woven cotton fabrics for inkjet printing using: (i) conventional color water-based pigment inks and (ii) conductive silver nanoparticle inks. CNFs, being similar in nature to cotton, introduced minimal alteration to woven cotton fabrics by preserving their visual appearance as well as their mechanical properties. We also showed that the use of CNF-based coatings facilitated ink droplet settling on the substrate, which ensured high quality with the potential of higher printing speed production. The coatings of CNFs plasticized with glycerol enabled concentrating the pigment on the surface of the fabric, preventing its penetration into the fabric depth, which allows increasing the resolution of the printed pattern. When used for color ink printing, it enhanced the print chroma and permitted to reduce the amount of deposited ink, yielding similar color lightness. The CNF coatings allowed to reduce substantially the amount of silver ink when printing the conductive tracks on fabrics. Furthermore, the nature of the coating imparts flexibility to the conductive layer, while maintaining electric signal quality, even when folded. This study provides a platform for manufacturing green disposable e-textiles.

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Introduction

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The development of electronic devices integrated into fabrics, known as electronic textiles

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(e-textiles) or, more generally, smart textiles, is a subject of increasing interest. Such products

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aim at offering advanced functionalities to the conventional textiles, while keeping such

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features as flexibility, foldability and lightweight. The e-textiles include wearable displays,

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light emitting diodes (LEDs), electromechanical actuators, power storage devices etc.1–3 The

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introduction of conductive elements into woven fabrics is not trivial. It is usually performed

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by weaving or knitting the conductive filaments (fibers, yarns or threads) into the textile

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structure.3 Such approach, however, lacks process flexibility and is limited in terms of

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conductive circuit design. Printing techniques that allow the conductive paths to be deposited

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on the fabric surfaces offer broader opportunities, more in line with the requirements of

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developing complex circuitry.

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Rotary and flatbed screen printing have been by far the most common technologies for

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printing on fabrics. However, due to a global trend of shortening of average run lengths and

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increase of speed of inkjet printheads, inkjet technology is becoming more attractive lately.4

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Inkjet printing allows printing on demand and gives opportunities of maskless and non-

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contact printing. Such features makes inkjet a promising platform for development of

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innovative smart textiles, while being well aligned with the economic constraints of small

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volume production. Another aspect where inkjet is becoming more attractive is textile dyeing

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(bulk coloring). In comparison with conventional deying techniques, inkjet has a lower

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environmental footprint.5 It also offers higher flexibility compared to novel methods of

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waterless dyeing using supercritical carbon dioxide.6

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In terms of electronic textile production, screen printing is appropriate for the deposition of

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relatively thick conductive layers using paste-like inks, which remain on the surface of fabric

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due to high ink viscosity.7 In comparison, the low-viscosity inks used in inkjet printing are

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much easier to penetrate into the fabric depth and the thickness of the deposited ink layer is

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much lower compared to that achieved by screen printing. This generates difficulties in

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achieving good conductivity of the printed path and the high fabric roughness becomes one of

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the main challenges for the print quality.8 The sufficient ink thickness can be thus achieved by

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multiple passes in the inkjet printer. Roughness reduction together with control of ink

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penetration to the fabric bulk are thus essential for the implementation of such technologies,

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since they can reduce the amount of deposited conductive inks, which are generally

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expensive. 2 ACS Paragon Plus Environment

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Recently, cellulose nanofibrils (CNFs) have gained an increasing interest for use in printed

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electronics as substrates or as constituents in functional conductive ink formulations.9 CNFs is

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a bio-based and biocompatible nanomaterial produced by disintegration of cellulosic fibers

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that are traditionally used in papermaking, textile and other industries. CNFs are potentially a

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low-cost material,10 generally having a diameter of 3–50 nm and a length of few micrometers,

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and are composed of alternating crystalline (ordered) and less crystalline (disordered)

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regions.11 Manufacturing of CNFs is generally performed by mechanical disintegration of

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microscopic cellulose fibers with preliminary enzymatic hydrolysis (e.g., using

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endoglucanase) or chemical surface modification (e.g., carboxylation, carboxymethylation or

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quaternization) that are used to facilitate the individualization of nanofibrils.11

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CNFs have been widely reported previously as paper strength-enhancing additive or

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coating,12–14 filler in composite materials,15–17 rheology modifiers,18,19 emulsion

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stabilizers,20,21 freestanding films,22–25 aerogels26–28 and hydrogels29,30. In addition to the

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above applications, CNFs were used as substrates for printed electronics.31–35 Chinga-

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Carrasco et al.31 reported the use of various grades of CNFs as film substrates for printed

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conductive circuits manufactured by inkjet printing of silver inks. CNFs produced by

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mechanical disintegration without chemical surface modification or with carboxylation or

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carboxymethylation pretreatments were examined. It was shown that the highest print

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resolution was achieved for chemically pretreated CNFs, owing to the lower surface

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roughness of the films. Moreover, higher print resolution was achieved by reducing the

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wettability of the film surfaces through grafting with hexamethyldisilazane.31

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Hseigh et al.32 demonstrated the advantageous use of CNF nanopapers compared to

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conventional pulp papers for fabrication of conductive circuits by gold sputtering or inkjet

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printing using silver nanoparticle inks or particle-free metallo-organic decomposition (MOD)

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silver inks. They reported a drastic decrease of electrical resistance (from 6340 Ω to 34 Ω for

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gold sputtering) for equally deposited circuits on nanopapers compared to those for traditional

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papers. This was attributed to the ability of CNFs to produce smooth and low porous surfaces.

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Composites of CNFs and inorganic filler particles36,37 or acrylic resins/CNFs38 were also

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proposed as substrates for flexible electronic devices.

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The aforementioned suggests that CNFs may be suitable to modify the surface of fabrics

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that may be subsequently used as substrates for printed electronics. The use of CNFs as

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coatings in woven fabrics has not been extensively studied yet. Some works describe the use

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of such coatings to improve print quality of non-woven and woven synthetic fiber sheets39,40

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and recently woven cotton fabrics.40 However, the influence of the CNF coatings on pigment 3 ACS Paragon Plus Environment

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penetration into the fabric bulk still requires investigation. Compared to various elastomer

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coatings widely used for fabrics, development of all-cellulose product applying wood-derived

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CNFs on cotton fabric appears very attractive.

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In this work, we aim at exploring the potential of wood-derived CNFs as a base coating for

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textile, focusing on improving the inkjet printing process with a potential in e-textile

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manufacturing. The CNF film-forming properties on woven cotton fabrics are examined and

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the influence of plasticized CNF coatings with different basis weight, as well as printing with

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various ink droplet volume, on the printed layer properties are investigated. Color water-based

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pigment ink is first assessed as a proof of concept that CNF networks control the pigment

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penetration to the depth of fabric. Then, conductive silver nanoparticle ink is tested to produce

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printed circuits on fabrics coated with CNFs and a plasticizer with the objective of enhancing

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the conductivity of the printed paths. The flexibility and foldability of the produced e-textile is

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also evaluated.

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Materials

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Unbleached cotton fabric with 2/1 twill weave, an basis weight of (112 ± 1) g/m2 and a

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thickness of 0.22 mm (determined according to ASTM D1777 – 96) was kindly provided by

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Eton Fashion AB (Sweden). Glycerol (≥99.5%) and hydrochloric acid (37%) were purchased

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from Sigma-Aldrich Sweden AB.

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Nanocellulose. CNFs in the form of aqueous suspension with solids content of 3.3 wt%

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were kindly provided by Stora Enso AB (Sweden). The CNFs were produced by means of

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mechanical fibrillation of softwood pulp (ca. 75% of pine and 25% of spruce, containing 85%

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of cellulose, 15% of hemicellulose and traces of lignin, as determined by the supplier) and had

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an average nanofibril diameter of 7 ± 3 nm and a length of ca. 1 µm, as determined from

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height profiles of atomic force microscopy images (see Fig. S1 in the Supporting

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Information). It had a charge density of (20.7 ± 0.6) µeq/g at pH 5.2 (measured using a

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particle charge detector PCD-02 (Mütek Analytic GmbH, Germany) titrated using

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polydiallyldimethylammonium chloride).

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Inks. Water-based cyan pigment ink (VelvetJet) was provided by Bordeaux Digital

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PrintInk Ltd. (USA). It had the solids content of ca. 30 wt%, the viscosity of 10.5 mPa s at the

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shear rate of 10,000 s−1 and the temperature of 35 °C and the surface tension of

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31.1 ± 1.2 mN/m at 25 °C. The pigment average particle size was determined as 110 nm at

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90° by means of dynamic light scattering using N4 Plus Submicron Particle Size Analyzer

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(Beckman Coulter, USA). Epson T2631 photo black ink cartridge was purchased from Seiko 4 ACS Paragon Plus Environment

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Epson Corporation (Japan). Water-based silver nanoparticle ink (NBSIJ-MU01) was

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purchased from Mitsubishi Paper GmbH (Germany). The ink had the silver content of

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15 wt%, the viscosity of 2.30 ± 0.50 mPa s at 25 °C and the surface tension of 31.0 ±

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3.0 mN/m, as reported by the supplier.

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Methods

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Fabric coating. The initial CNF suspension was diluted with deionized water to 1 wt%

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and 100 g of the suspension was homogenized using Heidolph DIAX 900 (Heidolph

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Instruments, Germany) equipped with 10 F shaft at power 2 (11,600 rpm). The formulation

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containing a plasticizer was prepared in a similar way by adding glycerol to CNFs to reach

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1/10 wt/wt ratio prior to the homogenization. Coating of woven cotton fabrics was performed

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via spraying of the above formulation using Cotech Airbrush Compressor AS18B (Clas

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Ohlson AB, Sweden) at a pressure of 3 bar. The coatings were deposited in 2, 4 or 6 runs with

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an intervals of 20 min. The samples were dried under fume hood at ambient temperature (ca.

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20 °C). As a result, an increase of basis weight by 8.1, 13.4 and 20.4 g/m2 was obtained for

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the fabric coated with CNFs and glycerol, as measured by gravimetry.

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Inkjet printing with cyan ink. Printing on fabrics uncoated or coated with CNFs/glycerol

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was performed using a custom-made inkjet printer Urtidium B200 (VdW-Consulting bvba,

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Belgium) equipped with a piezoelectric printhead Konica Minolta KM1024i, allowing the

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print resolution of 360 dpi. The ink was passed through a nylon syringe filter of 0.45 µm

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before feeding the printhead. Fabric specimens were printed by varying the ink volume per

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droplet ejected from a single nozzle, viz. 49, 101 and 145 pL. The printed substrate was

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subsequently cured in the oven at 150 °C for 5 min.

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Inkjet printing with silver nanoparticle ink. Uncoated and coated fabrics were printed

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with conductive silver nanoparticle ink using Epson Expression Premium XP-600 inkjet

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printer (Seiko Epson Corporation, Japan). The original Epson cartridges were replaced with

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compatible ones filled with the conductive inks through a nylon filter of 5 µm. The fabric

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samples were mounted on the CD tray for printing. Each fabric sample was processed by 3

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printing cycles. Before printing, the fabric was sprayed with 0.05 M HCl, which was

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necessary to disrupt the silver nanoparticle stabilizing agent and to achieve the required

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conductivity of the printed circuit, without thermal sintering step.

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Printing of resolution test chart. An Epson Expression Premium XP-600 inkjet printer (Seiko Epson Corporation, Japan) was used to print the resolution test chart on uncoated and

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coated fabrics using Epson T2631 photo black ink. The chart was designed with 1.2–5.2 line

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pairs per mm, where one line pair contained one printed line and one blank line.

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Scanning electron microscopy (SEM). Fabric specimens were examined using LEO Ultra

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55 field emission gun (FEG) SEM (Carl Zeiss, Germany), operating at an acceleration voltage

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of 2–3 kV. The specimens were glued on stubs using carbon tape and were coated at the edges

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with PELCO conductive liquid silver paint to improve the conductivity and finally were

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sputtered with Au layer of ca. 10 nm. Cross-sections of the specimens were prepared by

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cutting the fabric with a fresh razor blade stroke with a hammer.

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Optical microscopy. Optical microscopy images of the fabric cross sections and top

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surfaces were taken using Zeiss Axio Scope.A1 (Carl Zeiss, Germany) microscope equipped

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with Zeiss AxioCam MRc5 digital camera. ZEN 2012 acquisition software was used for

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image processing.

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Atomic force microscopy (AFM). The AFM was performed in a tapping mode using

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NTEGRA Prima equipped with NSG01 cantilever (NT-MDT, Russia) to examine the

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morphology of CNFs. The CNF suspensions were diluted to the concentration of 10−2 wt.%,

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and a droplet was placed on a freshly polished silicon wafer substrate and dried. The AFM

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height images were then processed in Gwyddion software.

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Colorimetry. Color coordinates of the prints were measured in the CIE L*a*b* color

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space by Datacolor Check II spectrophotometer (Datacolor, USA). The measurements were

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performed using D65 light source at 10° observer. Data processing was performed using the

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Datacolor TOOLS 2.1 software. The color coordinates were characterized by the values of: L*

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representing the lightness, which varies from 100 (white) to 0 (black), a* and b* representing

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the chromatic components, where +a* is the red, −a* is the green, +b* is the yellow, −b* is

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the blue directions and 0 value for both a* and b* represents a grayscale. The components a*

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and b* can be expressed by a single chroma parameter C* determined as [(a*)2+(b*)2]1/2.

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Tensile testing. Mechanical testing was performed according to ASTM D5034 – 09 (2013)

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method. Instron 5565A (Norwood, MA, USA) equipped with a static load cell of 5 kN and

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pneumatic clamps with a pressure of 5 bar was used for the measurements. Data processing

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was performed using the Bluehill software. Rectangular specimens with a length of 150 mm

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and a width of 20 mm were cut parallel to warp direction along the threads. The specimens

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were conditioned at least 12 h before the measurements at a temperature of 23 °C and a

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relative humidity of 60%. Each specimen was fixed in the clamps around steel pins to avoid

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the slippage. The measurements were performed at a constant extension rate of 300 mm/min

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at the gauge length of 20 mm. Seven measurements were performed for each sample and the 6 ACS Paragon Plus Environment

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average values were calculated. The terms related to the force and deformation properties

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were used as determined by ASTM D4848 – 98 (2012). The Young’s modulus values were

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determined from the linear viscoelastic region after passing the fabric toe region.

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Contact angle. Dynamic Angle Tester DAT 1100 (Fibro System AB, Sweden) was used to

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measure the angle of the ink or deionized water of the volume of ca. 3 µL that is in contact

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with the fabric as a function of time.

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Electric signal analysis. Soundcard-based virtual oscilloscope system Soundcard

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Oscilloscope V1.46 (Christian Zeitnitz, Germany) was used to generate and to record the

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complex signals with a frequency of 0.5–20 kHz through the inkjet-printed conductive paths

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on fabrics. In addition, measurements were carried out using a SHT75 humidity sensor

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(Sensirion AG, Switzerland). The readings were done using an open source platform Arduino

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Uno, which used the 2-wire library to dialogue with the 4-pin sensor. The electrical resistance

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was measured using an A830L digital multimeter.

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Results and Discussion

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The printing quality on woven fabrics can be improved by using coatings that force the

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pigment or colorant to concentrate and settle on the surface rather than to spread within the

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depth of the fabric. The desired coating should act as a support for printing ink while

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preserving the fabric flexibility. CNFs have the same nature as cotton, thus they can impose

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minimal alteration to woven cotton fabrics when used as coatings. However, the inherent

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brittleness of CNF films has to be overcome. In this work, glycerol was used as a plasticizer

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to impart flexibility to the CNF coatings.

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Fig. 1a–c show mechanical properties of the fabrics coated with CNFs and CNFs/glycerol

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(10/1 wt/wt) mixture. The breaking force of coated textiles remains practically unchanged at

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low amount of deposited formulations (see Fig. 1a). Whereas it tends to decrease slightly as

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the coating amount increases. Despite the large error bars, CNF/glycerol coatings seem to

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have slightly higher values of breaking force compared to CNF ones. The elongation at break

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remains constant for the fabric treated with CNFs/glycerol (see Fig. 1b) compared to the

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coatings of CNFs alone, elongation of which decreases progressively. In addition, Young’s

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modulus values (see Fig. 1c) indicate that the stiffness of coated textile increases with higher

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amount of applied formulations. These results demonstrate the reinforcing capacity of CNF

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coatings both with and without plasticizer. CNF/glycerol coatings at lower basis weight result

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in enhancement of Young’s modulus while keeping constant both the breaking force and the

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elongation at break, thus, suggesting that toughness of the coated fabrics slightly increases. 7 ACS Paragon Plus Environment

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The use of glycerol allows reducing brittleness of the coatings exposed to elongation. These

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conclusions are in agreement with the results found for other polysaccharides, e.g. starch,

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chitosan or cellulose derivatives.41–43 The introduction of the plasticizer is believed to enhance

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sliding of the nanofibers without compromising the overall mechanical resistance of the CNF

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coating.

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Fig. 1 Mechanical properties of woven cotton fabrics non-coated and coated with CNFs or CNFs/glycerol (10/1 wt/wt) with different basis weight (a, b, c) and visual appearance of CNF (d) and CNFs/glycerol (e, f) freestanding cast films (ca. 55 g/m2) that were 180° folded and unfolded; the films folded one (e) or three (f) times

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The effect of the introduction of glycerol on the mechanical properties is also reflected by

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the improved foldability of the freestanding cast films. The photographs of the CNF films

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(with a thickness of ca. 40 µm, measured using a digital micrometer (Model IDC-112MB;

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Mitutoyo Co, Japan) and an basis weight of ca. 55 g/m2) without and with glycerol, which

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were folded and unfolded for 180° one time, are shown in Fig. 1d and Fig. 1e, respectively.

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The film without glycerol breaks, whereas the plasticized film does not fall apart. Moreover,

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the addition of the plasticizer allows to fold-unfold the film several times without rupture (see

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Fig. 1f). Therefore, CNFs/glycerol coatings were further used to study the effect of the

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coating on printability of fabrics.

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Fig. 2a shows the contact angle of a droplet of water on the surface of fabric in the time

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interval of up to 10 s. The higher contact angle on the non-coated fabric can be explained by

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the presence of lubricant residues (e.g., tallow or mineral oil) widely used in fabric weaving

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processes44 that impart some hydrophobicity to cellulose. Therefore, the water droplet stays

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on the surface of the fabric without distinct penetration, reflected by the practically non-

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changed droplet volume. As expected, the contact angle is significantly reduced when the 8 ACS Paragon Plus Environment

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CNF-based coatings are applied. Additionally, the droplet absorption rate becomes faster. The

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above indicates both better surface wettability and better water penetration rate when the

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coated fabrics are used. The contact angle decreases further with the higher basis weight of

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the coating, which occurs due to the progressive introduction of more hydrophilic material.

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Fig. 2 Water (a) and pigment ink (b) contact angle measurements on the woven cotton fabrics with different amount of coated CNFs/glycerol

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When the cyan pigment ink is used for the contact angle measurements, the surface wetting

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becomes overall better (see Fig. 2b) compared to that when using water, which is explained

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by lower surface tension of the ink. Due to the better wetting, the ink penetrates faster into the

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substrate. However, the ink absorption rate becomes slower for the coated fabric compared to

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the uncoated one, indicated by slower decrease of the droplet volume. Such phenomena may

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be explained by the formation of filter cake,45 which is likely to occur when using CNF-based

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coatings with nanoscale fibril network. In such a process, pigment particles fill the pores,

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aggregate and hinder the water transfer through the substrate. When non-coated fabric is used,

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the rate of ink penetration into the fabric is higher due to higher porosity of the substrate.

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It was previously reported that by decreasing the ink contact angle on substrates, wider

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printed patterns are obtained by inkjet printing; thus, the printing resolution decreases.46 On

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the other hand, the surface roughness plays an important role for the printed pattern

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resolution. It is also noteworthy that the ink volume per unit area used for contact angle

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measurements is much higher than the maximum volume commonly used during inkjet

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printing. Thus, much less water is required to be absorbed by the coating during the printing

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process. The above contact angle measurements suggest that CNF-based coatings may be

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beneficial for higher speed inkjet printing on fabrics due to better surface wetting and faster

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ink droplet settling. 9 ACS Paragon Plus Environment

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SEM images of non-coated and coated woven cotton fabrics with various amount of

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CNFs/glycerol are shown in Fig. 3a. It can be seen that at 8.1 g/m2 the coating covers the

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surface of the fabric, even though some gaps remain not covered. The pores become

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completely filled when increasing the amount of the coating to 20.4 g/m2, resulting in a

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smooth layer that reduces the roughness of the fabric. These results are in good agreement

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with the previous studies showing the smoothening effect of CNF coatings on paper47–49 or on

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synthetic non-woven fabric mats.39

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Fig. 3 SEM images showing the top surface view of non-coated (a) and coated (b, c, d, e) woven cotton fabrics with 8.1 g/m2 (b), 13.4 g/m2 (c) and 20.4 g/m2 (d, e) of CNFs/glycerol and the cross-section view of the fabric coated with 20.4 g/m2 of CNFs/glycerol (f)

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Despite the nanoscale dimensions of CNFs, the coating mainly remains on the fabric

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surface and does not penetrate deep between the threads of the woven fabric (see Fig. 3f).

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This is likely to occur due to the entangled structure of the CNFs (see Fig. S1 in the

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Supporting Information). Since the CNF suspension was produced by mechanical fibrillation

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without chemical surface modification pretreatments, the nanofibrils are physically entangled.

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The size of these agglomerates decreases from ca. 300 µm to ca. 100 µm when exposed to

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shear flow,19 as during spraying. However, this size is still large enough for deep transfer into

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the fabric. Instead, these entanglements form a continuous film on the surface of the fabric.

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The inset in Fig. 3f illustrates the lamellar organization of the CNF coatings. Such a

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structure is not an artefact produced by the application of several spraying passes, but is an

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intrinsic property of CNF to self-assemble, which was also previously reported for CNF films

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prepared by casting/evaporation or vacuum filtration methods22,25,50 from surface modified50

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Optical microscopy was then performed in order to investigate whether the CNF network

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prevents the pigment transfer to the fabric bulk. Fig. 4a and b show the cross-section and top

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view images of non-coated and coated with CNF/glycerol fabrics that were inkjet printed with

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different amount of water-based cyan ink, viz. 49 pL/droplet (Fig. 4a) and 145 pL/droplet

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(Fig. 4b). When printed on non-coated fabric, irrespective of the droplet volume, the ink

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penetrates deeply into the fabric structure. An increase of the amount of ink results in more

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saturated color. The printing on coated fabrics shows a striking difference, since the ink

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pigment is localized on the surface of the CNF-based coating without penetrating the fabric

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threads. This observation is in agreement with the contact angle measurements (see Fig. 2)

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that suggested the filter cake formation phenomenon and pigment localization on the surface

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of the coating. This hypothesis is also supported by the pore size of the CNF layer that is in

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the same range as the pigment particles. The increase of the droplet size, as for the non-coated

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textile, leads also to a higher color saturation.

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319 320 321 322 323

Fig. 4 Optical microscope images of non-coated (up) and coated (bottom) with 8.1 g/m2 CNFs/glycerol (10/1 w/w) fabrics. The images of cross-section (a, b left) and top view (a, b right) of fabrics printed with cyan pigment ink volume of 49 pL/droplet (a) and 145 pL/droplet (b). The fabrics with printed patterns having two line pairs per mm (c)

324 325

The printing resolution also benefits of the CNF-based coatings, as demonstrated in Fig.

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4c, which shows the visual appearance of the printed pattern with two line pairs per mm. The

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resolution test chart with the wide range of line pairs (1.2–5.2) per mm printed on coated and

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non-coated fabrics is shown in Fig. S2 in the Supporting Information.

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In order to quantify the reduction of pigment penetration and its influence on color

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properties, colorimetry measurements were carried out using various cyan ink amount on non-

331

coated and coated textiles with different coating basis weight. Fig. 5a demonstrates the CIE

332

L*a*b* color space representing the change of chromatic components by varying the ink

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amount per droplet and printing on non-coated and coated fabrics with 8.1 g/m2 of

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CNFs/glycerol.

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The color properties of coated and non-coated fabrics before printing are very similar (see

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Fig. 5a) and tend towards yellow, representing the color of the unbleached cotton fabric.

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Therefore, the presence of CNF-based coating does not deteriorate the visual aspect of the

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fabrics. When the coatings are applied on fabrics, which are further printed with cyan ink,

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there is an enhancement of the print chroma. Therefore, the use of CNF-based coating can

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increase the color gamut, i.e. the capacity in reproducing a larger set of colors. This can be

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explained by: (i) the reduction of the pigment penetration to the fabric depth and (ii) the

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decrease of the substrate roughness and hence the light scattering.

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344 345 346 347

Fig. 5 Colorimetric properties of non-coated and coated textiles non-printed and printed with various ink volume per droplet: (a) CIE L*a*b* color space showing the change of chromatic components, (b) lightness and (c) chroma at different volumes of ink per droplet.

348 349

Variation of the chroma parameter C* as a function of coating basis weight is shown in

350

Fig. 5b. It can be seen that the chroma increases already at 8.1 g/m2 for all the amounts of ink

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per droplet. As the amount of deposited coating further increases, no distinct changes in

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chroma are observed, which is in line with Fig. 3 showing no drastic fabric surface coverage

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after the coating of 8.1 g/m2. On the other hand, Fig. 5c indicates that the lightness L*, i.e. the

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perceived brightness of an object, continues decreasing further with an increase of the amount

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of coating, which is in agreement with previous reports.40 It can be seen that similar values of

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L* can be obtained for fabrics coated with 8.1 g/m2 printed with 49 pL/droplet and non-coated 12 ACS Paragon Plus Environment

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fabrics printed with 101 pL/droplet, as a result of the increased pigment particle density on the

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surface.

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The above results, which showed the reduction of the pigment penetration to the fabric

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depth by application of the CNF/glycerol coatings, were further utilized to print conductive

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paths on the cotton fabrics. The use of silver nanoparticle-based ink has become relatively

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common for specific substrates, such as synthetic polymers, and often require a sintering step

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in order to enhance the interparticle contacts, needed to achieve proper conductivity. In the

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case of textile, however, the highly porous nature of the material does not allow to reach a

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sufficient particle density necessary to achieve good conductivity values when using low

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amount of ink.

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Fig. 6a shows an example of the circuitry that was inkjet printed using only three passes

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with silver nanoparticle ink on the fabric with 8.1 g/m2 CNF-based coating. When no coating

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was applied on the fabric, the sheet resistance of the printed pattern was >83.3 kΩ/sq (above

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the threshold of the multimeter). When the coating was used, the sheet resistance became

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significantly lower, viz. 2.9 ± 0.3 Ω/sq. Thus, the use of CNF-based coating reduced

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significantly the printed path resistance and allowed to manufacture the demonstration circuit

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composed of an inkjet-printed conductive path, a LED and a battery.

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375 376 377 378 379 380

Fig. 6 Manufacturing of inkjet-printed paths using silver nanoparticle ink on cotton woven fabrics coated with CNFs/glycerol (8.1 g/m2): (a, b) with connected LED and the battery; (c) with connected digital humidity sensor, the signal processing circuit and the LED display; and waveform of the signals at (d) 2 kHz and (e) 5 kHz recorded from the printed path (right path in a) on the fabric and the corresponding frequency spectrums in the insets.

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Fig. 6b and the video (see the Supporting Information) show that such circuitry operates

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well when the fabric is largely bent or folded several times. In the present case, the CNF layer

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enables to maintain the interparticle cohesion, which preserves the printed path conductivity.

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Additionally, the electric signal quality was assessed using oscilloscope by sending sine wave

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signals with a frequency of 0.5–20 kHz through the printed path (right path in Fig. 6a). The

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recorded signals for the frequencies of 2 and 5 kHz are shown in Fig. 6d and Fig. 6e,

388

respectively. No considerable distortions of amplitude could be noted.

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Another more complex demonstration of the e-textile is given in Fig. 6c, where the signal

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quality is evaluated via communication of the digital humidity sensor SHT75 (Sensirion AG,

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Switzerland) with a microcontroller through the inkjet-printed conductive paths on the fabric

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using an advanced data coding on two wires (I2C). The information from the sensor is

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processed by an Arduino Uno platform to be displayed on an LCD screen. In such a case, the

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transferred signal is of binary nature with pulse lengths typically ranging from 15 to 250 ns.

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This illustrates that the conductive paths are suitable for advanced electronic applications,

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whereas conductive paths of low qualities would not enable proper data decoding.

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The high quality of signal transfer through the conductive paths could be explained by the

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silver nanoparticle layer morphology on the coated fabric, as shown Fig. 7. When no coating

399

is applied, the layer of silver nanoparticles on the fabric is non-continuous (see Fig. 7a,b),

400

whereas, when CNF-based coating is present (see Fig. 7c,d), the silver nanoparticles remain

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on the surface of the coating and form a concentrated uniform layer, which finally results in

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highly conductive circuits. It is interesting to look further at the details of the dried ink

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droplets on the surface (Fig. 7c). Owing to the presence of the CNF layer, the liquid of the

404

picoliter-size ink droplet is drained and leaves a circular deposit of silver nanoparticles of ca.

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25 µm in diameter. This implies that the resolution limit of the printed pattern could approach

406

this specific size, allowing the conductive paths with a width as low as a few tens of

407

micrometers to be produced.

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409 410 411 412 413

Fig. 7 SEM images at different magnification showing the silver nanoparticle pigment inkjet-printed on (a, b) non-coated woven cotton fabrics, showing that the pigment does not create a uniform layer and on (c, d) CNFs/glycerol-coated woven cotton fabrics (8.1 g/m2), where the pigment well resides on the surface of the coating and forms a uniform layer.

414 415 416

Conclusions This study shows that plasticized CNFs can be applied as coating on woven cotton fabrics,

417

resulting in web-like networks of nanofibrils that reduce the fabric roughness and preserve

418

their visual appearance, being similar in nature to cotton. Compared to various elastomer

419

coatings, development of all-cellulose product applying wood-derived CNFs on cotton fabric

420

appears very attractive. The application of plasticized CNF coatings reduce the pigment

421

penetration into the fabric bulk, while not lowering their mechanical properties. By enhancing

422

the pigment density on the surface of the fabric, it is possible to improve the print quality or to

423

reduce the amount of needed inks. We show that such an approach can be used to produce

424

electronic textiles with inkjet-printed conductive paths made of silver nanoparticle ink. High

425

conductivity of printed paths can be achieved with low amount of printed ink, which is not

426

possible on non-coated fabrics.

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The use of such coatings may be further extended for inkjet printing of supercapacitors or

428

antennas. The use of inkjet printing gives a large flexibility in terms of printed pattern

429

geometry and offers opportunities of printing on demand, compared to the other techniques

430

based on weaving of the conductive elements into the fabric or screen printing. Moreover, 15 ACS Paragon Plus Environment

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inkjet printing allows multi-channel printing with several different inks in one pass,

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depending on the number of installed cartridges. Additionally, nanocellulose coatings may be

433

promising for better fabric recyclability, due to limited coloring of the fabric structure. This

434

may facilitate the transition from the traditional dyeing technology towards the

435

environmentally friendly and market-driven inkjet printing.

436

There is still a limitation of using such an approach if the washable fabrics are desired,

437

since there is not enough adhesion between the CNF coating and the fabric. The further work

438

on improving the robustness of CNF coatings on fabrics, e.g., using cross-linking approach,35

439

can provide wider opportunities for industrial application of such technology. On the other

440

hand, however, such coatings can be readily used for the production of green disposable

441

electronic textiles and garments, e.g. for medical and health care applications, where the

442

washability is not a limiting factor.

443

Associated content

444

Supporting Information

445

Video of bending of the produced e-textile (MP4).

446

AFM and optical microscopy images of CNFs, SEM images of non-coated and

447

CNF/glycerol-coated fabrics printed with cyan pigment ink; photographs of the fabrics with

448

printed resolution test charts (PDF).

449

Author information

450

Corresponding Authors

451

* (O.N.) e-mail: [email protected]

452

* (R.B.) e-mail: [email protected]

453

Notes

454

The authors declare no competing financial interest.

455 456

Acknowledgments The authors are grateful to Anders Mårtensson from Chalmers University of Technology

457

for the support with SEM measurements and to Mats Johansson and Sina Seipel from

458

University of Borås for their assistance in inkjet printing and colorimetric measurements,

459

respectively. J.Y. and V.N. are grateful for the financial support from KK-stiftelsen (The

460

Knowledge Foundation) and TEKO for enabling this research. 16 ACS Paragon Plus Environment

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References

462 463 464 465 466 467 468 469 470 471 472 473 474 475 476 477 478 479 480 481 482 483 484 485 486 487 488 489 490 491 492 493 494 495 496 497 498 499 500 501 502 503 504 505 506 507 508

(1) (2)

(3) (4)

(5) (6)

(7) (8)

(9) (10)

(11) (12) (13)

(14)

(15) (16) (17)

(18)

(19)

Park, S.; Jayaraman, S. Smart Textiles: Wearable Electronic Systems. MRS Bull. 2003, 28 (08), 585–591. Hu, L.; Pasta, M.; Mantia, F. L.; Cui, L.; Jeong, S.; Deshazer, H. D.; Choi, J. W.; Han, S. M.; Cui, Y. Stretchable, Porous, and Conductive Energy Textiles. Nano Lett. 2010, 10 (2), 708–714. Weng, W.; Chen, P.; He, S.; Sun, X.; Peng, H. Smart Electronic Textiles. Angew. Chem. Int. Ed. 2016, 55 (21), 6140–6169. Philips, T. Revolutionizing Textile Decoration and Finishing with Digital Inkjet Technology. In International Conference on Textile Coating and Laminating; Cannes, France, 2010. Kant, R. Textile Dyeing Industry an Environmental Hazard. 2012, 4 (1), 22–26. Long, J.-J.; Xu, H.-M.; Cui, C.-L.; Wei, X.-C.; Chen, F.; Cheng, A.-K. A Novel Plant for Fabric Rope Dyeing in Supercritical Carbon Dioxide and Its Cleaner Production. J. Clean. Prod. 2014, 65, 574–582. Stoppa, M.; Chiolerio, A. Wearable Electronics and Smart Textiles: A Critical Review. Sensors 2014, 14 (7), 11957–11992. Stempien, Z.; Rybicki, E.; Rybicki, T.; Lesnikowski, J. Inkjet-Printing Deposition of Silver Electro-Conductive Layers on Textile Substrates at Low Sintering Temperature by Using an Aqueous Silver Ions-Containing Ink for Textronic Applications. Sens. Actuators B Chem. 2016, 224, 714–725. Hoeng, F.; Denneulin, A.; Bras, J. Use of Nanocellulose in Printed Electronics: A Review. Nanoscale 2016, 8, 13131–13154. Chauve, G.; Bras, J. Industrial Point of View of Nanocellulose Materials and Their Possible Applications. In Handbook of Green Materials; Materials and Energy; World Scientific, 2014; Vol. Volume 5, pp 233–252. Nechyporchuk, O.; Belgacem, M. N.; Bras, J. Production of Cellulose Nanofibrils: A Review of Recent Advances. Ind. Crops Prod. 2016, 93, 2–25. Bardet, R.; Bras, J. Cellulose Nanofibers and Their Use in Paper Industry. In Handbook of Green Materials; World Scientific, 2014; pp 207–232. Brodin, F. W.; Gregersen, Ø. W.; Syverud, K. Cellulose Nanofibrils: Challenges and Possibilities as a Paper Additive or Coating Material – A Review. Nord. Pulp Pap. Res. J. 2014, 29 (01), 156–166. Hassan, E. A.; Hassan, M. L.; Abou-zeid, R. E.; El-Wakil, N. A. Novel Nanofibrillated Cellulose/Chitosan Nanoparticles Nanocomposites Films and Their Use for Paper Coating. Ind. Crops Prod. 2016, 93, 219–226. Siró, I.; Plackett, D. Microfibrillated Cellulose and New Nanocomposite Materials: A Review. Cellulose 2010, 17 (3), 459–494. Miao, C.; Hamad, W. Y. Cellulose Reinforced Polymer Composites and Nanocomposites: A Critical Review. Cellulose 2013, 20 (5), 2221–2262. Nechyporchuk, O.; Pignon, F.; Botelho Do Rego, A. M.; Belgacem, M. N. Influence of Ionic Interactions between Nanofibrillated Cellulose and Latex on the Ensuing Composite Properties. Compos. Part B Eng. 2016, 85, 188–195. Dimic-Misic, K.; Gane, P. A. C.; Paltakari, J. Micro- and Nanofibrillated Cellulose as a Rheology Modifier Additive in CMC-Containing Pigment-Coating Formulations. Ind. Eng. Chem. Res. 2013, 52 (45), 16066–16083. Nechyporchuk, O.; Belgacem, M. N.; Pignon, F. Current Progress in Rheology of Cellulose Nanofibril Suspensions. Biomacromolecules 2016, 17 (7), 2311–2320.

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509 510 511 512 513 514 515 516 517 518 519 520 521 522 523 524 525 526 527 528 529 530 531 532 533 534 535 536 537 538 539 540 541 542 543 544 545 546 547 548 549 550 551 552 553 554 555 556 557 558

Page 18 of 21

(20) Xhanari, K.; Syverud, K.; Chinga-Carrasco, G.; Paso, K.; Stenius, P. Structure of Nanofibrillated Cellulose Layers at the O/W Interface. J. Colloid Interface Sci. 2011, 356 (1), 58–62. (21) Gestranius, M.; Stenius, P.; Kontturi, E.; Sjöblom, J.; Tammelin, T. Phase Behaviour and Droplet Size of Oil-in-Water Pickering Emulsions Stabilised with Plant-Derived Nanocellulosic Materials. Colloids Surf. Physicochem. Eng. Asp. 2016, 519, 60–70. (22) Henriksson, M.; Berglund, L. A.; Isaksson, P.; Lindström, T.; Nishino, T. Cellulose Nanopaper Structures of High Toughness. Biomacromolecules 2008, 9 (6), 1579–1585. (23) Fukuzumi, H.; Saito, T.; Iwata, T.; Kumamoto, Y.; Isogai, A. Transparent and High Gas Barrier Films of Cellulose Nanofibers Prepared by TEMPO-Mediated Oxidation. Biomacromolecules 2009, 10 (1), 162–165. (24) González, I.; Alcalà, M.; Chinga-Carrasco, G.; Vilaseca, F.; Boufi, S.; Mutjé, P. From Paper to Nanopaper: Evolution of Mechanical and Physical Properties. Cellulose 2014, 21 (4), 2599–2609. (25) Li, Q.; Chen, W.; Li, Y.; Guo, X.; Song, S.; Wang, Q.; Liu, Y.; Li, J.; Yu, H.; Zeng, J. Comparative Study of the Structure, Mechanical and Thermomechanical Properties of Cellulose Nanopapers with Different Thickness. Cellulose 2016, 23 (2), 1375–1382. (26) Pääkkö, M.; Vapaavuori, J.; Silvennoinen, R.; Kosonen, H.; Ankerfors, M.; Lindström, T.; Berglund, L. A.; Ikkala, O. Long and Entangled Native Cellulose I Nanofibers Allow Flexible Aerogels and Hierarchically Porous Templates for Functionalities. Soft Matter 2008, 4 (12), 2492. (27) Sehaqui, H.; Zhou, Q.; Berglund, L. A. High-Porosity Aerogels of High Specific Surface Area Prepared from Nanofibrillated Cellulose (NFC). Compos. Sci. Technol. 2011, 71 (13), 1593–1599. (28) Hamedi, M.; Karabulut, E.; Marais, A.; Herland, A.; Nyström, G.; Wågberg, L. Nanocellulose Aerogels Functionalized by Rapid Layer-by-Layer Assembly for High Charge Storage and Beyond. Angew. Chem. Int. Ed. 2013, 52 (46), 12038–12042. (29) Abe, K.; Yano, H. Formation of Hydrogels from Cellulose Nanofibers. Carbohydr. Polym. 2011, 85 (4), 733–737. (30) Abe, K.; Yano, H. Cellulose Nanofiber-Based Hydrogels with High Mechanical Strength. Cellulose 2012, 19 (6), 1907–1912. (31) Chinga-Carrasco, G.; Tobjörk, D.; Österbacka, R. Inkjet-Printed Silver Nanoparticles on Nano-Engineered Cellulose Films for Electrically Conducting Structures and Organic Transistors: Concept and Challenges. J. Nanoparticle Res. 2012, 14 (11), 1– 10. (32) Hsieh, M.-C.; Kim, C.; Nogi, M.; Suganuma, K. Electrically Conductive Lines on Cellulose Nanopaper for Flexible Electrical Devices. Nanoscale 2013, 5 (19), 9289– 9295. (33) Nogi, M.; Komoda, N.; Otsuka, K.; Suganuma, K. Foldable Nanopaper Antennas for Origami Electronics. Nanoscale 2013, 5 (10), 4395–4399. (34) Yagyu, H.; Saito, T.; Isogai, A.; Koga, H.; Nogi, M. Chemical Modification of Cellulose Nanofibers for the Production of Highly Thermal Resistant and Optically Transparent Nanopaper for Paper Devices. ACS Appl. Mater. Interfaces 2015, 7 (39), 22012–22017. (35) Zhu, H.; Narakathu, B. B.; Fang, Z.; Aijazi, A. T.; Joyce, M.; Atashbar, M.; Hu, L. A Gravure Printed Antenna on Shape-Stable Transparent Nanopaper. Nanoscale 2014, 6 (15), 9110–9115. (36) Torvinen, K.; Sievänen, J.; Hjelt, T.; Hellén, E. Smooth and Flexible FillerNanocellulose Composite Structure for Printed Electronics Applications. Cellulose 2012, 19 (3), 821–829. 18 ACS Paragon Plus Environment

Page 19 of 21

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559 560 561 562 563 564 565 566 567 568 569 570 571 572 573 574 575 576 577 578 579 580 581 582 583 584 585 586 587 588 589 590 591 592 593 594 595 596

(37) Penttilä, A.; Sievänen, J.; Torvinen, K.; Ojanperä, K.; Ketoja, J. A. FillerNanocellulose Substrate for Printed Electronics: Experiments and Model Approach to Structure and Conductivity. Cellulose 2013, 20 (3), 1413–1424. (38) Okahisa, Y.; Yoshida, A.; Miyaguchi, S.; Yano, H. Optically Transparent Wood– cellulose Nanocomposite as a Base Substrate for Flexible Organic Light-Emitting Diode Displays. Compos. Sci. Technol. 2009, 69 (11–12), 1958–1961. (39) Hamada, H.; Bousfield, D. W. Nanofibrillated Cellulose as a Coating Agent to Improve Print Quality of Synthetic Fiber Sheets. Tappi J. 2010, 9 (11), 25–29. (40) Hamada, H.; Mitsuhashi, M. Effect of Cellulose Nanofibers as a Coating Agent for Woven and Nonwoven Fabrics. Nord. Pulp Pap. Res. J. 2016, 31 (2). (41) Arvanitoyannis, I.; Biliaderis, C. G. Physical Properties of Polyol-Plasticized Edible Blends Made of Methyl Cellulose and Soluble Starch. Carbohydr. Polym. 1999, 38 (1), 47–58. (42) Avérous, L.; Fringant, C.; Moro, L. Plasticized Starch–cellulose Interactions in Polysaccharide Composites. Polymer 2001, 42 (15), 6565–6572. (43) Srinivasa, P. C.; Ramesh, M. N.; Tharanathan, R. N. Effect of Plasticizers and Fatty Acids on Mechanical and Permeability Characteristics of Chitosan Films. Food Hydrocoll. 2007, 21 (7), 1113–1122. (44) Moss, E. The Lubrication of Cotton and Other Textiles. Br. J. Appl. Phys. 1951, 2 (S1), 19. (45) Desie, G.; Deroover, G.; De Voeght, F.; Soucemarianadin, A. Printing of Dye and Pigment-Based Aqueous Inks Onto Porous Substrates. J. Imaging Sci. Technol. 2004, 48 (5), 389–397. (46) Smith, P. J.; Shin, D.-Y.; Stringer, J. E.; Derby, B.; Reis, N. Direct Ink-Jet Printing and Low Temperature Conversion of Conductive Silver Patterns. J. Mater. Sci. 2006, 41 (13), 4153–4158. (47) Ankerfors, M.; Lindstroem, T.; Hoc, M.; Song, H. Composition for Coating of Printing Paper. WO2009123560 (A1), October 8, 2009. (48) Aulin, C.; Gällstedt, M.; Lindström, T. Oxygen and Oil Barrier Properties of Microfibrillated Cellulose Films and Coatings. Cellulose 2010, 17 (3), 559–574. (49) Lavoine, N.; Desloges, I.; Bras, J. Microfibrillated Cellulose Coatings as New Release Systems for Active Packaging. Carbohydr. Polym. 2014, 103, 528–537. (50) Huang, J.; Zhu, H.; Chen, Y.; Preston, C.; Rohrbach, K.; Cumings, J.; Hu, L. Highly Transparent and Flexible Nanopaper Transistors. ACS Nano 2013, 7 (3), 2106–2113. (51) Spence, K. L.; Venditti, R. A.; Rojas, O. J.; Pawlak, J. J.; Hubbe, M. A. Water Vapor Barrier Properties of Coated and Filled Microfibrillated Cellulose Composite Films. BioResources 2011, 6 (4), 4370–4388.

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Title: Cellulose nanofibril-based coatings of woven cotton fabrics for improved inkjet

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printing with a potential in e-textile manufacturing

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Authors: Oleksandr Nechyporchuk, Junchun Yu, Vincent Nierstrasz, Romain Bordes

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TOC/Abstract graphic:

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Synopsis: Cellulose nanofibril-based coatings control the ink penetration to woven cotton

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fabrics and are beneficial to reduce the amount of conductive silver ink used for electronic

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textile manufacturing.

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