Cellulose Nanofibril-Based Coatings of Woven ... - ACS Publications

May 5, 2017 - Each fabric sample was processed by three printing cycles. ... using an open source platform Arduino Uno, which used the 2-wire ..... hu...
0 downloads 0 Views 2MB Size
Subscriber access provided by University of Florida | Smathers Libraries

Article

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

Just Accepted “Just Accepted” manuscripts have been peer-reviewed and accepted for publication. They are posted online prior to technical editing, formatting for publication and author proofing. The American Chemical Society provides “Just Accepted” as a free service to the research community to expedite the dissemination of scientific material as soon as possible after acceptance. “Just Accepted” manuscripts appear in full in PDF format accompanied by an HTML abstract. “Just Accepted” manuscripts have been fully peer reviewed, but should not be considered the official version of record. They are accessible to all readers and citable by the Digital Object Identifier (DOI®). “Just Accepted” is an optional service offered to authors. Therefore, the “Just Accepted” Web site may not include all articles that will be published in the journal. After a manuscript is technically edited and formatted, it will be removed from the “Just Accepted” Web site and published as an ASAP article. Note that technical editing may introduce minor changes to the manuscript text and/or graphics which could affect content, and all legal disclaimers and ethical guidelines that apply to the journal pertain. ACS cannot be held responsible for errors or consequences arising from the use of information contained in these “Just Accepted” manuscripts.

ACS Sustainable Chemistry & Engineering is published by the American Chemical Society. 1155 Sixteenth Street N.W., Washington, DC 20036 Published by American Chemical Society. Copyright © American Chemical Society. However, no copyright claim is made to original U.S. Government works, or works produced by employees of any Commonwealth realm Crown government in the course of their duties.

Page 1 of 21

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

ACS Sustainable Chemistry & Engineering

1

Cellulose nanofibril-based coatings of woven cotton

2

fabrics for improved inkjet printing with a potential

3

in e-textile manufacturing

4

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

5 6



7 8

§

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

9

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

10

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

11 12 13 14 15 16 17 18 19 20 21 22 23

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

24

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

25

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.

26

1 ACS Paragon Plus Environment

ACS Sustainable Chemistry & Engineering

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

27

Page 2 of 21

Introduction

28

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

29

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

30

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

31

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

32

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

33

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

34

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

35

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

36

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

37

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

38

developing complex circuitry.

39

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

40

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

41

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

42

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

43

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

44

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

45

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

46

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

47

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

48

waterless dyeing using supercritical carbon dioxide.6

49

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

50

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

51

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

52

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

53

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

54

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

55

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

56

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

57

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

58

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

59

expensive. 2 ACS Paragon Plus Environment

Page 3 of 21

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

ACS Sustainable Chemistry & Engineering

60

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

61

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

62

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

63

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

64

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

65

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

66

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

67

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

68

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

69

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

70

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

71

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

72

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

73

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

74

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

75

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

76

mechanical disintegration without chemical surface modification or with carboxylation or

77

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

78

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

79

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

80

wettability of the film surfaces through grafting with hexamethyldisilazane.31

81

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

82

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

83

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

84

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

85

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

86

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

87

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

88

proposed as substrates for flexible electronic devices.

89

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

90

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

91

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

92

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

93

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

ACS Sustainable Chemistry & Engineering

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

Page 4 of 21

94

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

95

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

96

CNFs on cotton fabric appears very attractive.

97

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

98

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

99

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

100

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

101

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

102

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

103

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

104

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

105

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

106

also evaluated.

107

Materials

108

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

109

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

110

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

111

from Sigma-Aldrich Sweden AB.

112

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

113

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

114

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

115

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

116

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

117

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

118

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

119

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

120

polydiallyldimethylammonium chloride).

121

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

122

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

123

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

124

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

125

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

126

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

Page 5 of 21

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

ACS Sustainable Chemistry & Engineering

127

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

128

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

129

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

130

3.0 mN/m, as reported by the supplier.

131

Methods

132

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

133

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

134

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

135

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

136

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

137

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

138

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

139

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

140

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

141

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

142

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

143

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

144

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

145

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

146

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

147

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

148

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

149

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

150

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

151

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

152

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

153

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

154

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

155

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

156

conductivity of the printed circuit, without thermal sintering step.

157 158

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

5 ACS Paragon Plus Environment

ACS Sustainable Chemistry & Engineering

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

159

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

160

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

Page 6 of 21

161

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

162

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

163

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

164

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

165

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

166

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

167

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

168

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

169

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

170

image processing.

171

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

172

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

173

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

174

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

175

height images were then processed in Gwyddion software.

176

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

177

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

178

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

179

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

180

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

181

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

182

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

183

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

184

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

185

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

186

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

187

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

188

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

189

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

190

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

191

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

192

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

Page 7 of 21

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

ACS Sustainable Chemistry & Engineering

193

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

194

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

195

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

196

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

197

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

198

with the fabric as a function of time.

199

Electric signal analysis. Soundcard-based virtual oscilloscope system Soundcard

200

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

201

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

202

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

203

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

204

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

205

was measured using an A830L digital multimeter.

206

Results and Discussion

207

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

208

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

209

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

210

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

211

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

212

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

213

to impart flexibility to the CNF coatings.

214

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

215

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

216

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

217

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

218

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

219

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

220

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

221

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

222

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

223

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

224

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

225

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

ACS Sustainable Chemistry & Engineering

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

Page 8 of 21

226

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

227

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

228

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

229

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

230

coating.

231

232 233 234 235 236

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

237 238

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

239

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

240

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

241

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

242

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

243

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

244

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

245

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

246

coating on printability of fabrics.

247

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

248

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

249

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

250

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

251

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

252

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

Page 9 of 21

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

ACS Sustainable Chemistry & Engineering

253

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

254

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

255

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

256

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

257 258 259

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

260 261

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

262

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

263

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

264

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

265

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

266

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

267

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

268

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

269

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

270

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

271

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

272

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

273

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

274

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

275

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

276

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

277

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

278

ink droplet settling. 9 ACS Paragon Plus Environment

ACS Sustainable Chemistry & Engineering

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

Page 10 of 21

279

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

280

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

281

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

282

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

283

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

284

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

285

synthetic non-woven fabric mats.39

286

287 288 289 290

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)

291 292

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

293

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

294

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

295

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

296

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

297

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

298

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

299

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

300

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

301

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

302

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

303

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

304

and non-modified22,25,51 CNFs. 10 ACS Paragon Plus Environment

Page 11 of 21

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

ACS Sustainable Chemistry & Engineering

305

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

306

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

307

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

308

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

309

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

310

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

311

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

312

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

313

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

314

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

315

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

316

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

317

textile, leads also to a higher color saturation.

318

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.

326

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

327

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

328

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

329

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

330

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

11 ACS Paragon Plus Environment

ACS Sustainable Chemistry & Engineering

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

333

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

334

CNFs/glycerol.

335

Page 12 of 21

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

336

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

337

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

338

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

339

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

340

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

341

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

342

decrease of the substrate roughness and hence the light scattering.

343

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

351

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

352

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

353

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

354

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

355

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

356

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

Page 13 of 21

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

ACS Sustainable Chemistry & Engineering

357

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

358

surface.

359

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

360

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

361

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

362

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

363

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

364

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

365

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

366

amount of ink.

367

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

368

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

369

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

370

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

371

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

372

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

373

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

374

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.

381 13 ACS Paragon Plus Environment

ACS Sustainable Chemistry & Engineering

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

Page 14 of 21

382

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

383

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

384

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

385

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

386

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

387

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.

389

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

390

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

391

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

392

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

393

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

394

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

395

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

396

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

397

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

398

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

401

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

402

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

403

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.

405

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.

408

14 ACS Paragon Plus Environment

Page 15 of 21

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

ACS Sustainable Chemistry & Engineering

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.

427

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

ACS Sustainable Chemistry & Engineering

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

Page 16 of 21

431

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

432

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

Page 17 of 21

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

ACS Sustainable Chemistry & Engineering

461

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.

17 ACS Paragon Plus Environment

ACS Sustainable Chemistry & Engineering

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

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

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

ACS Sustainable Chemistry & Engineering

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.

597 598 599

19 ACS Paragon Plus Environment

ACS Sustainable Chemistry & Engineering

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

600

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

601

printing with a potential in e-textile manufacturing

602

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

603

TOC/Abstract graphic:

Page 20 of 21

604 605

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

606

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

607

textile manufacturing.

20 ACS Paragon Plus Environment

Page 21 of 21

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

ACS Sustainable Chemistry & Engineering

TOC graphic 80x35mm (300 x 300 DPI)

ACS Paragon Plus Environment