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Tailoring Adhesion and Wetting Properties of Cellulose Fibres and Model Surfaces Using Layer-by-Layer Technology
KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Fibre Technology. KTH, School of Chemical Science and Engineering (CHE), Centres, Wallenberg Wood Science Center.
2014 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The versatile layer-by-layer (LbL) technique, for consecutive adsorption of polyelectrolytes and charged nanoparticles onto a substrate, was used to modify cellulose fibres and model surfaces for improved mechanical and wetting properties. In addition to being used to modify cellulose substrates, the LbL technique was also used to create cellulose surfaces suitable for high resolution adhesion measurements. LbL assembly of cellulose nanofibrils and polyethylenimine was used to prepare cellulose model surfaces on polydimethylsiloxane hemispheres which allowed for the first known Johnson-Kendall-Roberts (JKR) adhesion measurements between cellulose and smooth, well-defined model surfaces of cellulose, lignin and glucomannan. The work of adhesion on loading and the adhesion hysteresis were comparable for all three systems which suggest that adhesion between wood constituents is similar. The LbL technique was also used to decrease the hydrophilicity of paper, while improving the dry strength, by coating cellulose fibres with a polylallylamine hydrochloride (PAH) and polyacrylic acid (PAA) LbL film, followed by adsorption of anionic wax particles. Paper sheets made from the modified fibres were highly hydrophobic with a contact angle of 150°, while retaining, and in some cases improving, the tensile index of the paper. It was also observed that PAH/PAA modified sheets without the addition of wax became hydrophobic when heat treated. The mechanism behind the increased hydrophobicity was studied by the interface sensitive technique, vibrational sum frequency spectroscopy, which indicated that the increased hydrophobicity is a result of the reorientation of polymer chains to expose more hydrophobic CH2 and CH groups at the polymer-air interface. Paper sheets prepared from LbL-modified bleached softwood fibres using PAH and the biopolymer hyaluronic acid (HA) exhibited a 6.5% strain at break and a tensile index which was increased 3-fold compared to unmodified fibres. The wet adhesive properties of the PAH/HA system were studied by colloidal probe atomic force microscopy and correlated to film growth and viscoelastic behavior. The presence of background salt was a crucial parameter for achieving high adhesion but time in contact and LbL film thickness also strongly affected the adhesion. Finally, the wet adhesive properties of carboxymethylcellulose (CMC), which had been irreversibly adsorbed to regenerated cellulose, and polyvinylamine (PVAm) were evaluated by means of 90° peel tests. Strong wet adhesion was achieved for dried rewetted samples without any obvious chemical crosslinking, which was attributed to interdigitation and complex formation in PVAm-CMC films. This system also gave significant wet adhesion for non-dried systems at water contents around 45%.

Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2014. , vi, 73 p.
Series
TRITA-CHE-Report, ISSN 1654-1081 ; 2014:55
National Category
Polymer Technologies Materials Chemistry Paper, Pulp and Fiber Technology
Research subject
Fibre and Polymer Science
Identifiers
URN: urn:nbn:se:kth:diva-155932ISBN: 978-91-7595-347-2 (print)OAI: oai:DiVA.org:kth-155932DiVA: diva2:763483
Public defence
2014-12-04, F3, Lindstedtsvägen 26, KTH, Stockholm, 14:00 (English)
Opponent
Supervisors
Note

QC 20141117

Available from: 2014-11-17 Created: 2014-11-14 Last updated: 2014-11-17Bibliographically approved
List of papers
1. Direct Adhesive Measurements between Wood Biopolyrner Model Surfaces
Open this publication in new window or tab >>Direct Adhesive Measurements between Wood Biopolyrner Model Surfaces
2012 (English)In: Biomacromolecules, ISSN 1525-7797, E-ISSN 1526-4602, Vol. 13, no 10, 3046-3053 p.Article in journal (Refereed) Published
Abstract [en]

For the first time the dry adhesion was measured for an all-wood biopolymer system using Johnson-Kendall-Roberts (JKR) contact mechanics. The polydimethylsiloxane hemisphere was successfully surface-modified with a Cellulose I model surface using layer-by-layer assembly of nanofibrillated cellulose and polyethyleneimine. Flat surfaces of cellulose were equally prepared on silicon dioxide substrates, and model surfaces of glucomannan and lignin were prepared on silicon dioxide using spin-coating. The measured work of adhesion on loading and the adhesion hysteresis was found to be very similar between cellulose and all three wood polymers, suggesting that the interaction between these biopolymers do not differ greatly. Surface energy calculations from contact angle measurements indicated similar dispersive surface energy components for the model surfaces. The dispersive component was dominating the surface energy for all surfaces. The JKR work of adhesion was lower than that calculated from contact angle measurements, which partially can be ascribed to surface roughness of the model surfaces and overestimation of the surface energies from contact angle determinations.

Keyword
Adhesion, Angle measurement, Biomolecules, Biopolymers, Cellulose, Contact angle, Deformation, Interfacial energy, Loading; Silica, Silicones, Surface roughness
National Category
Chemical Sciences Paper, Pulp and Fiber Technology
Identifiers
urn:nbn:se:kth:diva-104696 (URN)10.1021/bm300762e (DOI)000309488600005 ()2-s2.0-84867475444 (Scopus ID)
Note

QC 20121112. Updated from Manuscript to Article

Available from: 2012-11-12 Created: 2012-11-09 Last updated: 2017-12-07Bibliographically approved
2. Treatment of cellulose fibres with polyelectrolytes and wax colloids to create tailored highly hydrophobic fibrous networks
Open this publication in new window or tab >>Treatment of cellulose fibres with polyelectrolytes and wax colloids to create tailored highly hydrophobic fibrous networks
2012 (English)In: Colloids and Surfaces A: Physicochemical and Engineering Aspects, ISSN 0927-7757, E-ISSN 1873-4359, Vol. 414, 415-421 p.Article in journal (Refereed) Published
Abstract [en]

Paper is a versatile material with obvious advantages in being both inexpensive and environment friendly. However, a major drawback compared with many other materials, such as plastics, is that it is sensitive to both liquid water and moist air. Traditionally paper is protected from liquid water by sizing. The present work presents a new way to make paper water resistant by combining the layer-by-layer (LbL) technique with the adsorption of a colloidal wax onto the multilayer structure. After the adsorption of five layers of poly(allylamine hydrochloride) and poly(acrylic acid) followed by the adsorption of 8. mg paraffin wax per gram fibre, the contact angle measured 60. s after a drop of water was applied to the sheet was about 138°. If the sheets were cured for 30. min at 160. °C after sheet making, the contact angle was ca. 150°. The heat treatment of sheets prepared from LbL-modified fibres without the addition of wax gave a contact angle of about 113°. To decouple structural effects from changes in surface energy upon heat treatment of PAH/PAA LbL films, model experiments were carried out where LbL assemblies were prepared on silicon oxide and cellulose model surfaces. The contact angle increased when these films were heat treated but it did not exceed 90°. The reason for this is due to the lack of structure of the model surfaces on a micrometre scale. The adsorption of wax impaired the mechanical properties of paper sheets made from modified fibres compared to sheets from the LbL-modified fibres. However, at an adsorption of 8. mg paraffin wax per gram fibre there was still an increase by 37 ± 1% in tensile strength index compared to the untreated reference pulp (33.8 ± 0.7 and 24.7 ± 0.6. kNm/kg respectively).

Keyword
Cellulose fibres, Dry strength, Hydrophobicity, Polyelectrolyte multilayers, Wax nanoparticles
National Category
Materials Engineering Paper, Pulp and Fiber Technology Nano Technology
Identifiers
urn:nbn:se:kth:diva-91373 (URN)10.1016/j.colsurfa.2012.08.042 (DOI)000312472000055 ()2-s2.0-84868329804 (Scopus ID)
Note

QC 20121212. Updated from submitted to published.

Available from: 2012-03-13 Created: 2012-03-13 Last updated: 2017-12-07Bibliographically approved
3. Vibrational sum frequency spectroscopy on polyelectrolyte multilayers – effect of molecular surface structure on macroscopic wetting properties
Open this publication in new window or tab >>Vibrational sum frequency spectroscopy on polyelectrolyte multilayers – effect of molecular surface structure on macroscopic wetting properties
Show others...
(English)Manuscript (preprint) (Other academic)
National Category
Polymer Chemistry Materials Chemistry Polymer Technologies
Identifiers
urn:nbn:se:kth:diva-155930 (URN)
Note

QS 2014

Available from: 2014-11-14 Created: 2014-11-14 Last updated: 2014-11-17Bibliographically approved
4. Robust and Tailored Wet Adhesion in Biopolymer Thin Films
Open this publication in new window or tab >>Robust and Tailored Wet Adhesion in Biopolymer Thin Films
Show others...
2014 (English)In: Biomacromolecules, ISSN 1525-7797, E-ISSN 1526-4602, Vol. 15, no 12, 4420-4428 p.Article in journal (Refereed) Published
Abstract [en]

Model layer-by-layer (LbL) assemblies of poly(allylamine hydrochloride) (PAH) and hyaluronic acid (HA) were fabricated in order to study their wet adhesive behavior. The film characteristics were investigated to understand the inherent structures during the assembly process. Subsequently, the adhesion of these systems was evaluated to understand the correlation between the structure of the film and the energy required to separate these LbL assemblies. We describe how the conditions of the LbL fabrication can be utilized to control the adhesion between films. The characteristics of the film formation are examined in the absence and presence of salt during the film formation. The dependence on contact time and LbL film thickness on the critical pull-off force and work of adhesion are discussed. Specifically, by introducing sodium chloride (NaCl) in the assembly process, the pull-off forces can be increased by a factor of 10 and the work of adhesion by 2 orders of magnitude. Adjusting both the contact time and the film thickness enables control of the adhesive properties within these limits. Based on these results, we discuss how the fabrication procedure can create tailored adhesive interfaces with properties surpassing analogous systems found in nature.

Keyword
Assembly, Fabrication, Film thickness, Hyaluronic acid, Sodium chloride, Adhesive interfaces, Adhesive properties, Fabrication procedure, Film characteristics, Layer-by-layer assemblies, Orders of magnitude, Poly(allylamine hydrochloride), Sodium chloride (NaCl)
National Category
Polymer Chemistry Polymer Technologies Materials Chemistry
Identifiers
urn:nbn:se:kth:diva-155931 (URN)10.1021/bm501202s (DOI)000346114400005 ()25333327 (PubMedID)2-s2.0-84916624800 (Scopus ID)
Note

QC 20150108

Available from: 2014-11-14 Created: 2014-11-14 Last updated: 2017-12-05Bibliographically approved

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