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Treatment of cellulose fibres with polyelectrolytes and wax colloids to create tailored highly hydrophobic fibrous networks
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.
KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Fibre Technology.ORCID iD: 0000-0002-7410-0333
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.ORCID iD: 0000-0001-8622-0386
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).

Place, publisher, year, edition, pages
2012. Vol. 414, 415-421 p.
Keyword [en]
Cellulose fibres, Dry strength, Hydrophobicity, Polyelectrolyte multilayers, Wax nanoparticles
National Category
Materials Engineering Paper, Pulp and Fiber Technology Nano Technology
Identifiers
URN: urn:nbn:se:kth:diva-91373DOI: 10.1016/j.colsurfa.2012.08.042ISI: 000312472000055Scopus ID: 2-s2.0-84868329804OAI: oai:DiVA.org:kth-91373DiVA: diva2:509695
Note

QC 20121212. Updated from submitted to published.

Available from: 2012-03-13 Created: 2012-03-13 Last updated: 2017-12-07Bibliographically approved
In thesis
1. Tailoring adhesion and wetting properties of cellulose fibers and model surfaces
Open this publication in new window or tab >>Tailoring adhesion and wetting properties of cellulose fibers and model surfaces
2012 (English)Licentiate thesis, comprehensive summary (Other academic)
Abstract [en]

The layer-by-layer (LbL) technique was used to modify the surface of cellulose fibers by consecutive adsorption of poly(allylamine hydrochloride) (PAH) and poly(acrylic acid) (PAA) followed by a final adsorbed layer of anionic paraffin wax colloids. Paper hand sheets made from the modified fibers were found to be highly hydrophobic with a contact angle of 150°. In addition to the significantly increased hydrophobicity, the sheets showed improved mechanical properties, such as a higher tensile strength. Heat treatment of the prepared sheets further enhanced both the mechanical properties and the hydrophobicity. These results demonstrate the flexibility and robustness of the LbL technique, which allows us to combine the known adhesive effect of PAH/PAA LbL films with the functionality of wax nanoparticles, creating a stronger and highly hydrophobic paper.

It was further observed that LbL modified sheets without wax also displayed increased hydrophobicity when heat treated. The mechanism was studied through model experiments where LbL films of PAH/PAA were assembled on flat non-porous model cellulose surfaces. Contact angle measurements showed the same trend due to heat treatment of the model films, although, the absolute value of the contact angles were smaller. Analysis using the highly interfacial sensitive vibrational sum frequency spectroscopy technique showed an enrichment of CH3 groups (from the polymer chain ends) at the solid/air interface. These results indicate that during the heat treatment, a reorientation of polymer chains occurs to minimize the surface energy of the LbL film.

In the second part of this work, the adhesive interactions between the main constituents of wood fibers were studied using high-resolution measuring techniques and well-defined model films of cellulose, hemicellulose and lignin. Successful surface modification of polydimethylsiloxane (PDMS) caps, needed in the Johnson-Kendall-Roberts (JKR) measuring methodology, by LbL deposition of nanofibrillated cellulose (NFC) and poly(ethylene imine) (PEI) allowed for the first known all-wood biopolymer JKR measurements of the adhesion between cellulose/cellulose, cellulose/lignin and the cellulose/glucomannan surfaces. The work of adhesion on loading and the adhesion hysteresis were similar for all three systems, suggesting that adhesion between the different wood biopolymers does not differ greatly.

Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2012. 33 p.
Series
TRITA-CHE-Report, ISSN 1654-1081 ; 2012:8
National Category
Materials Chemistry Paper, Pulp and Fiber Technology Nano Technology
Identifiers
urn:nbn:se:kth:diva-91296 (URN)978-91-7501-268-1 (ISBN)
Presentation
2012-03-19, K1, KTH, Teknikringen 56, Stockholm, 14:00 (English)
Opponent
Supervisors
Note

QC 20120314

Available from: 2012-03-14 Created: 2012-03-12 Last updated: 2014-10-03Bibliographically approved
2. Tailoring Adhesion and Wetting Properties of Cellulose Fibres and Model Surfaces Using Layer-by-Layer Technology
Open this publication in new window or tab >>Tailoring Adhesion and Wetting Properties of Cellulose Fibres and Model Surfaces Using Layer-by-Layer Technology
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:nbn:se:kth:diva-155932 (URN)978-91-7595-347-2 (ISBN)
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

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Larsson, Per A.Wågberg, Lars

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