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Robust and Tailored Wet Adhesion in Biopolymer Thin Films
KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Fibre Technology.ORCID iD: 0000-0002-5444-7276
KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Fibre Technology.
KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Fibre Technology.
KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Fibre Technology.
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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.

Place, publisher, year, edition, pages
2014. Vol. 15, no 12, 4420-4428 p.
Keyword [en]
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
URN: urn:nbn:se:kth:diva-155931DOI: 10.1021/bm501202sISI: 000346114400005PubMedID: 25333327ScopusID: 2-s2.0-84916624800OAI: diva2:763481

QC 20150108

Available from: 2014-11-14 Created: 2014-11-14 Last updated: 2015-01-08Bibliographically approved
In thesis
1. 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.
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
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)

QC 20141117

Available from: 2014-11-17 Created: 2014-11-14 Last updated: 2014-11-17Bibliographically approved

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