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Superhydrophobic Bio-fibre Surfaces via Tailored Grafting Architecture
KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology.
KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology.
KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology.
KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology.ORCID iD: 0000-0002-9372-0829
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2006 (English)In: Chemical Communications, ISSN 1359-7345, E-ISSN 1364-548X, no 34, 3594-3596 p.Article in journal (Refereed) Published
Abstract [en]

Superhydrophobic bio-fibre surfaces with a micro-nano-binary surface structure have been achieved via the surface-confined grafting of glycidyl methacrylate, using a branched "graft-on-graft'' architecture, followed by post-functionalisation to obtain fluorinated brushes.

Place, publisher, year, edition, pages
2006. no 34, 3594-3596 p.
Keyword [en]
glycidylmethacrylate; methacrylic acid derivative; unclassified drug; article; chemical analysis; chemical structure; fiber; fluorination; hydrophobicity; nanotechnology; surface property; Cellulose; Fluorocarbon Polymers; Hydrophobicity; Molecular Structure; Polymethacrylic Acids; Surface Properties
National Category
Polymer Chemistry
Identifiers
URN: urn:nbn:se:kth:diva-8369DOI: 10.1039/b607411aISI: 000239937600006Scopus ID: 2-s2.0-33747616433OAI: oai:DiVA.org:kth-8369DiVA: diva2:13673
Note
QC 20100805Available from: 2008-05-08 Created: 2008-05-08 Last updated: 2010-10-25Bibliographically approved
In thesis
1. From Responsive Interfaces to Honeycomb Membranes by Controlled Radical Polymerisation
Open this publication in new window or tab >>From Responsive Interfaces to Honeycomb Membranes by Controlled Radical Polymerisation
2008 (English)Doctoral thesis, comprehensive summary (Other scientific)
Abstract [en]

In this study, surface modification of both organic and inorganic substrates (in terms of cellulose and silica nanoparticles, respectively) has been explored using surface-initiated atom transfer radical polymerisation (ATRP).

The desire to modify bio-based materials to fit into new application areas and the need for bio-based materials with improved material properties is steadily increasing due to environmental concern.

Superhydrophobic and self-cleaning cellulose surfaces were fabricated by combining ATRP with post-functionalisation. Glycidyl methacrylate was grafted from filter paper, and the epoxide groups were used as reactive handles to create a branched “graft-on-graft” architecture. Post-functionalisation of this architecture with perfluorinated chains or alkyl chains resulted in the formation of superhydrophobic surfaces.

Grafting of N-isopropylacrylamide (NIPAAm) from filter paper yielded cellulose surfaces capable of switching the wettability, from hydrophilic to hydrophobic, in response to changes in temperature. The wettability of cellulose surfaces grafted with poly(4-vinylpyridine) (P4VP) could be adjusted from hydrophilic to hydrophobic by changing pH. Furthermore, cellulose surfaces responding to changes in both pH and temperature were obtained via grafting of block copolymers of PNIPAAm and P4VP.

The use of inorganic nano-particles in composites has attracted considerable academic and industrial interest due to their excellent mechanical and thermal properties. Styrene was grafted from the surface of silica nanoparticles using ATRP. The resulting organic-inorganic hybrid materials did not aggregate to the same extent as the un-modified silica particles.

The polystyrene-modified silica particles were used for the fabrication of honeycomb membranes. It was evident that the pore sizes and the number of porous layers could be tuned by varying the conditions used for film casting. To broaden the range of polymers available for film casting into honeycomb membranes, a block copolymer of polystyrene and poly(methyl methacrylate) was grafted from silica nanoparticles. Polymer-blends of polystyrene-modified particles and poly(9,9´-dihexylfluorene) (PDHF) were also used as an alternative to incorporate functionality into honeycomb membranes.

Place, publisher, year, edition, pages
Stockholm: KTH, 2008. 67 p.
Series
Trita-CHE-Report, ISSN 1654-1081 ; 2008:37
Keyword
Isoporous membranes, Silica nanoparticles, ATRP, Functional surfaces, cellulose
National Category
Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-4733 (URN)978-91-7178-982-2 (ISBN)
Public defence
2008-05-29, F3, Lindstedtväg 26, Stockholm, 10:00
Opponent
Supervisors
Note
QC 20100901Available from: 2008-05-08 Created: 2008-05-08 Last updated: 2010-09-01Bibliographically approved
2. Tailoring Surface Properties of Bio-Fibers via Atom Transfer Radical Polymerization
Open this publication in new window or tab >>Tailoring Surface Properties of Bio-Fibers via Atom Transfer Radical Polymerization
2007 (English)Doctoral thesis, comprehensive summary (Other scientific)
Abstract [en]

The potential use of renewable, bio-based polymers in high-technological applications has attracted great interest due to increased environmental concern. Cellulose is the most abundant biopolymer resource in the world, and it has great potential to be modified to suit new application areas. The development of controlled polymerization techniques, such as atom transfer radical polymerization (ATRP), has made it possible to graft well-defined polymers from cellulose surfaces. In this study, graft-modification of cellulose substrates by ATRP was explored as a tool for tailoring surface properties and for the fabrication of functional cellulose surfaces.

Various native and regenerated cellulose substrates were successfully graft-modified to investigate the effect of surface morphology on the grafting reactions. It was found that significantly denser polymer brushes were grafted from the native than from the regenerated cellulose substrates, most likely due to differences in surface area.

A method for detaching the grafted polymer from the substrate was developed, based on the selective cleavage of silyl ether bonds with tetrabutylammonium fluoride. The results from the performed kinetic study suggest that the surface-initiated polymerization of methyl methacrylate from cellulose proceeds faster than the concurrent solution polymerization at low monomer conversions, but slows down to match the kinetics of the solution polymerization at higher conversions.

Superhydrophobic and self-cleaning bio-fiber surfaces were obtained by grafting of glycidyl methacrylate using a branched graft-on-graft architecture, followed by post-functionalization to obtain fluorinated polymer brushes. AFM analysis showed that the surface had a micro-nano-binary structure. It was also found that superhydrophobic surfaces could be achieved by post-functionalization with an alkyl chain, with no use of fluorine.

Thermo-responsive cellulose surfaces have been prepared by graft-modification with the stimuli responsive polymer poly(N-isopropylacrylamide) (PNIPAAm). Brushes of poly(4-vinylpyridine) (P4VP) rendered a pH-responsive cellulose surface. Dual-responsive cellulose surfaces were achieved by grafting block-copolymers of PNIPAAm and P4VP.

Place, publisher, year, edition, pages
Stockholm: KTH, 2007. 56 p.
Series
Trita-CHE-Report, ISSN 1654-1081 ; 2007:16
Keyword
cellulose, bio-fiber, atom transfer radical polymerization, surface modification, grafting, polymer brushes, functional surfaces, superhydrophobic, stimuli-responsive
National Category
Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-4325 (URN)978-91-7178-616-6 (ISBN)
Public defence
2007-04-20, D3, Lindstedtsvägen 5, Stockholm, 10:00
Opponent
Supervisors
Note
QC 20100804Available from: 2007-04-10 Created: 2007-04-10 Last updated: 2010-08-05Bibliographically approved
3. Tuning Properties of Surfaces and Nanoscopic Objects using Dendronization and Controlled Polymerizations
Open this publication in new window or tab >>Tuning Properties of Surfaces and Nanoscopic Objects using Dendronization and Controlled Polymerizations
2007 (English)Doctoral thesis, comprehensive summary (Other scientific)
Abstract [en]

In this study, dendronization and grafting via controlled polymerization techniques, atom transfer radical polymerization (ATRP) and ring-opening polymerization (ROP), have been explored. Modification of surfaces and cellulose using these techniques, which enable grafting of well-defined polymer architectures, has been investigated. The interest in using cellulose stems from its renewability, biocompatibility, high molecular weight, and versatile functionalization possibilities.

Dendronization was performed using disulfide-cored didendrons of 2,2-bis(methylol)propionic acid (bis-MPA) on gold surfaces, for the formation of self-assembled monolayers. It was found that the height of the monolayer increased with increasing dendron generation and that the end-group functionality controlled the wettability of the modified surface.

Superhydrophobic cellulose surfaces could be obtained when a ‘graft-on-graft’ architecture was obtained using ATRP from filter paper after subsequent post-functionalized using a perfluorinated compound. The low wettability could be explained by a combination of a high surface roughness and the chemical composition.

Biobased dendronized polymers were synthesized through the ‘attach to’ route employing dendronization of soluble cellulose, in the form of hydroxypropyl cellulose (HPC). The dendronized polymers were studied as nanosized objects using atomic force microscopy (AFM) and it was found that the dendron end-group functionality had a large effect on the molecular conformation on surfaces of spun cast molecules.

ATRP of vinyl monomers was conducted from an initiator-functionalized HPC and an initiator-functionalized first generation dendron, which was attached to HPC. The produced comb polymers showed high molecular weight and their sizes could be estimated via AFM of spun cast molecules on mica and from dynamic light scattering in solution, to around 100-200 nm. The comb polymers formed isoporous membranes, exhibiting pores of a few micrometers, when drop cast from a volatile solvent in a humid environment. HPC was also used to initiate ROP of ε-caprolactone, which was chain extended using ATRP to achieve amphiphilic comb block copolymers. These polymers could be suspended in water, cross-linked and were able to solubilize a hydrophobic compound.

Place, publisher, year, edition, pages
Stockholm: KTH, 2007. 70 p.
Series
Trita-CHE-Report, ISSN 1654-1081 ; 2007:83
Keyword
Dendrimers, dendronized polymers, cellulose, Atom Transfer Radical Polymerization, Ring-Opening Polymerization, surface modification, grafting, superhydrophobic, amphiphilic polymer, block copolymer, Atomic Force Microscopy
National Category
Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-4550 (URN)978-91-7178-820-7 (ISBN)
Public defence
2007-12-14, D3, Huvudbyggnaden, Lindstedtsvägen 5, Stockholm, 14:00
Opponent
Supervisors
Note
QC 20100826Available from: 2007-11-23 Created: 2007-11-23 Last updated: 2010-08-26Bibliographically approved

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