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From Responsive Interfaces to Honeycomb Membranes by Controlled Radical Polymerisation
KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology.
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 [en]
Isoporous membranes, Silica nanoparticles, ATRP, Functional surfaces, cellulose
National Category
Polymer Chemistry
Identifiers
URN: urn:nbn:se:kth:diva-4733ISBN: 978-91-7178-982-2 (print)OAI: oai:DiVA.org:kth-4733DiVA: diva2:13679
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
List of papers
1. Superhydrophobic Bio-fibre Surfaces via Tailored Grafting Architecture
Open this publication in new window or tab >>Superhydrophobic Bio-fibre Surfaces via Tailored Grafting Architecture
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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.

Keyword
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:nbn:se:kth:diva-8369 (URN)10.1039/b607411a (DOI)000239937600006 ()2-s2.0-33747616433 (Scopus ID)
Note
QC 20100805Available from: 2008-05-08 Created: 2008-05-08 Last updated: 2017-12-14Bibliographically approved
2. Bouncing Water Droplets on Superhydrophobic Cellulose Surfaces
Open this publication in new window or tab >>Bouncing Water Droplets on Superhydrophobic Cellulose Surfaces
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(English)In: Journal of Materials Chemistry, ISSN 0959-9428, E-ISSN 1364-5501Article in journal (Other academic) Submitted
National Category
Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-8370 (URN)
Note
QC 20100901Available from: 2008-05-08 Created: 2008-05-08 Last updated: 2017-12-14Bibliographically approved
3. Intelligent Dual-Responsive Cellulose Surfaces via Surface-Initiated ATRP
Open this publication in new window or tab >>Intelligent Dual-Responsive Cellulose Surfaces via Surface-Initiated ATRP
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2008 (English)In: Biomacromolecules, ISSN 1525-7797, E-ISSN 1526-4602, Vol. 9, no 8, 2139-2145 p.Article in journal (Refereed) Published
Abstract [en]

Novel thermo-responsive cellulose (filter paper) surfaces of N-isopropylacrylamide (NIPAAm) and pH-responsive cellulose surfaces of 4-vinylpyridine (4VP) have been achieved via surface-initiated ATRP. Dual-responsive (pH and temperature) cellulose surfaces were also obtained through the synthesis of block-copolymer brushes of PNIPAAm and P4VP. With changes in pH and temperature, these "intelligent" surfaces showed a reversible response to both individual triggers, as indicated by the changes in wettability from highly hydrophilic to highly hydrophobic observed by water contact angle measurements. Adjusting the composition of the grafted block-copolymer brushes allowed for further tuning of the wettability of these "intelligent" cellulose surfaces.

Keyword
Acrylic monomers; Amides; Angle measurement; Atom transfer radical polymerization; Brushes; Cellulose; Contact angle; Copolymerization; Nanostructured materials; Plastic products; Polymers; 4-vinylpyridine; Block co polymers; Cellulose surfaces; Filter papers; N-Isopropylacrylamide; pH-responsive; PNIPAAm; Surface-initiated ATRP; Water contact angle; Acrylamides; Acrylic Resins; Biocompatible Materials; Cellulose; Copper; Filtration; Hydrogen-Ion Concentration; Hydrolysis; Polymers; Pyridines; Spectrophotometry, Infrared; Spectroscopy, Fourier Transform Infrared; Surface Properties; Temperature; Wettability
National Category
Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-8371 (URN)10.1021/bm800193n (DOI)000258400200008 ()18636775 (PubMedID)2-s2.0-52649118631 (Scopus ID)
Note
QC 20100805. Uppdaterad från In press till Published 20100805.Available from: 2008-05-08 Created: 2008-05-08 Last updated: 2017-12-14Bibliographically approved
4. Highly-ordered hybrid organic-inorganic isoporous membranes from polymer modified nanoparticles
Open this publication in new window or tab >>Highly-ordered hybrid organic-inorganic isoporous membranes from polymer modified nanoparticles
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2005 (English)In: Macromolecular rapid communications, ISSN 1022-1336, E-ISSN 1521-3927, Vol. 26, no 7, 524-528 p.Article in journal (Refereed) Published
Abstract [en]

Organic-inorganic hybrid materials consisting of nanosized silica particles with surface grafted PS or PS-b-PMMA were synthesized using ATRP. These hybrid materials were used in the fabrication of highly-ordered isoporous membranes. Optical characterization revealed that the membranes consisted of hexagonally ordered pores of uniform size. The combination of an open pore structure and high surface area makes isoporous membranes into materials of high interest in fields as biotechnology and photonics.

Keyword
atomic force microscopy (AFM), atom transfer radical polymerization (ATRP), block copolymers, self-assembly, silica nanoparticles
National Category
Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-8372 (URN)10.1002/marc.200400617 (DOI)000228436600004 ()2-s2.0-20444470076 (Scopus ID)
Note
QC 20100901Available from: 2008-05-08 Created: 2008-05-08 Last updated: 2017-12-14Bibliographically approved
5. Self-assembly of poly(9,9 '-dihexylfluorene) to form highly ordered isoporous films via blending
Open this publication in new window or tab >>Self-assembly of poly(9,9 '-dihexylfluorene) to form highly ordered isoporous films via blending
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2006 (English)In: Langmuir, ISSN 0743-7463, E-ISSN 1520-5827, Vol. 22, no 9, 3959-3961 p.Article in journal (Refereed) Published
Abstract [en]

Highly ordered hexagonal arrays of isoporous films prepared from poly(9,9'-dihexylfluorene) and polystyrene-grafted silica nanoparticles (Si-graft-PS) are presented. These close-packed arrays were formed in areas of many square millimeters. The pore size varied from 3.6 to 8.5 mu m, depending on the concentration of Si-graft-PS and the processing conditions. Solid-state photoluminescence resulted in a significant red shift of up to 30 nm in these films compared to that in conventional processing techniques. These differences are attributed to enhanced aggregation of the polymers caused by polymer-solvent interactions. These highly ordered polymer films may find use in microelectronic and biological and/or chemical sensor applications.

Keyword
Biosensors, Blending, Chemical sensors, Grafting (chemical), Nanostructured materials, Photoluminescence, Polystyrenes, Self assembly, Silica, Polymer films, Polymer-solvent interactions
National Category
Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-8373 (URN)10.1021/la053025q (DOI)000236989300003 ()2-s2.0-33646442760 (Scopus ID)
Note
QC 20100901Available from: 2008-05-08 Created: 2008-05-08 Last updated: 2017-12-14Bibliographically approved
6. Honeycomb Patterned Membranes from Polymer Modified Silica Nanoparticles
Open this publication in new window or tab >>Honeycomb Patterned Membranes from Polymer Modified Silica Nanoparticles
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(English)Manuscript (Other academic)
Keyword
AFM, SEM, ATRP, honeycomb membranes, self-assembly, silica nanoparticles
National Category
Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-8374 (URN)
Note
QC 20100901Available from: 2008-05-08 Created: 2008-05-08 Last updated: 2010-09-01Bibliographically approved

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