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Bifunctional Dendronized Cellulose Surfaces as Biosensors
KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology. KTH, School of Engineering Sciences (SCI), Centres, VinnExcellence Center BiMaC Innovation.
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.
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2011 (English)In: Biomacromolecules, ISSN 1525-7797, E-ISSN 1526-4602, Vol. 12, no 6, 2114-2125 p.Article in journal (Refereed) Published
Abstract [en]

Well-defined dendronized cellulose substrates displaying multiple representations of dual-functionality were constructed by taking advantage of the efficiency of the click reaction combined with traditional anhydride chemistry. First, activated cellulose surfaces were decorated with several generations of dendrons, and their peripheral reactive groups were subsequently reacted with a trifunctional orthogonal monomer. The generated substrate tool box was successfully explored by accurately tuning the surface function using a versatile orthogonal dual postfunctionalization approach. In general, the reactions were monitored by using a click-dye reagent or a quartz crystal microbalance (QCM) technique, and the resulting surfaces were well-characterized using XPS, and contact angle measurements. Utilizing this approach two different surfaces have been obtained; that is, triethylenglycol oligomers and amoxicillin molecules were efficiently introduced to the dendritic surface. As a second example, mannose-decorated hydroxyl functional surfaces illustrated their potential as biosensors by multivalent detection of lectin protein at concentration as low as 5 nM.

Place, publisher, year, edition, pages
2011. Vol. 12, no 6, 2114-2125 p.
Keyword [en]
CLICK-CHEMISTRY, EFFICIENT SYNTHESIS, FUTURE-DIRECTIONS, DENDRIMERS, AZIDE, FILMS
National Category
Chemical Sciences
Identifiers
URN: urn:nbn:se:kth:diva-35633DOI: 10.1021/bm200201yISI: 000291499900019Scopus ID: 2-s2.0-79958779836OAI: oai:DiVA.org:kth-35633DiVA: diva2:429232
Funder
Swedish Research Council, 2006-3617Swedish Research Council, 2009-3259
Note
QC 20110704Available from: 2011-07-04 Created: 2011-07-04 Last updated: 2017-12-11Bibliographically approved
In thesis
1. Surface Modification of Cellulose-based Materials for Tailoring of Interfacial Interactions
Open this publication in new window or tab >>Surface Modification of Cellulose-based Materials for Tailoring of Interfacial Interactions
2012 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The awareness of our need for a sustainable society has encouraged the search for renewable, high quality materials that can replace oil-based products. This, in combination with increased competition in the forest industry, has stimulated a lot of research into different types of wood-based materials where cellulose-rich fibers are combined with different types of polymers. There is hence a great need to develop efficient fiber modification techniques by which the fibers can be tailored to obtain specific properties. A significant change in properties can be achieved by modifying only the surface of fibers although only a relatively small amount of the total fiber material is modified. In this thesis, several surface modification techniques are presented as new tools to design the properties of different cellulose-based materials.

In paper I, thermoresponsive nanocomposites have been assembled from specially designed thermoresponsive block copolymers and nanofibrillated cellulose. The block copolymers have one thermoresponsive block and one cationically charged block which can thus attach the polymer to an oppositely charged fiber/fibril surface. Multilayers were assembled with these block copolymers and nanofibrillated cellulose (NFC) utilizing the Layer-by-Layer (LbL) technique, resulting in thin films with a thermoresponsive behavior.

In papers II and III, amphiphilic block copolymers with one less polar high molecular weight block and one cationic block were synthesized for use as a compatibilizer between fibers/fibrils and less polar polymer matrices in composites. The less polar block consisted of polystyrene (PS) in paper II and poly(ɛ-caprolactone) (PCL) in paper III. These polymers self-assemble into cationic micelles in water which can adsorb to oppositely charged surfaces, such as cellulose-based fibers/fibrils, in water under mild conditions and decrease the surface energy of the surface. Atomic force microscopy (AFM) was used to evaluate the adhesive properties of surfaces treated with these compatibilizers which clearly showed the formation of physical entanglements across the interfaces, which are essential for improved interfacial adhesion in the final composites. This modification technique could probably be utilized to make fiber-based composites with better mechanical properties. To be able to better compare this physical modification technique with a more traditional covalent grafting-from approach a method to measure attached amounts of grafted PCL onto cellulose model surfaces was developed in paper IV using a quartz crystal microbalance (QCM).

In paper V, multilayers of poly(allylamine hydrochloride) (PAH) and hyaluronic acid (HA) were assembled using the LbL technique and surface structure, build-up and adhesive behavior of the multilayers were evaluated. AFM force measurements showed that a significant adhesion even at long separation distances between two surfaces treated with PAH/HA multilayers could be achieved due to extensive interdiffusion across the interface during contact, leading to significant disentanglement during separation. Fundamental parameters contributing to improved adhesion for this type of system have been evaluated and this knowledge could be used to improve cellulose-based fiber networks and possibly also other types of cellulose-based materials.

In paper VI, click chemistry was used to covalently attach dendrons to cellulose surfaces and further modify them with mannose groups to obtain specific interactions with Concanavalin A. The protein interactions were studied at different protein concentrations with a QCM. The multivalent dendronized surface showed a 10-fold increase in sensitivity to the protein compared to a monovalent reference surface demonstrating greatly improved interfacial interactions. This approach could be used to improve interactions at different types of interfaces.

Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2012. viii, 53 p.
Series
Trita-CHE-Report, ISSN 1654-1081 ; 2012:37
National Category
Chemical Sciences Materials Chemistry Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-102368 (URN)978-91-7501-462-3 (ISBN)
Public defence
2012-10-05, F3, Lindstedtsvägen 26, KTH, Stockholm, 13:00 (English)
Opponent
Supervisors
Note

QC 20120918

Available from: 2012-09-18 Created: 2012-09-14 Last updated: 2012-09-18Bibliographically approved
2. Multifunctional Dendritic Scaffolds: Synthesis, Characterization and Potential applications
Open this publication in new window or tab >>Multifunctional Dendritic Scaffolds: Synthesis, Characterization and Potential applications
2013 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The development of materials for advanced applications requires innovative macromolecules with well-defined structures and the inherent ability to be tailored in a straightforward manner. Dendrimers, being a subgroup of the dendritic polymer family, possess properties which fulfill such demands. They have a highly branched architecture with a high number of functional groups and are one of the most well-defined types of macromolecules ever synthesized. However, despite their well-defined nature and high functional density, traditional dendrimers commonly lack diverse chemical functionalities. Therefore, this thesis focuses on the synthesis of more complex dendritic materials to extend their tailoring capacity by introduction of dualfunctionalities for multipurpose actions. It covers the synthesis of dualfunctional dendrimers, dendritic modification of linear poly(ethylene glycol) polymers and cellulose surfaces, and the synthesis of linear dendritic hybrids. The building blocks enabling this synthesis, AB2C monomers, were also developed during this work. The orthogonal nature between click groups (azide, alkyne and alkene) and hydroxyl groups have efficiently been utilized for postfunctionalization by robust click chemistry and traditional esterification reactions. Furthermore, linear dendritic hybrids were synthesized, merging the properties of linear and dendritic macromolecules. The dendritic frameworks were tailored towards the production of bone fracture adhesives, novel biofunctional dendritic hydrogels, biosensors and micellar drug delivery vehicles.

Abstract [sv]

Utveckling av material för avancerade applikationer kräver innovativa makromolekyler med väldefinierade strukturer och som kan skräddarsys på ett enkelt sätt. Dendrimerer är en undergrupp av dendritiska polymerer vars egenskaper uppfyller dessa krav. De har en mycket förgrenad arkitektur med många funktionella grupper och är en av de mest väldefinierade befintliga syntetiska makromolekylerna. Trots dess väldefinierade karaktär och höga funktionalitet saknar ofta traditionella dendrimerer multipla kemiska funktionaliteter. Denna avhandling fokuserar därför på syntesen av mer komplexa dendritiska material för att förbättra deras kapacitet att skräddarsys, detta görs genom att introducera fler funktionaliteter som kan utnyttjas för multipla ändamål . Avhandlingen redogör för syntesen av difunktionella dendrimerer, dendritiska modifikationer av polyetylenglykol och cellulosaytor samt syntes av traditionella dendritiska hybrider. Byggstenarna som möjliggör syntesen, AB2C monomerer, framställdes också under detta arbete. Den ortogonala karaktären mellan klick grupper (azid, alkyn och alkene) och hydroxylgrupper har utnyttjats effektivt för funktionaliseringar genom användande av robust ”Click”-kemi och traditionella esterifikationsreaktioner. Vidare tillverkades de linjära dendritiska hybrider för att kombinera egenskaperna hos både linjära och traditionella dendritiska polymerer i en och samma makromolekyl. Samtliga dendritiska strukturer skräddarsyddes för applikationer så som benlimmer, biofunktionella dendritiska hydrogeler, biosensorer och läkemedels-bärande miceller.

Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2013. 87 p.
Series
Trita-CHE-Report, ISSN 1654-1081 ; 2013:32
Keyword
Dendrimer, AB2C monomer, Click chemistry, CuAAC, thiol-ene coupling chemistry, TEC, linear dendritic hybrids, micelle, hydrogel, bone adhesive
National Category
Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-127429 (URN)978-91-7501-817-1 (ISBN)
Public defence
2013-09-20, Sal F3, Lindstedtsvägen 26, KTH, Stockholm, 10:00 (English)
Opponent
Supervisors
Note

QC 20130830

Available from: 2013-08-30 Created: 2013-08-29 Last updated: 2013-08-30Bibliographically approved

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Malmström, EvaWågberg, LarsHult, AndersMalkoch, Michael

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