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  • 1.
    Andrén, Oliver C. J.
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Ingverud, Tobias
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Hult, Daniel
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Håkansson, Joakim
    Bogestål, Yalda
    Caous, Josefin S.
    Blom, Kristina
    Zhang, Yuning
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology.
    Andersson, Therese
    Pedersen, Emma
    Björn, Camilla
    Löwenhielm, Peter
    Malkoch, Michael
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Antibiotic-Free Cationic Dendritic Hydrogels as Surgical-Site-Infection-Inhibiting Coatings2019In: Advanced Healthcare Materials, ISSN 2192-2640, E-ISSN 2192-2659, Vol. 8, no 5Article in journal (Refereed)
    Abstract [en]

    Abstract A non-toxic hydrolytically fast-degradable antibacterial hydrogel is herein presented to preemptively treat surgical site infections during the first crucial 24 h period without relying on conventional antibiotics. The approach capitalizes on a two-component system that form antibacterial hydrogels within 1 min and consist of i) an amine functional linear-dendritic hybrid based on linear poly(ethylene glycol) and dendritic 2,2-bis(hydroxymethyl)propionic acid, and ii) a di-N-hydroxysuccinimide functional poly(ethylene glycol) cross-linker. Broad spectrum antibacterial effect is achieved by multivalent representation of catatonically charged ?-alanine on the dendritic periphery of the linear dendritic component. The hydrogels can be applied readily in an in vivo setting using a two-component syringe delivery system and the mechanical properties can accurately be tuned in the range equivalent to fat tissue and cartilage (G? = 0.5?8 kPa). The antibacterial effect is demonstrated both in vitro toward a range of relevant bacterial strains and in an in vivo mouse model of surgical site infection.

  • 2.
    Andrén, Oliver
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Surface and Corrosion Science. KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Coating Technology.
    Ingverud, Tobias
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Coating Technology.
    Hult, Daniel
    Håkansson, Joakim
    Caous, Josefin
    Zhang, Yuning
    Anderson, Therese
    Pedersen, Emma
    Björn, Camilla
    Löwenhielm, Peter
    Malkoch, Michael
    Linear-Dendritic Polyesters as Antimicrobial HydrogelsManuscript (preprint) (Other academic)
  • 3.
    Carlsson, Linn
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology. KTH, School of Chemical Science and Engineering (CHE), Centres, Wallenberg Wood Science Center.
    Ingverud, Tobias
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology.
    Blomberg, Hanna
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology.
    Carlmark, Anna
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology.
    Larsson, Per Tomas
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology. KTH, School of Chemical Science and Engineering (CHE), Centres, Wallenberg Wood Science Center. Innventia AB, Sweden.
    Malmström, Eva
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology.
    Surface characteristics of cellulose nanoparticles grafted by surface-initiated ring-opening polymerization of epsilon-caprolactone2015In: Cellulose (London), ISSN 0969-0239, E-ISSN 1572-882X, Vol. 22, no 2, p. 1063-1074Article in journal (Refereed)
    Abstract [en]

    In this study, surface-initiated ring-opening polymerization has been employed for the grafting of epsilon-caprolactone from cellulose nanoparticles, made by partial hydrolysis of cellulose cotton linters. A sacrificial initiator was employed during the grafting reactions, to form free polymer in parallel to the grafting reaction. The degree of polymerization of the polymer grafts, and of the free polymer, was varied by varying the reaction time. The aim of this study was to estimate the cellulose nanoparticle degree of surface substitution at different reaction times. This was accomplished by combining measurement results from spectroscopy and chromatography. The prepared cellulose nanoparticles were shown to have 3.1 (+/- 0.3) % of the total anhydroglucose unit content present at the cellulose nanoparticle surfaces. This effectively limits the amount of cellulose that can be targeted by the SI-ROP reactions. For a certain SI-ROP reaction time, it was assumed that the resulting degree of polymerization (DP) of the grafts and the DP of the free polymer were equal. Based on this assumption it was shown that the cellulose nanoparticle surface degree of substitution remained approximately constant (3-7 %) and seemingly independent of SI-ROP reaction time. We believe this work to be an important step towards a deeper understanding of the processes and properties controlling SI-ROP reactions occurring at cellulose surfaces.

  • 4.
    Carlsson, Linn
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Coating Technology. KTH, School of Chemical Science and Engineering (CHE), Centres, Wallenberg Wood Science Center.
    Larsson, Per Tomas
    KTH, School of Chemical Science and Engineering (CHE), Centres, Wallenberg Wood Science Center.
    Ingverud, Tobias
    KTH, School of Chemical Science and Engineering (CHE), Centres, Wallenberg Wood Science Center.
    Blomberg, Hanna
    KTH, School of Chemical Science and Engineering (CHE), Centres, Wallenberg Wood Science Center.
    Carlmark, Anna
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Coating Technology. KTH, School of Chemical Science and Engineering (CHE), Centres, Wallenberg Wood Science Center.
    Malmström, Eva
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Coating Technology. KTH, School of Chemical Science and Engineering (CHE), Centres, Wallenberg Wood Science Center.
    Solid State CP/MAS 13C-NMR investigation of hydrolyzed cotton linters grafted by surface‐initiated ring‐opening polymerization of ε‐caprolactoneManuscript (preprint) (Other academic)
  • 5.
    Erlandsson, Johan
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Fibre Technology.
    Pettersson, Torbjörn
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology. KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Centres, Wallenberg Wood Science Center.
    Ingverud, Tobias
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology. KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Centres, Wallenberg Wood Science Center.
    Granberg, H.
    Larsson, Per A.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology. KTH, School of Engineering Sciences (SCI), Centres, VinnExcellence Center BiMaC Innovation.
    Malkoch, Michael
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Wågberg, Lars
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology. KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Centres, Wallenberg Wood Science Center.
    On the mechanism behind freezing-induced chemical crosslinking in ice-templated cellulose nanofibril aerogels2018In: Journal of Materials Chemistry A, ISSN 2050-7488, Vol. 6, no 40, p. 19371-19380Article in journal (Refereed)
    Abstract [en]

    The underlying mechanism related to freezing-induced crosslinking of aldehyde-containing cellulose nanofibrils (CNFs) has been investigated, and the critical parameters behind this process have been identified. The aldehydes introduced by periodate oxidation allows for formation of hemiacetal bonds between the CNFs provided the fibrils are in sufficiently close contact before the water is removed. This is achieved during the freezing process where the cellulose components are initially separated, and the growth of ice crystals forces the CNFs to come into contact in the thin lamellae between the ice crystals. The crosslinked 3-D structure of the CNFs can subsequently be dried under ambient conditions after solvent exchange and still maintain a remarkably low density of 35 kg m-3, i.e. a porosity greater than 98%. A lower critical amount of aldehydes, 0.6 mmol g-1, was found necessary in order to generate a crosslinked 3-D CNF structure of sufficient strength not to collapse during the ambient drying. The chemical stability of the 3-D structure can be further enhanced by converting the hemiacetals to acetals by treatment with an alcohol under acidic conditions.

  • 6.
    Ingverud, Tobias
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology. KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Centres, Wallenberg Wood Science Center.
    Exploring crosslinked networks of polymers and hybrid cellulose materials2019Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    The field of polymer chemistry has in recent decades had an immense development, resulting in new functional materials with groundbreaking applications. This has been driven partly by strong interdisciplinary alliances between the fields of medicine, biology, chemistry, and materials science. Thermoresponsive block copolymers, have been built for their ability to self-assemble, giving possibility of encapsulation and release of medicine. The dendritic polymer family have been demonstrated as a prime example of highly reactive and interactive functional materials, suitable for biomedical applications. The importance of amines is greatly appreciated in general and especially in polymer chemistry, due to their nucleophilic characteristics in reactions, but also for their ability to interact with other species. There’s also an increase in awareness of standard of living, the effects of climate change and population growth. These are challenges, in need of our outmost focus and knowledge, to direct our path to, towards a more bio based circular economy. This starts, in Sweden, by taking better care of our forest and utilizing its resourceful crop. This thesis seek out spontaneous crosslinking, of various functional polymers, with focus towards hybridizing with nanocellulosic material.

    Initially, interactive permanently charged amine-functional thermoresponsive tri- and star-block copolymers were composed. These were evaluated and used as electrostatic macro-crosslinker of cellulose nanofibrils (CNFs), resulting in thermoresponsive, low dry weight content hydrogels, with notable temperature dependent storage modulus.

    Secondly, reactive and interactive amine-functional dendritic-linear-dendritic (DLD) species were constructed and evaluated in vitro and in vivo. The DLD scaffolds were utilized as fast-degrading, inhibiting surgical site infection (SSIs) antibacterial hydrogel coatings. The crosslinking of the poly(ethylene glycol) (PEG) system was optimized in order to create a two component system, which could be applied with dual syringes. This enabled instantaneous gelation under physiological conditions. The hydrogels moduli could be varied to match various tissues.

    Thirdly, insights and characterizations were provided in the commercial heterofunctional poly(amido amine) carboxylate hyperbranched Helux. Amine post-modifications and intrinsic heterofunctionality alterations of Helux were explored, by increasing the molecular weight and forming Helux self-crosslinked films. Furthermore, two component hydrogels based on Helux and PEG demonstrated curing temperature dependent moduli in the rheometer.

    Finally, utilizing Helux in combination with CNFs to demonstrate the potential to mix on the nanoscale without aggregation. The CNF-Helux could form hydrogels, and wet-stable thermo-crosslinked CNF-Helux composites assemblies such as films and aerogels, with further excess of amines ready for post-modifications of the crosslinked 3D-network.

    The full text will be freely available from 2020-04-16 12:13
  • 7.
    Ingverud, Tobias
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology. KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Centres, Wallenberg Wood Science Center.
    Erlandsson, Johan
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Fibre Technology.
    Wågberg, Lars
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Fibre Technology.
    Malkoch, Michael
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    The combination of a dendritic polyampholyte and cellulose nanofibrils – a new type of functional materialManuscript (preprint) (Other academic)
  • 8.
    Ingverud, Tobias
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology. KTH, School of Chemical Science and Engineering (CHE), Centres, Wallenberg Wood Science Center.
    Larsson, Emma
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology. KTH, School of Engineering Sciences (SCI), Centres, VinnExcellence Center BiMaC Innovation.
    Hemmer, Guillaume
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology.
    Rojas, Ramiro
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology. KTH, School of Chemical Science and Engineering (CHE), Centres, Wallenberg Wood Science Center.
    Malkoch, Michael
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology.
    Carlmark, Anna
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology. KTH, School of Engineering Sciences (SCI), Centres, VinnExcellence Center BiMaC Innovation.
    High water-content thermoresponsive hydrogels via electrostatic macrocrosslinking of cellulose nanofibrils2016In: Journal of Polymer Science Part A: Polymer Chemistry, ISSN 0887-624X, E-ISSN 1099-0518, Vol. 54, no 21, p. 3415-3424Article in journal (Refereed)
    Abstract [en]

    Atom transfer radical polymerization (ATRP) has been utilized to synthesize tri- and star-block copolymers of poly(di(ethylene glycol)methyl ether methacrylate) (PDEGMA) and quaternized poly(2-(dimethylamino)ethyl methacrylate) (qPDMAEMA). The block copolymers, all with a minimum of two cationically charged blocks, were sequentially used for electrostatic macrocrosslinking of a dilute dispersion of anionic TEMPO-oxidized cellulose nanofibrils (CNF, 0.3 wt%), forming free-standing hydrogels. The cationic block copolymers adsorbed irreversibly to the CNF, enabling the formation of ionically crosslinked hydrogels, with a storage modulus of up to 2.9 kPa. The ability of the block copolymers to adsorb to CNF was confirmed by quartz crystal microbalance with dissipation monitoring (QCM-D) and infrared spectroscopy (FT-IR), and the thermoresponsive properties of the hydrogels were investigated by rheological stress and frequency sweep, and gravimetric measurements. This method was shown to be promising for the facile production of thermoresponsive hydrogels based on CNF.

  • 9.
    Ingverud, Tobias
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Malkoch, Michael
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Helux: A heterofunctional hyperbranched poly(amido amine) carboxylateManuscript (preprint) (Other academic)
  • 10.
    Kamada, Ayaka
    et al.
    KTH, School of Engineering Sciences (SCI), Mechanics. KTH, School of Engineering Sciences (SCI), Centres, Linné Flow Center, FLOW.
    Mittal, Nitesh
    KTH, School of Engineering Sciences (SCI), Mechanics. KTH, School of Chemical Science and Engineering (CHE), Centres, Wallenberg Wood Science Center. KTH, School of Engineering Sciences (SCI), Centres, Linné Flow Center, FLOW.
    Söderberg, L. Daniel
    KTH, School of Engineering Sciences (SCI), Mechanics. KTH, School of Engineering Sciences (SCI), Centres, Linné Flow Center, FLOW. KTH, School of Chemical Science and Engineering (CHE), Centres, Wallenberg Wood Science Center.
    Ingverud, Tobias
    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.
    Ohm, Wiebke
    Roth, Stephan V.
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology. Photon Science, Deutsches Elektronen-Synchrotron (DESY), D-22607 Hamburg, Germany.
    Lundell, Fredrik
    KTH, School of Chemical Science and Engineering (CHE), Centres, Wallenberg Wood Science Center. KTH, School of Engineering Sciences (SCI), Centres, Linné Flow Center, FLOW. KTH, School of Engineering Sciences (SCI), Mechanics.
    Lendel, Christofer
    KTH, School of Chemical Science and Engineering (CHE), Chemistry.
    Flow-assisted assembly of nanostructured protein microfibers2017In: Proceedings of the National Academy of Sciences of the United States of America, ISSN 0027-8424, E-ISSN 1091-6490, Vol. 114, no 6, p. 1232-1237Article in journal (Refereed)
    Abstract [en]

    Some of the most remarkable materials in nature are made from proteins. The properties of these materials are closely connected to the hierarchical assembly of the protein building blocks. In this perspective, amyloid-like protein nanofibrils (PNFs) have emerged as a promising foundation for the synthesis of novel bio-based materials for a variety of applications. Whereas recent advances have revealed the molecular structure of PNFs, the mechanisms associated with fibril-fibril interactions and their assembly into macroscale structures remain largely unexplored. Here, we show that whey PNFs can be assembled into microfibers using a flow-focusing approach and without the addition of plasticizers or cross-linkers. Microfocus small-angle X-ray scattering allows us to monitor the fibril orientation in the microchannel and compare the assembly processes of PNFs of distinct morphologies. We find that the strongest fiber is obtained with a sufficient balance between ordered nanostructure and fibril entanglement. The results provide insights in the behavior of protein nanostructures under laminar flow conditions and their assembly mechanism into hierarchical macroscopic structures.

  • 11.
    Larsson, Emma
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Coating Technology. KTH, School of Engineering Sciences (SCI), Centres, VinnExcellence Center BiMaC Innovation.
    Ingverud, Tobias
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Coating Technology. KTH, School of Chemical Science and Engineering (CHE), Centres, Wallenberg Wood Science Center.
    Hemmer, Guillaume
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Coating Technology.
    Rojas, Ramiro
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Coating Technology. KTH, School of Chemical Science and Engineering (CHE), Centres, Wallenberg Wood Science Center.
    Malkoch, Michael
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Coating Technology.
    Carlmark, Anna
    KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Coating Technology. KTH, School of Engineering Sciences (SCI), Centres, VinnExcellence Center BiMaC Innovation. KTH, School of Chemical Science and Engineering (CHE), Centres, Wallenberg Wood Science Center.
    Thermoresponsive hydrogels of cellulose nanofibrils and triblock copolymersManuscript (preprint) (Other academic)
    Abstract [en]

    Atom transfer radical polymerization (ATRP) has been utilized to synthesize triblock and star-block copolymers of quaternized poly(2-(dimethylamino)ethyl methacrylate) (qPDMAEMA) and poly(di(ethylene glycol) methyl ether methacrylate (PDEGMA). The block copolymers, that all contained a minimum of two charged blocks, were sequential adsorbed to negatively charged cellulose nanofibrils (CNF) in dilute water suspension, forming thermoresponsive hydrogels. The presence of more than one charge block allowed for the polymers to form permanent, physically crosslinked, gels when adsorbed to the CNF. The ability of the polymers to adsorb to CNF was confirmed by quartz crystal microbalance with dissipation monitoring (QCM-D), and the thermoresponsive properties of the gels were investigated by rheological measurements and gravimetric measurements. This method was shown to be promising for the facile, production of thermoresponsive hydrogels composed of CNF.

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