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  • 1.
    Arseneault, Mathieu
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Granskog, Viktor
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Khosravi, Sara
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Heckler, Ilona
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Mesa-Antunez, Pablo
    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.
    Zhang, Yuning
    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.
    Highly crosslinked triazine-trione materials for fracture fixation based on TEC and TYC chemistryManuscript (preprint) (Other academic)
  • 2.
    Cobo Sanchez, Carmen
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Inorganic and organic polymer-grafted nanoparticles: their nanocomposites and characterization2018Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    Nanocomposites (NCs) have been widely studied in the past decades due to the promising properties that nanoparticles (NPs) offer to a polymer matrix, such as increased thermal stability and non-linear electrical resistivity. It has also been shown that the interphase between the two components is the key to achieving the desired improvements. In addition, polymer matrices are often hydrophobic while NPs are generally hydrophilic, leading to NP aggregation. To overcome these challenges, NPs can be surface-modified by adding specific molecules and polymers. In the present work, a range of organic and inorganic NPs have been surface-modified with polymers synthesized by atom transfer radical polymerization (ATRP) or surface-initiated ATRP (SI-ATRP).Cellulose nanofibrils (CNF) and cellulose nanocrystals (CNC) are highly crystalline NPs that can potentially increase the Young’s modulus of the NC. In this study, a matrix-free NC was prepared by physisorption of a block-copolymer containing a positively charged (quaternized poly(2-(dimethylamino)ethyl methacrylate), qPDMAEMA) and a thermo-responsive (poly di(ethylene glycol) methyl ether methacrylate, PDEGMA). The modified CNF exhibited a thermo-responsive, reversible behavior. CNCs were polymer-modified either via SI-ATRP or physisorbed with poly (butyl methacrylate) (PBMA) to improve the dispersion and interphase between them and a polycaprolactone (PCL) matrix during extrusion. The mechanical properties of the NCs containing CNC modified via SI-ATRP were superior to the reference and unmodified materials, even at a high relative humidity.Reduced graphene oxide (rGO) and aluminum oxide (Al2O3) are interesting for electrical and electronic applications. However, the matrices used for these applications, such as poly(ethylene-co-butyl acrylate) (EBA) and low density polyethylene (LDPE) are mainly hydrophobic, while the NPs are hydrophilic. rGO was modified via SI-ATRP using different chain lengths of PBMA and subsequently mixed with an EBA matrix. Al2O3 was modified with two lengths of poly(lauryl methacrylate) (PLMA), and added to LDPE prior to extrusion. Agglomeration and dispersion of the NCs were dependent on the lengths and miscibilities of the grafted polymers and the matrices. rGO-EBA NCs showed non-linear direct current (DC) resistivity upon modification, as the NP dispersion improved with increasing PBMA length. Al2O3-LDPE systems improved the mechanical properties of the NCs when low amounts of NPs (0.5 to 1 wt%) were added, while decreasing power dissipation on the material.Finally, PLMA-grafted NPs with high polymer quantities and two grafting densities in Al2O3 and silicon oxide (SiO2) nanoparticles were synthesized by de-attaching some of the silane groups from the surfaces, either by hydrolysis or by a mild tetrabutylammonium fluoride (TBAF) cleavage. These compounds were characterized and compared to the bulk PLMA, and were found to have very interesting thermal properties.

    The full text will be freely available from 2020-04-24 14:42
  • 3.
    Engström, Joakim
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Centres, Wallenberg Wood Science Center. KTH, Superseded Departments (pre-2005), Fibre and Polymer Technology. KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Tailored adhesion of PISA-latexes for cellulose modification and new materials2019Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    This thesis is focused on applying modification chemistry to already known cellulosic substrates from wood (i.e. cellulose nanofibrils, CNFs, and cellulose nanocrystals, CNCs). The modification is needed to overcome the drawbacks with the nanocellulosics alone, such as sensitivity to water (hydrophilicity) and the brittle material properties (however great stiffness). The first aim is to incorporate nanocellulosics into hydrophobic degradable materials of poly(ε-caprolactone) (PCL), resulting in aggregation if not modified. The challenge is to reach high fraction of nanocellulosics, whilst maintaining the flexibility of PCL and improving the properties of the resulting nanocomposite with the corresponding stiffness of the nanocellulosics. The second aim is to increase toughness and strain-at-break for nanocomposite materials of CNF-networks, to increase the plastic deformation equivalent of fossil-based polymeric materials such as polypropylene (PP). Aiming to achieve these goals, the thesis also includes new synthetic strategies of tailored-made set of block copolymers as modifying components. The modifying components, were synthesised by surfactant-free emulsion polymerisation and polymerisation induced self-assembly (PISA), so called PISA-latexes.

    Two types of cationic polyelectrolytes, (poly(2-dimethylaminoethy methacrylate) (PDMAEMA) and poly(N-[3-(dimethylamino)propyl] methacrylamide (PDMAPMA)), being the corona of the latex, were synthesised. Followed by chain-extension with different hydrophobic monomers such as methyl methacrylate and butyl methacrylate, making up the core polymer of the resulting PISA-latex. The cationic PISA-latexes show narrow size distributions and the glass transition (Tg) of the core polymer can be varied between -40 °C to 150 °C. The PISA-latexes show strong adhesion to silica and cellulose surfaces as assessed by quartz crystal microbalance (QCM-D). Results also indicate that latexes with Tg below room temperature, considered soft, behave different in the wet state than latexes with Tg above room temperature, considered rigid. The softer latexes form clusters (visualised by imaging with microscopy and atomic force measurements (AFM)) and undergo film formation in the wet state. The latter, shown by colloidal probe measurements using AFM resulting in very large work of adhesion and pull-off forces.

    The PISA-latexes compatibilize CNCs and different CNFs with PCL as a matrix polymer, observed by a small increase in stiffness for the final nanocomposites, however not at a level expected by rule-of-mixtures. The promising wet feeding technique results in large increase in stiffness but maintain PCL’s flexibility, above 200% strain-at-break, which is rarely observed for CNF-reinforced nanocomposites. The, in this case, rigid latex facilitate the dispersion of CNFs in the matrix without aggregation, until finally coalescing after processing and possibly giving rise to improved adhesion between CNF and the latex in the matrix, indicated by rheology measurements. Lastly, new nanocomposite films consisting of 75wt% CNF and 25wt% of PISA-latexes were produced and evaluated. The results show that CNF and rigid 100 nm sized PISA-latex, with PMMA core, gives a very tough double network, with strain-at-break above 28%, stiffness of 3.5 GPa and a strength of 110 MPa. These are impressive properties compared to commonly used fossil-based plastic materials.

    The full text will be freely available from 2020-02-01 15:00
  • 4.
    Engström, Joakim
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Centres, Wallenberg Wood Science Center.
    Asem, Heba
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Brismar, Hjalmar
    KTH, Superseded Departments (pre-2005), Physics. KTH, Centres, Science for Life Laboratory, SciLifeLab. KTH, School of Engineering Sciences (SCI), Applied Physics.
    Zhang, Yuning
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology.
    Malkoch, Michael
    KTH, Superseded Departments (pre-2005), Fibre and Polymer Technology. KTH, Superseded Departments (pre-2005), Polymer Technology. KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Malmström, Eva
    KTH, Superseded Departments (pre-2005), Fibre and Polymer Technology.
    In situ encapsulation of Nile red or Doxorubicinduring RAFT‐mediated emulsion polymerizationvia PISAManuscript (preprint) (Other academic)
  • 5.
    Engström, Joakim
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Centres, Wallenberg Wood Science Center. KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Benselfelt, Tobias
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Centres, Wallenberg Wood Science Center. 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, Coating Technology. KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Centres, Wallenberg Wood Science Center.
    D'Agosto, Franck
    Université de Lyon, Univ Lyon 1, CPE Lyon, CNRS UMR 5265, C2P2 (Chemistry, Catalysis, Polymers & Processes), LCPP, 69616 Villeurbanne, France .
    Lansalot, Muriel
    Université de Lyon, Univ Lyon 1, CPE Lyon, CNRS UMR 5265, C2P2 (Chemistry, Catalysis, Polymers & Processes), LCPP, 69616 Villeurbanne, France .
    Carlmark, Anna
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Centres, Wallenberg Wood Science Center. KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology. RISE.
    Malmström, Eva
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Tailoring adhesion of anionic surfaces using cationic PISA-latexes – towards tough nanocellulose materials in the wet state2019In: Nanoscale, ISSN 2040-3364, E-ISSN 2040-3372Article in journal (Refereed)
    Abstract [en]

    Cationic latexes with Tgs ranging between −40 °C and 120 °C were synthesised using n-butyl acrylate (BA) and/or methyl methacrylate (MMA) as the core polymers. Reversible addition–fragmentation chain transfer (RAFT) combined with polymerisation-induced self-assembly (PISA) allowed for in situ chain-extension of a cationic macromolecular RAFT agent (macroRAFT) of poly(N-[3-(dimethylamino)propyl] methacrylamide) (PDMAPMA), used as stabiliser in so-called surfactant-free emulsion polymerisation. The resulting narrowly distributed nanosized latexes adsorbed readily onto silica surfaces and to model surfaces of cellulose nanofibrils, as demonstrated by quartz crystal microbalance with dissipation monitoring (QCM-D) measurements. Adsorption to anionic surfaces increased when increasing ionic strength to 10 mM, indicating the influence of the polyelectrolyte effect exerted by the corona. The polyelectrolyte corona affected the interactions in the wet state, the stability of the latex and re-dispersibility after drying. The QCM-D measurements showed that a lower Tg of the core results in a more strongly interacting adsorbed layer at the solid–liquid interface, despite a comparable adsorbed mass, indicating structural differences of the investigated latexes in the wet state. The two latexes with Tg below room temperature (i.e. PBATg-40 and P(BA-co-MMA)Tg3) exhibited film formation in the wet state, as shown by AFM colloidal probe measurements. It was observed that P(BA-co-MMA)Tg3 latex resulted in the largest pull-off force, above 200 m Nm−1 after 120 s in contact. The strongest wet adhesion was achieved with PDMAPMA-stabilized latexes soft enough to allow for interparticle diffusion of polymer chains, and stiff enough to create a strong adhesive joint. Fundamental understanding of interfacial properties of latexes and cellulose enables controlled and predictive strategies to produce strong and tough materials with high nanocellulose content, both in the wet and dry state.

  • 6.
    Engström, Joakim
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Centres, Wallenberg Wood Science Center.
    Stamm, Arne
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Tengdelius, Mattias
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Syrén, Per-Olof
    KTH, Centres, Science for Life Laboratory, SciLifeLab. KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Fogelström, Linda
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Malmström, Eva
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology.
    Cationic latexes of bio‐based hydrophobicmonomer Sobrerol methacrylate (SobMA)Manuscript (preprint) (Other academic)
  • 7.
    Granskog, Viktor
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Thiol-Ene/Yne Adhesives for Tissue Fixation2018Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    The utilization of adhesives in surgery has not reached its full potential and research in the field is encouraged by the surgeons’ desire for improved alternatives to today’s tissue fixation strategies. Here, adhesive resins based on thiol-ene coupling (TEC) chemistry or thiol-yne coupling (TYC) chemistry are exploited to develop tissue adhesives that cure fast and on-demand via photoinitiation. In order to make safer adhesives, macromolecular components and systems with high conversion of functional groups were developed to minimize leakage of unreacted monomers.To develop macromolecular resin components, allyl-functional dendritic-linear-dendritic (DLD) co-polymers were synthesized with a poly(ethylene glycol) (PEG) core chain and hyperbranched structures of 2,2-bis(hydroxymethyl) propionic acid (bis-MPA) to capitalize on the rheological properties of dendritic structures. The dendritic structures interfered with the crystallization of the PEG segment and the DLD’s liquid appearance enabled their use as macromolecular components without solvent. The DLDs were cured with a thiol crosslinker and the strategy disclosed degradable soft tissue adhesives with good adhesion to wet porcine skin.Mussel inspired dopamine derivatives was evaluated as adhesion-enhancing primers for bone adhesives. The addition of NaOH to the primer solutions increased the shear bond strengths of the adhesive to bone. The highest bond strengths with the tested dopamine derivatives were obtained when a combination of thiol and ene-functional derivatives were used.With inspiration from dental resin adhesives, a fully TEC based adhesive system was developed with excellent shear bond strength to wet bone substrates. The adhesive system enabled superior fixation of phalangeal fracture models compared to the daily used Kirschner wires and could even compete with a screw fixated metal plate. The adhesive materials proved biocompatible in initial in vitro and in vivo studies.Strong and rigid materials for fracture fixation were developed via a strategy of using highly crosslinked triazine-trione monomers and TEC or TYC chemistry. The development resulted in TYC resin based materials with mechanical properties that very well can compete with poly(ether ether ketone) (PEEK) that is used in biomedical load bearing applications due to its high strength, toughness and inertness.

  • 8.
    Granskog, Viktor
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    García-Gallego, Sandra
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    von Kieseritzky, Johanna
    Department of Clinical Science and Education and the Department of Hand Surgery, Karolinska Institutet.
    Rosendahl, Jennifer
    RISE Research Institutes of Sweden, Bioscience and Materials–Medical Device Technology.
    Stenlund, Patrik
    RISE Research Institutes of Sweden, Bioscience and Materials–Medical Device Technology.
    Zhang, Yuning
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Petronis, Sarunas
    RISE Research Institutes of Sweden, Bioscience and Materials–Medical Device Technology.
    Lyvén, Benny
    RISE Research Institutes of Sweden, Bioscience and Materials–Medical Device Technology.
    Arner, Marianne
    Department of Clinical Science and Education and the Department of Hand Surgery, Karolinska Institutet.
    Håkansson, Joakim
    RISE Research Institutes of Sweden, Bioscience and Materials–Medical Device Technology.
    Malkoch, Michael
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    High-Performance Thiol–Ene Composites Unveil a New Era of Adhesives Suited for Bone Repair2018In: Advanced Functional Materials, ISSN 1616-301X, E-ISSN 1616-3028, Vol. 28, no 26, article id 1800372Article in journal (Refereed)
    Abstract [en]

    The use of adhesives for fracture fixation can revolutionize the surgical procedures toward more personalized bone repairs. However, there are still no commercially available adhesive solutions mainly due to the lack of biocompatibility, poor adhesive strength, or inadequate fixation protocols. Here, a surgically realizable adhesive system capitalizing on visible light thiol–ene coupling chemistry is presented. The adhesives are carefully designed and formulated from a novel class of chemical constituents influenced by dental resin composites and self-etch primers. Validation of the adhesive strengthis conducted on wet bone substrates and accomplished via fiber-reinforced adhesive patch (FRAP) methodology. The results unravel, for the first time, on the promise of a thiol–ene adhesive with an unprecedented shear bondstrength of 9.0 MPa and that surpasses, by 55%, the commercially available acrylate dental adhesive system Clearfil SE Bond of 5.8 MPa. Preclinical validation of FRAPs on rat femur fracture models details good adhesion to the bone throughout the healing process, and are found biocompatible not giving rise to any inflammatory response. Remarkably, the FRAPs are found to withstand loads up to 70 N for 1000 cycles on porcine metacarpal fractures outperforming clinically used K-wires and match metal plates and screw implants.

  • 9.
    Hendrikse, Natalie
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology. KTH, Centres, Science for Life Laboratory, SciLifeLab. Swedish Orphan Biovitrum AB, Stockholm, Sweden.
    Charpentier, Gwenaelle
    KTH, Centres, Science for Life Laboratory, SciLifeLab. ESCOM, 1 Allee Reseau Jean Marie Buckmaster, F-60200 Compiegne, France..
    Nordling, Erik
    Swedish Orphan Biovitrum AB, Stockholm, Sweden..
    Syrén, Per-Olof
    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), Protein Science, Protein Technology. KTH, Centres, Science for Life Laboratory, SciLifeLab. Swedish Orphan Biovitrum AB, Stockholm, Sweden.
    Ancestral diterpene cyclases show increased thermostability and substrate acceptance2018In: The FEBS Journal, ISSN 1742-464X, E-ISSN 1742-4658, Vol. 285, no 24, p. 4660-4673Article in journal (Refereed)
    Abstract [en]

    Bacterial diterpene cyclases are receiving increasing attention in biocatalysis and synthetic biology for the sustainable generation of complex multicyclic building blocks. Herein, we explore the potential of ancestral sequence reconstruction (ASR) to generate remodeled cyclases with enhanced stability, activity, and promiscuity. Putative ancestors of spiroviolene synthase, a bacterial class I diterpene cyclase, display an increased yield of soluble protein of up to fourfold upon expression in the model organism Escherichia coli. Two of the resurrected enzymes, with an estimated age of approximately 1.7 million years, display an upward shift in thermostability of 7-13 degrees C. Ancestral spiroviolene synthases catalyze cyclization of the natural C-20-substrate geranylgeranyl diphosphate (GGPP) and also accept C-15 farnesyl diphosphate (FPP), which is not converted by the extant enzyme. In contrast, the consensus sequence generated from the corresponding multiple sequence alignment was found to be inactive toward both substrates. Mutation of a nonconserved position within the aspartate-rich motif of the reconstructed ancestral cyclases was associated with modest effects on activity and relative substrate specificity (i.e., k(cat)/K-M for GGPP over k(cat)/K-M for FPP). Kinetic analyses performed at different temperatures reveal a loss of substrate saturation, when going from the ancestor with highest thermostability to the modern enzyme. The kinetics data also illustrate how an increase in temperature optimum of biocatalysis is reflected in altered entropy and enthalpy of activation. Our findings further highlight the potential and limitations of applying ASR to biosynthetic machineries in secondary metabolism.

  • 10.
    Hult, Daniel
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Versatile Synthetic Strategies to Highly Functional Polyesters and Polycarbonates2018Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    Polymers have become ubiquitous in today’s society and are found in everything from household items to airplanes and automobiles. Synthetic polymeric materials are as diverse as their applications and their final properties are highly reliant on the building blocks and methods used to assemble them. In the field of biomedical materials, polyesters and polycarbonates have been hailed as excellent materials in large part due to their inherent hydrolytic degradability. With this in mind, careful choice of monomers can ensure that materials not only conform to the desired physical properties, but also elicit a favorable biological response. The utilization of post-polymerization modification of these promising materials has the capability of opening up further avenues to target even more advanced applications. Unfortunately, rigorous and difficult reaction conditions, including multi-step synthesis have to a certain extent held back the adoption of these complex functional materials in applied research. In a pragmatic approach, a sustainable framework was developed in this thesis to seek out more practical methods, limiting the amount of reaction steps and overtly hazardous chemicals.

    In a first study, we set out to simplify and scale-up the synthesis of cyclic carbonates with pendant functional groups, capable of undergoing controlled ring-opening polymerization. By avoiding the use of protective-group chemistry we were able two devise a two-step method to create a library of functional monomers. Results in this study show that reactive intermediates could be isolated on 100 g scales, which in a second step was functionalized with a desired alcohol.

    With this framework in mind, key practical decisions were made to drastically re-think the work up procedures for greater scalability of bis-MPA dendrimers. In this work, a more efficient, scalable and sustainable approach was devised. Elimination of traditional arduous purification steps led to the synthesis of monodisperse dendrimers up to the sixth generation, with 192 functional groups on 50 g scales. Further work included the omission of protective group-chemistry, using orthogonal functional groups to cut the number of synthetic steps by half.

    The know-how developed in the first two projects led us to pursue greater scalability of functional polycarbonates through a simpler polymerization technique. The method allowed the step-growth polymerization of functional materials from more easily accessible monomers isolated on 100 g scales. Subsequent polymerization afforded materials with glass transition temperatures in the range of -45 °C to 169 °C. The method served as a complement to cyclic carbonates, offering a wider range of functional monomers. Furthermore, by careful choice of assembly method, both alternating and scrambled compositions could be achieved.

    In a final study, we set out to take advantage of the scrambling mechanism. Control of the final composition of highly rigid degradable polycarbonates was pursued, using renewable building-blocks derived from sugar. In a proof of concept study, thermal and hydrolytic stability of these materials is shown to be dependent on both amount and configuration of each monomer in the final material.

  • 11.
    Hult, Daniel
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Garcia-Gallego, Sandra
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Ingverud, Tobias
    Andrén, Oliver
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemical Engineering, Applied Electrochemistry.
    Malkoch, Michael
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Degradable High Tg Sugar Derived Polycarbonates from Isosorbide and Dihydroxyacetone2018In: Polymer Chemistry, ISSN 1759-9954, E-ISSN 1759-9962Article in journal (Refereed)
    Abstract [en]

    Polycarbonates from isosorbide and dihydroxyacetone (DHA) have been synthesised using organocatalytic step-growth polymerization of their corresponding diols and bis-carbonylimidazolides monomers. By choice of feed ratio and monomer activation, either isosorbide or ketal protected DHA, random and alternating poly(Iso-co-DHA) carbonates have been formed. Thermal properties by DSC and TGA were herein strongly correlated to monomer composition. Dilution studies using 1H-NMR of a model compound DHA-diethyl carbonate in acetonitrile and deuterated water highlighted the influence of α-substituents on the keto/hydrate equilibrium of DHA. Further kinetics studies of in the pH* range of 4.7 to 9.6 serve to show the hydrolytic pH-profile of DHA-carbonates. The Hydrolytic degradation of deprotected polymer pellets show an increased degradation with increasing DHA content. Pellets with a random or alternating configuration show different characteristics in terms of mass loss and molecular weight loss profile over time.

  • 12.
    Kaldéus, Tahani
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Centres, Wallenberg Wood Science Center. KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Nordenström, Malin
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Fibre Technology.
    Erlandsson, Johan
    Wågberg, Lars
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Fibre Technology.
    Malmström, Eva
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Redispersibility properties of dried cellulose nanofibrils - influence on structure and mechanical properties2019In: Article in journal (Other academic)
  • 13.
    Kaldéus, Tahani
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Telaretti Leggieri, Maria Rosella
    Cobo Sanchez, Carmen
    Malmström, Eva
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology.
    All-aqueous SI-ARGET ATRP from cellulose nanofibrils using hydrophilic and hydrophobic monomers2019In: Article in journal (Other academic)
  • 14.
    Kaldéus, Tahani
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Centres, Wallenberg Wood Science Center. KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Träger, Andrea
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Fibre Technology.
    Berglund, Lars
    KTH, School of Engineering Sciences (SCI), Aeronautical and Vehicle Engineering.
    Malmström, Eva
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology.
    Lo Re, Giada
    Chalmers University of Technology.
    Molecular engineering of cellulose-PCL bio-nanocomposite interface by reactive amphiphilic copolymer nanoparticles2019In: Article in journal (Refereed)
  • 15.
    Kürten, Charlotte
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology. KTH, Centres, Science for Life Laboratory, SciLifeLab.
    Eriksson, Adam
    Maddalo, Gianluca
    Edfors, Fredrik
    Uhlén, Mathias
    KTH, Centres, Science for Life Laboratory, SciLifeLab.
    Syrén, Per-Olof
    KTH, Centres, Science for Life Laboratory, SciLifeLab.
    Engineering of water networks in class II terpene cyclases underscores the importance of amino acid hydration and entropy in biocatalysis and enzyme designManuscript (preprint) (Other academic)
  • 16.
    Lo Re, Giada
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Biocomposites.
    Engström, Joakim
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Centres, Wallenberg Wood Science Center. KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Wu, Qiong
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Biocomposites.
    Malmström, Eva
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Centres, Wallenberg Wood Science Center.
    Gedde, Ulf W
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology.
    Olsson, Richard
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Polymeric Materials.
    Berglund, Lars
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Biocomposites.
    Improved Cellulose Nanofibril Dispersion in Melt-Processed Polycaprolactone Nanocomposites by a Latex-Mediated Interphase and Wet Feeding as LDPE Alternative2018In: ACS Applied Nano Materials, Vol. 1, no 6, p. 2669-2677Article in journal (Refereed)
    Abstract [en]

    This work reports the development of a sustainable and green one-step wet-feeding method to prepare tougher and stronger nanocomposites from biodegradable cellulose nanofibrils (CNF)/polycaprolactone (PCL) constituents, compatibilized with reversible addition fragmentation chain transfer-mediated surfactant-free poly(methyl methacrylate) (PMMA) latex nanoparticles. When a PMMA latex is used, a favorable electrostatic interaction between CNF and the latex is obtained, which facilitates mixing of the constituents and hinders CNF agglomeration. The improved dispersion is manifested in significant improvement of mechanical properties compared with the reference material. The tensile tests show much higher modulus (620 MPa) and strength (23 MPa) at 10 wt % CNF content (compared to the neat PCL reference modulus of 240 and 16 MPa strength), while maintaining high level of work to fracture the matrix (7 times higher than the reference nanocomposite without the latex compatibilizer). Rheological analysis showed a strongly increased viscosity as the PMMA latex was added, that is, from a well-dispersed and strongly interacting CNF network in the PCL.

  • 17.
    Martin-Serrano Ortiz, Angela
    et al.
    IBIMA Reg Univ Hosp Malaga UMA, Hosp Civil, Res Lab, Plaza Hosp Civil, Malaga 29009, Spain.;IBIMA Reg Univ Hosp Malaga UMA, Hosp Civil, Allergy Unit, Plaza Hosp Civil, Malaga 29009, Spain.;BIONAND Andalusian Ctr Nanomed & Biotechnol, Parque Tecnol Andalucia, Malaga 29590, Spain..
    Stenström, Patrik
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology.
    Antunez, Pablo Mesa
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Andrén, Oliver C. J.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Torres, Maria J.
    IBIMA Reg Univ Hosp Malaga UMA, Hosp Civil, Res Lab, Plaza Hosp Civil, Malaga 29009, Spain.;IBIMA Reg Univ Hosp Malaga UMA, Hosp Civil, Allergy Unit, Plaza Hosp Civil, Malaga 29009, Spain.;BIONAND Andalusian Ctr Nanomed & Biotechnol, Parque Tecnol Andalucia, Malaga 29590, Spain..
    Montanez, Maria I.
    IBIMA Reg Univ Hosp Malaga UMA, Hosp Civil, Res Lab, Plaza Hosp Civil, Malaga 29009, Spain.;IBIMA Reg Univ Hosp Malaga UMA, Hosp Civil, Allergy Unit, Plaza Hosp Civil, Malaga 29009, Spain.;BIONAND Andalusian Ctr Nanomed & Biotechnol, Parque Tecnol Andalucia, Malaga 29590, Spain..
    Malkoch, Michael
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Design of multivalent fluorescent dendritic probes for site-specific labeling of biomolecules2018In: Journal of Polymer Science Part A: Polymer Chemistry, ISSN 0887-624X, E-ISSN 1099-0518, Vol. 56, no 15, p. 1609-1616Article in journal (Refereed)
    Abstract [en]

    Herein, the synthesis and characterization of orthogonal dendrons decorated with multiple units of fluorescent and a chemoselective group at a focal point, followed by specific antibody labeling, is presented. Fluorescence results confirm the applicability of the fluorescent probes for biomolecule labeling and fluorescent signal amplification.

  • 18.
    Nameer, Samer
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Larsen, Daniel B.
    Tech Univ Denmark, Dept Chem & Biochem Engn, DPC, Soltofts Plads Bldg 227, DK-2800 Lyngby, Denmark.;Tech Univ Denmark, Dept Chem, Bygning 207, DK-2800 Lyngby, Denmark..
    Duus, Jens O.
    Tech Univ Denmark, Dept Chem, Bygning 207, DK-2800 Lyngby, Denmark..
    Daugaard, Anders E.
    Tech Univ Denmark, Dept Chem & Biochem Engn, DPC, Soltofts Plads Bldg 227, DK-2800 Lyngby, Denmark..
    Johansson, Mats
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Biobased Cationically Polymerizable Epoxy Thermosets from Furan and Fatty Acid Derivatives2018In: ACS Sustainable Chemistry and Engineering, ISSN 2168-0485, Vol. 6, no 7, p. 9442-9450Article in journal (Refereed)
    Abstract [en]

    In the pursuit of environmentally friendly building blocks in polymer chemistry the utilization of biobased monomers is highly desired. In the present study, the biobased monomer 2,5-furandicarboxylic acid (FDCA) has been extended into epoxy thermosets. The study presents the synthesis of diallyl furan-2,5-dicarboxylate (DAFDC) followed by an epoxidation of the allyls to form diglycidyl furan-2,5-dicarboxylate (DGFDC). DGFDC was then copolymerized in both stoichiometric and off-stoichiometric ratios with epoxidized fatty methyl esters to form a range of thermosets. The cross-linking reaction was either thermally or UV-induced cationic polymerization utilizing onium salt initiators where the reactivity was studied by DSC and real-time fourier transform infrared analysis. Furthermore, the structure-property relationships of the final thermosets were determined by dynamic mechanical thermal analysis revealing a possibility to tune the properties over a wide range. In addition thermosets were made from diglycidyl Bisphenol-A (DGEBA) with epoxidized fatty methyl esters made for comparative purposes.

  • 19.
    Nordström, Randi
    et al.
    Ms, Dept Pharm, Uppsala, Sweden..
    Nyström, Lina
    Uppsala Univ, Dept Pharm, Uppsala, Sweden..
    Andrén, Oliver C. J.
    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.
    Umerska, Anita
    MINT Univ Angers, Angers, France..
    Davoudi, Mina
    Lund Univ, Dept Clin Sci, Lund, Sweden..
    Schmidtchen, Artur
    Lund Univ, Dept Clin Sci, Lund, Sweden..
    Malmsten, Martin
    Uppsala Univ, Dept Pharm, Uppsala, Sweden..
    Poly(acrylic acid) microgels as carriers for antimicrobial peptides2018In: Abstract of Papers of the American Chemical Society, ISSN 0065-7727, Vol. 255Article in journal (Other academic)
  • 20.
    Norström, Emelie
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Hemicelluloses and other Polysaccharides for Wood Adhesive Applications2018Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    The growing environmental awareness has led to an increased interest in bio-based polymers as replacement for fossil-based materials. The purpose of the work described in this thesis was to investigate the possibility of using hemicelluloses and other polysaccharides as replacement for fossil-based polymers in wood adhesives. Together with cellulose and lignin, hemicellulose is the main constituent of wood. In the pulp industry, significant amounts of hemicelluloses are obtained as by-products and combusted for energy recovery, but there is a growing interest in the biorefinery concept where all side-streams are utilized. If valuable applications, such as adhesives, of hemicelluloses and other by-products are found, large amounts can be obtained from the pulp industry. Water dispersions of hemicelluloses and other polysaccharides have been prepared and evaluated as adhesives for bonding different wood substrates together. The dry bond strength, water resistance, and heat resistance were investigated by exposing the bonded wood specimens to different conditioning methods and thereafter measuring the tensile shear strengths. As a replacement, the bio-based wood adhesive must possess similar or even better properties than the fossil-based adhesives. A commercial poly(vinyl acetate) (PVAc) wood adhesive used for indoor applications has been used as a reference benchmark. Wood hemicelluloses themselves do not have sufficient bonding performance probably because their low molecular weight does not provide adequate strength and makes the adhesive too brittle. The addition of dispersing agents and crosslinkers to the hemicellulose dispersions can significantly improve the bonding performance, and hemicellulose in combination with poly(vinyl amine) showed promising results superior those of PVAc. A fully bio-based adhesive comprising of hemicellulose and chitosan, another bio-based polysaccharide, obtain surprisingly good bonding performance especially with regard to water resistance. Gums, polysaccharides with similar structures to those of hemicelluloses but with higher molecular weights, have also been studied and locust bean gum dispersions without any modification showed a very good bonding performance with high dry bond strength and water resistance on a par with those of PVAc and a heat resistance superior to that of PVAc. Chitosan has very good adhesive properties especially with regard to water resistance, but the high viscosity of the chitosan dispersion makes it difficult to apply. Chitosan-grafted-PVAc dispersions were therefore prepared and an adhesive very similar in appearance to PVAc was obtained with a good bonding performance as well as good applicability.

  • 21. Pavlidis, I. V.
    et al.
    Hendrikse, Natalie
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Syrén, Per-Olof
    KTH, Centres, Science for Life Laboratory, SciLifeLab.
    Chapter 5: Computational Techniques for Efficient Biocatalysis2018In: RSC Catalysis Series, no 32, p. 119-152Article in journal (Refereed)
    Abstract [en]

    Addressing some of the most challenging problems that we face today, including depletion of natural resources, sustainable energy production and the generation of green polymeric materials by the biocatalytic upcycling of renewable synthons, requires an expansion of the current available biochemical reaction space. Creating biocatalysts harboring novel chemistries - whether inside or outside the cell - is dependent on the discovery of novel enzymes and metabolic pathways, together with the de novo design of enzymes and directed evolution. Herein we review the high potential of using bioinformatics and in silico computer modelling tools to guide protein engineering and to enhance our fundamental understanding of biocatalysis. Following an overview of technical considerations and the current state-of-the art in sequence- and structure-based protein engineering methodologies, we highlight recent successful examples of their implementation in biocatalysis and synthetic biology. Moreover, we discuss how selected computational tools in concert with experimental biocatalysis could decipher how the sequence, structure and dynamics of proteins dictate their function. Using the methodologies discussed in this chapter, an accelerated biocatalytic manufacturing of chemicals, pharmaceuticals, biofuels and monomeric building blocks is envisioned.

  • 22. Reverdy, C.
    et al.
    Belgacem, N.
    Moghaddam, M. S.
    Sundin, M.
    Swerin, Agne
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology. RISE Research Institutes of Sweden – Bioscience and Materials, Box 5607, Stockholm, Sweden.
    Bras, J.
    One-step superhydrophobic coating using hydrophobized cellulose nanofibrils2018In: Colloids and Surfaces A: Physicochemical and Engineering Aspects, ISSN 0927-7757, E-ISSN 1873-4359, Vol. 544, p. 152-158Article in journal (Refereed)
    Abstract [en]

    Superhydrophobic surfaces have high potential in self-cleaning and anti-fouling applications. We developed a one-step superhydrophobic coating formulation containing sodium oleate (NaOl), hydrophobized precipitated calcium carbonate and biobased cellulose nanofibrils (CNFs) hydrophobized with either alkyl ketene dimer (AKD) or amino propyl trimethoxy silane (APMS) as a binder to fix and distribute the particles. Coatings were made on paperboard and the wetting behavior of the surface was assessed. Static, advancing and receding contact angles with water as well as roll-off and water shedding angle were compared to coatings made with styrene butadiene latex as binder instead of CNFs. Modifications with alkyl ketene dimer showed most promising results for a viable process in achieving superhydrophobic paperboard but required reformulation of the coating with optimized and reduced amount of NaOl to avoid surfactant-induced wetting via excess NaOl. A static water contact angle of 150° was reached for the CNF-AKD. The use of CNFs enables the improvement of coating quality avoiding cracking with the use of nanocellulose as a renewable binder.

  • 23.
    Syrén, Per-Olof
    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), Protein Science, Protein Technology. KTH, Centres, Science for Life Laboratory, SciLifeLab. KTH Royal Inst Technol, Sch Engn Sci Chem Biotechnol & Hlth, Sci Life Lab, Dept Fibre & Polymer Technol, S-17165 Solna, Sweden.;KTH Royal Inst Technol, Dept Prot Sci, S-17165 Solna, Sweden..
    Enzymatic Hydrolysis of Tertiary Amide Bonds by anti Nucleophilic Attack and Protonation2018In: Journal of Organic Chemistry, ISSN 0022-3263, E-ISSN 1520-6904, Vol. 83, no 21, p. 13543-13548Article in journal (Refereed)
    Abstract [en]

    The molecular mechanisms conferring high resistance of planar tertiary amide bonds to hydrolysis by most enzymes have remained elusive. To provide a chemical explanation to this unresolved puzzle, UB3LYP calculations were performed on an active site model of Xaa-Pro peptidases. The calculated reaction mechanism demonstrates that biocatalysts capable of tertiary amide bond hydrolysis capitalize on anti nucleophilic attack and protonation of the amide nitrogen, in contrast to the traditional syn displayed by amidases and proteases acting on secondary amide bonds.

  • 24.
    Vilela, Carla
    et al.
    Department of Chemistry, CICECO – Aveiro Institute of Materials, University of Aveiro, Aveiro 3810-193, Portugal.
    Engström, Joakim
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Centres, Wallenberg Wood Science Center. KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Valente, Bruno F. A.
    Department of Chemistry, CICECO – Aveiro Institute of Materials, University of Aveiro, Aveiro 3810-193, Portugal.
    Jawerth, Marcus
    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.
    Carlmark, Anna
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Coating Technology.
    Freire, Carmen S. R.
    Department of Chemistry, CICECO – Aveiro Institute of Materials, University of Aveiro, Aveiro 3810-193, Portugal.
    Exploiting poly(ɛ-caprolactone) and cellulose nanofibrils modified with latex nanoparticles for the development of biodegradable nanocomposites2018In: Polymer Composites, ISSN 0272-8397, E-ISSN 1548-0569Article in journal (Refereed)
    Abstract [en]

    This study reports the development of nanocomposites based on poly(?-caprolactone) (PCL) and cellulose nanofibrils (CNF) modified with cationic latex nanoparticles. The physical adsorption of these water-based latexes on the surface of CNF was studied as an environment-friendly strategy to enhance the compatibility of CNF with a hydrophobic polymeric matrix. The latexes are composed of amphiphilic block copolymers based on cationic poly(N,N-dimethylaminoethyl methacrylate-co-methacrylic acid) as the hydrophilic block, and either poly(methyl methacrylate) or poly(n-butyl methacrylate) as the hydrophobic block. The simple and practical melt-mixing of PCL- and latex-modified CNF yielded white homogeneous nanocomposites with complete embedment of the nanofibrils in the thermoplastic matrix. All nanocomposites are semicrystalline materials with good mechanical properties (Young's modulus?=?43.6?52.3 MPa) and thermal stability up to 335?340°C. Degradation tests clearly showed that the nanocomposites slowly degrade in the presence of lipase-type enzyme. These PCL/CNF-latex nanocomposite materials show great promise as future environmentally friendly packaging materials. POLYM. COMPOS., 2018. ? 2018 Society of Plastics Engineers

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