| 1. |
- Andrén, Oliver C. J., et al.
(författare)
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Antibiotic-Free Cationic Dendritic Hydrogels as Surgical-Site-Infection-Inhibiting Coatings
- 2019
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Ingår i: Advanced Healthcare Materials. - : Wiley. - 2192-2640 .- 2192-2659.
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Tidskriftsartikel (refereegranskat)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 β-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.
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| 2. |
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| 4. |
- Carlsson, Linn, et al.
(författare)
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Surface characteristics of cellulose nanoparticles grafted by surface-initiated ring-opening polymerization of epsilon-caprolactone
- 2015
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Ingår i: Cellulose. - : Springer Science and Business Media LLC. - 0969-0239 .- 1572-882X. ; 22:2, s. 1063-1074
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Tidskriftsartikel (refereegranskat)abstract
- 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.
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| 5. |
- Erlandsson, Johan, et al.
(författare)
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On the mechanism behind freezing-induced chemical crosslinking in ice-templated cellulose nanofibril aerogels
- 2018
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Ingår i: Journal of Materials Chemistry A. - : Royal Society of Chemistry. - 2050-7488 .- 2050-7496. ; 6:40, s. 19371-19380
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Tidskriftsartikel (refereegranskat)abstract
- 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.
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| 6. |
- Hult, Daniel, 1986-, et al.
(författare)
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Degradable High Tg Sugar Derived Polycarbonates from Isosorbide and Dihydroxyacetone
- 2018
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Ingår i: Polymer Chemistry. - : Royal Society of Chemistry. - 1759-9954 .- 1759-9962. ; 9:17, s. 2238-2246
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Tidskriftsartikel (refereegranskat)abstract
- 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.
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| 7. |
- Ingverud, Tobias, et al.
(författare)
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Dendritic Polyampholyte-Assisted Formation of Functional Cellulose Nanofibril Materials
- 2020
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Ingår i: Biomacromolecules. - : American Chemical Society (ACS). - 1525-7797 .- 1526-4602. ; 21:7, s. 2856-2863
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Tidskriftsartikel (refereegranskat)abstract
- A new platform of functional hybrid materials from anionically charged high-aspect-ratio cellulose nanofibrils (CNFs) and a dendritic polyampholyte, Helux, is herein proposed. The polyampholytic character of Helux enabled facile and efficient nanoscale mixing with the CNFs, and the resulting composite mixtures of CNFs and Helux displayed thixotropic behavior and formed physical and reversibly cross-linked gels when left unperturbed for short spans of time. The gel could be chemically cross-linked into self-supporting solid hydrogels containing impressive water contents of 99.6% and a storage modulus of 1.8 kPa by thermal activation. Non-cross-linked mixtures of CNF/Helux were assembled into composites, such as films by solvent casting and aerogels with densities as low as 4 kg/m(3) by lyophilizing ice-templated CNF/Helux mixtures. The resulting materials exhibited excellent wet stability due to the heat-activated cross-linking and were readily available for postfunctionalization via amidation chemistry using Helux-accessible amines in aqueous conditions. The mechanical performance of the films was not jeopardized by the addition of Helux. Additionally, by varying the amount of Helux, the compressive elastic modulus of aerogels was tunable in both the non-cross-linked and cross-linked states. The fast and efficient nanoscale mixing of anionic CNFs and a polymer containing cationic groups is unique, novel, and promising as a functional material platform. Sustainable CNFs guided by heterofunctional dendritic polyampholytes are envisaged to act as a pillar toward high-performance applications, including biomedicine and biomaterials.
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| 8. |
- Ingverud, Tobias, 1989-
(författare)
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Exploring crosslinked networks of polymers and hybrid cellulose materials
- 2019
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- 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.
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| 9. |
- Ingverud, Tobias, et al.
(författare)
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Helux : A Heterofunctional Hyperbranched Poly(amido amine) Carboxylate
- 2019
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Ingår i: ACS APPLIED POLYMER MATERIALS. - : AMER CHEMICAL SOC. - 2637-6105. ; 1:7, s. 1845-1853
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Tidskriftsartikel (refereegranskat)abstract
- Herein we present the first scientific report on the commercially available Helux 33/16 - a heterofunctional poly(amido amine carboxylate) hyperbranched polymer (Native Helux). The Native Helux, built from diethyl maleate (DEM) and diaminohexane (HMDA), was characterized, in part aided by reverse engineering of a similar scaffold with the same monomers. Different purification methods resulted in higher molecular weight polymers ranging from 8.4 to 51.7 kDa (M-w), and the Helux considered the purest, having 10 mmol (primary and secondary amines)/g as well as 2-4 mmol carboxylic/g Helux. Additionally, aqueous-mediated postmodifications of Helux were achieved including Michael addition, guanylation, and ring-opening of sultone, as well as water/ethyl acetate-mediated amidation of imidazole-activated pentenoic acid. The inherent heterofunctionality of Helux, amines and carboxylic groups, was further explored by a one-component self-cross-linking approach that yielded a dendritic poly(amido amine) network with autofluorescence-exhibiting properties and a T-g of 59 degrees C. The Helux network exhibited a storage modulus (G') of 7.9 MPa at 25 degrees C and in dry state, and 0.9 MPa (G') when plasticized by 50 wt % swelling (in water) of the network. Finally, dendritic hydrogels based on Helux were produced by a spontaneous NHS-amidation reaction with difunctional 10kPEG-NHS. The mechanical properties of the hydrogels were found to be dependent on the curing temperature for the hydrogel, yielding a G' of 8 and 14.5 kPa, a stress at break of 11.5 and 22.7 kPa, and a strain-at-break of 161 and 163%, at 25 and 37 degrees C, respectively.
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