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  • 1.
    Engel, Emile
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Fibre Technology. Department of Chemistry, University of Bath, Claverton Down, Bath, BA2 7AY UK.
    Calabrese, Vincenzo
    Department of Chemistry, University of Bath, Claverton Down, Bath, BA2 7AY UK.
    Hossain, Kazi M. Z.
    Department of Chemistry, University of Bath, Claverton Down, Bath, BA2 7AY UK.
    Edler, Karen J.
    Department of Chemistry, University of Bath, Claverton Down, Bath, BA2 7AY UK.
    Scott, Janet L.
    Department of Chemistry, University of Bath, Claverton Down, Bath, BA2 7AY UK.
    Composite Hydrogel Spheroids Based on Cellulose Nanofibrils and Nanofibrous Chiral Coordination Polymer by Green Synthesis2020In: Advanced Sustainable Systems, ISSN 2366-7486Article in journal (Refereed)
    Abstract [en]

    Cellulose-based hydrogels are promising sustainable materials for a variety of applications, including tissue engineering, water treatment, and drug delivery. However, the tailoring of diverse properties by efficient green chemistry methods is an ongoing challenge. Here, composite hydrogels of consistent spheroidal structure, incorporating TEMPO-oxidized cellulose nanofibrils and nanofibrous chiral Cu(II) aspartate coordination polymer, are presented. The hydrogels are prepared by a single-step procedure in aqueous media at ambient temperature and pressure, adhering to the principles of green chemistry. With a view to adapting this method for a variety of alternative coordination polymers (to tailor functional properties), the following critical factors for formation of robust composite hydrogel spheroids are identified: rheological properties of the primary matrix used for spheroidal hydrogel formation and coordination polymer self-assembly rate.

  • 2.
    Engel, Emile
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Fibre Technology. Univ Bath, Dept Chem, Bath BA2 7AY, Avon, England..
    Scott, Janet L.
    Univ Bath, Dept Chem, Bath BA2 7AY, Avon, England..
    Advances in the green chemistry of coordination polymer materials2020In: Green Chemistry, ISSN 1463-9262, E-ISSN 1463-9270, Vol. 22, no 12, p. 3693-3715Article, review/survey (Refereed)
    Abstract [en]

    Coordination polymers, including metal-organic frameworks, are a diverse class of materials with myriad properties and potential applications. However, a number of drawbacks have hindered the scaling up of such materials towards commercial applications. These include health and safety risks, environmental hazards, poor cost efficiency and sustainability shortfalls. In contrast to the systematic progress of organic green chemistry, which has contributed to improvements in the sustainability of chemical processing, the development of green chemistry in the context of coordination polymers has been fragmented and sporadic. This review describes advances in the use of green components: benign sustainable ligands and non-hazardous earth abundant metals. Additionally, solvent considerations, synthesis strategies for improved sustainability and the performance of coordination polymers relative to alternative competing materials are discussed.

  • 3.
    Jain, Karishma
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Fibre Technology.
    Wang, Zhen
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Fibre Technology.
    Garma, Leonardo D.
    Karolinska Inst, Med Biochem & Biophys, Stockholm, Sweden..
    Engel, Emile
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Fibre Technology.
    Ciftci, Göksu Cinar
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology.
    Fager, Cecilia
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology.
    Larsson, Per A.
    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. KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Centres, Wallenberg Wood Science Center.
    3D printable composites of modified cellulose fibers and conductive polymers and their use in wearable electronics2023In: APPLIED MATERIALS TODAY, ISSN 2352-9407, Vol. 30, article id 101703Article in journal (Refereed)
    Abstract [en]

    There are many bioelectronic applications where the additive manufacturing of conductive polymers may be of use. This method is cheap, versatile and allows fine control over the design of wearable electronic devices. Nanocellulose has been widely used as a rheology modifier in bio-based inks that are used to print electrical components and devices. However, the preparation of nanocellulose is energy and time consuming. In this work an easy-to-prepare, 3D-printable, conductive bio-ink; based on modified cellulose fibers and poly(3,4-ethylene dioxythiophene) poly(styrene sulfonate) (PEDOT:PSS), is presented. The ink shows excellent printability, the printed samples are wet stable and show excellent electrical and electrochemical performance. The printed structures have a conductivity of 30 S/cm, high tensile strains (>40%), and specific capacitances of 211 F/g; even though the PEDOT:PSS only accounts for 40 wt% of the total ink composition. Scanning electron microscopy (SEM), wide-angle X-ray scattering (WAXS), and Raman spectroscopy data show that the modified cellulose fibers induce conformational changes and phase separation in PEDOT:PSS. It is also demonstrated that wearable supercapacitors and biopotential-monitoring devices can be prepared using this ink.

  • 4.
    Lo Re, Giada
    et al.
    Chalmers Univ Technol, Ind & Mat Sci IMS, SE-41296 Gothenburg, Sweden.;Chalmers Univ Technol, FibRe Ctr Lignocellulose Based Thermoplast, Dept Phys, SE-41296 Gothenburg, Sweden..
    Engel, Emile R.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Fibre Technology.
    Bjorn, Linnea
    Chalmers Univ Technol, Dept Phys, SE-41296 Gothenburg, Sweden.;Chalmers Univ Technol, FibRe Ctr Lignocellulose Based Thermoplast, Dept Phys, SE-41296 Gothenburg, Sweden..
    Sicairos, Manuel Guizar
    Paul Scherrer Inst, Swiss Light Source, CH-5232 Villigen, Switzerland..
    Liebi, Marianne
    Chalmers Univ Technol, FibRe Ctr Lignocellulose Based Thermoplast, Dept Phys, SE-41296 Gothenburg, Sweden.;Paul Scherrer Inst, Swiss Light Source, CH-5232 Villigen, Switzerland.;Empa, Ctr Xray Analyt, Swiss Fed Labs Mat Sci & Technol, CH-9014 St Gallen, Switzerland..
    Wahlberg, Jan
    Tetra Pak, SE-22186 Lund, Sweden..
    Jonasson, Katarina
    Chalmers Univ Technol, Ind & Mat Sci IMS, SE-41296 Gothenburg, Sweden.;Tetra Pak, SE-22186 Lund, Sweden..
    Larsson, Per A.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Fibre Technology. Chalmers Univ Technol, Ind & Mat Sci IMS, SE-41296 Gothenburg, Sweden..
    Melt processable cellulose fibres engineered for replacing oil-based thermoplastics2023In: Chemical Engineering Journal, ISSN 1385-8947, E-ISSN 1873-3212, Vol. 458, p. 141372-, article id 141372Article in journal (Refereed)
    Abstract [en]

    If cellulosic materials are to replace materials derived from non-renewable resources, it is necessary to overcome intrinsic limitations such as fragility, permeability to gases, susceptibility to water vapour and poor three-dimensional shaping. Novel properties or the enhancement of existing properties are required to expand the applications of cellulosic materials and will create new market opportunities. Here we have overcome the well-known restrictions that impede melt-processing of high cellulose content composites. Cellulose fibres, partially derivatised to dialcohol cellulose, have been used to manufacture three-dimensional high-density materials by conventional melt processing techniques, with or without the addition of a thermoplastic polymer. This work demonstrates the use of melt processable chemically modified cellulose fibres in the preparation of a new generation of highly sustainable materials with tuneable properties that can be tailored for specific applications requiring complex three-dimensional parts.

  • 5. Mehandzhiyski, A. Y.
    et al.
    Engel, Emile
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Fibre Technology.
    Larsson, Per A.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Fibre Technology.
    Re, G. L.
    Zozoulenko, I. V.
    Microscopic Insight into the Structure-Processing-Property Relationships of Core-Shell Structured Dialcohol Cellulose Nanoparticles2022In: ACS Applied Bio Materials, E-ISSN 2576-6422, Vol. 5, no 10, p. 4793-4802Article in journal (Refereed)
    Abstract [en]

    In the quest to develop sustainable and environmentally friendly materials, cellulose is a promising alternative to synthetic polymers. However, native cellulose, in contrast to many synthetic polymers, cannot be melt-processed with traditional techniques because, upon heating, it degrades before it melts. One way to improve the thermoplasticity of cellulose, in the form of cellulose fibers, is through chemical modification, for example, to dialcohol cellulose fibers. To better understand the importance of molecular interactions during melt processing of such modified fibers, we undertook a molecular dynamics study of dialcohol cellulose nanocrystals with different degrees of modification. We investigated the structure of the nanocrystals as well as their interactions with a neighboring nanocrystal during mechanical shearing, Our simulations showed that the stress, interfacial stiffness, hydrogen-bond network, and cellulose conformations during shearing are highly dependent on the degree of modification, water layers between the crystals, and temperature. The melt processing of dialcohol cellulose with different degrees of modification and/or water content in the samples was investigated experimentally by fiber extrusion with water used as a plasticizer. The melt processing was easier when increasing the degree of modification and/or water content in the samples, which was in agreement with the conclusions derived from the molecular modeling. The measured friction between the two crystals after the modification of native cellulose to dialcohol cellulose, in some cases, halved (compared to native cellulose) and is also reduced with increasing temperature. Our results demonstrate that molecular modeling of modified nanocellulose fibers can provide fundamental information on the structure-property relationships of these materials and thus is valuable for the development of new cellulose-based biomaterials.

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