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  • 1.
    Ebadi, Mahsa
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Marchiori, Cleber
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Theory.
    Mindemark, Jonas
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Araujo, Carlos Moyses
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Theory.
    Assessing structure and stability of polymer/lithium-metal interfaces from first-principles calculations2019In: Journal of Materials Chemistry A, ISSN 2050-7488, Vol. 7, no 14, p. 8394-8404Article in journal (Refereed)
    Abstract [en]

    Solid polymer electrolytes (SPEs) are promising candidates for Li metal battery applications, but the interface between these two categories of materials has so far been studied only to a limited degree. A better understanding of interfacial phenomena, primarily polymer degradation, is essential for improving battery performance. The aim of this study is to get insights into atomistic surface interaction and the early stages of solid electrolyte interphase formation between ionically conductive SPE host polymers and the Li metal electrode. A range of SPE candidates are studied, representative of major host material classes: polyethers, polyalcohols, polyesters, polycarbonates, polyamines and polynitriles. Density functional theory (DFT) calculations are carried out to study the stability and the electronic structure of such polymer/Li interfaces. The adsorption energies indicated a stronger adhesion to Li metal of polymers with ester/carbonate and nitrile functional groups. Together with a higher charge redistribution, a higher reactivity of these polymers is predicted as compared to the other electrolyte hosts. Products such as alkoxides and CO are obtained from the degradation of ester- and carbonate-based polymers by AIMD simulations, in agreement with experimental studies. Analogous to low-molecular-weight organic carbonates, decomposition pathways through C-carbonyl-O-ethereal and C-ethereal-O-ethereal bond cleavage can be assumed, with carbonate-containing fragments being thermodynamically favorable.

  • 2.
    Eriksson, Therese
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Mindemark, Jonas
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Yue, Ma
    Northwestern Polytech Univ, Ctr Nano Energy Mat, Sch Mat Sci & Engn, Youyi West Rd 127, Xian, Shaanxi, Peoples R China.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Effects of nanoparticle addition to poly(epsilon-caprolactone) electrolytes: Crystallinity, conductivity and ambient temperature battery cycling2019In: Electrochimica Acta, ISSN 0013-4686, E-ISSN 1873-3859, Vol. 300, p. 489-496Article in journal (Refereed)
    Abstract [en]

    It has previously been shown that nanoparticle additives can, in a simple way, significantly improve the ionic conductivity in solid polymer electrolyte systems with the semi-crystalline poly(ethylene oxide) (PEO) as a host material. It has been suggested that the improved ionic conductivity is a result of reduced degree of crystallinity and additional conductivity mechanisms occurring in the material. In this work, this principle is applied to another semi-crystalline polymer host: poly(epsilon-caprolactone) (PCL). This is a polymer with comparable properties (T-g, T-m, etc.) as PEO, and constitute a promising material for use in solid polymer electrolytes for lithium ion batteries. 15 wt% of the respective nanoparticles TiO2, Al2O3 and h-BN have been added to the PCL-LiTFSI solid polymer electrolyte in an attempt to increase the conductivity and achieve stable room temperature cyclability. The crystallinity, ionic conductivity and electrochemical properties were investigated by differential scanning calorimetry, electrochemical impedance spectroscopy and galvanostatic cycling of cells. The results showed that with an addition of 15 wt% Al2O3, the degree of crystallinity is reduced to 6-7% and the ionic conductivity increased to 6-7 x 10(-6) S cm(-1) at room temperature, allowing successful cycling of cells at 30 degrees C, while h-BN did not contribute to similar improvements. The effect of nanoparticles, however, differ significantly from previous observations in PEO systems, which could be explained by different surface-polymer interactions or the degree of ordering in the amorphous phases of the materials.

  • 3.
    Eriksson, Therese
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Mindemark, Jonas
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Polymer Chemistry. Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Yue, Ma
    School of Materials Science and Engineering, Center for Nano Energy materials, Northwestern Polytechnical University, Youyi west road 127, Xi'an, China.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Nanoparticle Additives in Poly(ε-Caprolactone)-Based Solid PolymerElectrolytes; Towards Lower Crystallinity and Higher Ionic Conductivity.2018Conference paper (Refereed)
  • 4.
    Gerz, Isabelle
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Kullgren, Jolla
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Mindemark, Jonas
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Oligomer electrolytes for light-emitting electrochemical cells: Experimental and computational insights2018Conference paper (Refereed)
  • 5.
    Hernández, Guiomar
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Naylor, Andrew J.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Mindemark, Jonas
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Edström, Kristina
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Non-Fluorinated Electrolytes for Si-based Li-ion Battery Anodes2018Conference paper (Other academic)
    Abstract [en]

    Although the performance of lithium-ion batteries has been improved to some extent since the initial commercialization,1 cycling stability, safety and sustainability still present some challenges and concerns. In this regard, the battery electrolyte plays an important role. State-of-the-art electrolytes contain the electrolyte salt LiPF6, susceptible to undergo defluorination reactions and form toxic and corrosive compounds, such as HF. Yet, fluorine-containing electrolytes are often considered necessary for enhanced battery performance. On the other hand, replacing LiPF6 with fluorine-free salts would reduce cost, increase safety and decrease toxicity, both in the manufacturing and recycling processes. Among the available fluorine-free salts, lithium bis(oxalato)borate (LiBOB) is a viable candidate due to its enhanced thermal stability.2 Furthermore, additives in the electrolyte are another common source of fluorine, not least fluoroethylene carbonate (FEC) which can form a stable solid electrolyte interface (SEI).3

    Herein, we compare the cell performance of fluorinated and non-fluorinated electrolytes in NMC/Si-Graphite full cells. Three electrolytes are tested: (1) LP57 (1 M LiPF6 in ethylene carbonate (EC):ethyl methyl carbonate (EMC) 3:7 vol/vol); (2) LP57 with 10 wt% FEC and 2 wt%  vinylene carbonate (VC); and (3) 0.7 M LiBOB in EC:EMC 3:7 vol/vol and 2 wt% VC.

    The cells containing the conventional electrolyte, LP57, feature a rapid capacity fade and continuous decrease in coulombic efficiency. The cell performance is improved when adding SEI-forming additives to the electrolyte (LP57 with FEC and VC). In addition, stable cycling for over 200 cycles are obtained for both the fluorinated (LP57 with FEC and VC) and non-fluorinated (LiBOB with VC) electrolytes.

    Characterisation by X-ray photoelectron spectroscopy (XPS) of the anode surface showed higher amounts of carbonate species and a thicker SEI layer with the non-fluorinated electrolyte compared to the fluorinated one.

    1 J. Electrochem. Soc. 2017, 164, A5019-A5025.

    2 ChemSusChem 2017, 10, 2431-2448.

    3 J. Electrochem. Soc. 2014, 161, A1933-A1938.

  • 6. Höglund, Odd V.
    et al.
    Hagman, Ragnvi
    Olsson, Kerstin
    Mindemark, Jonas
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Materials Chemistry, Polymer Chemistry.
    Borg, Niklas
    Lagerstedt, Anne-Sofie
    A new resorbable device for ligation of blood vessels - A pilot study2011In: Acta Veterinaria Scandinavica, ISSN 1751-0147, E-ISSN 1751-0147, Vol. 53, p. 47-Article in journal (Refereed)
    Abstract [en]

    Background: During surgery, controlled haemostasis to prevent blood loss is vital for a successful outcome. It can be difficult to ligate vessels located deep in the abdomen. A device that is easy to use and enables secure ligatures could be beneficial. Cable ties made of nylon have been used for ligation but the non-resorbable material caused tissue reactions. The objective of this study was to use a resorbable material to construct a device with a self-locking mechanism and to test its mechanical strength and ligation efficiency. Methods: The device was manufactured by injection moulding of polydioxanone, a resorbable polymer used for suture materials. Polydioxanone with inherent viscosities of 1.9 dL/g and 1.3 dL/g were tested. The device consisted of a perforated flexible band which could be pulled through a case with a locking mechanism. After a first version of the device had been tested, some improvements were made. The locking case was downsized, corners were rounded off, the band was made thicker and the mould was redesigned to produce longer devices. Tensile tests were performed with the second version. The first version of the device was used to ligate the ovarian pedicle in a euthanized dog and to test echogenicity of the device with ultrasound. Compression of vessels of the ovarian pedicle was examined by histology. Both versions of the device were tested for haemostasis of and tissue grip on renal arteries in six anaesthetised pigs. Results: The tensile strength of the flexible band of the devices with inherent viscosity of 1.9 dL/g was 50.1 +/- 5.5 N (range 35.2-62.9 N, n = 11) and the devices with inherent viscosity of 1.3 dL/g had a tensile strength of 39.8 +/- 8.1 N (range 18.6-54.2 N, n = 11). Injection moulding of the polymer with lower inherent viscosity resulted in a longer flow distance. Both versions of the device had an effective tissue grip and complete haemostasis of renal arteries was verified. The device attached to the ovarian pedicle could be seen with ultrasound, and vessel compression and occlusion were verified by histology. Conclusions: Tests of functionality of the device showed complete haemostasis and good tissue grip. Devices with a band of sufficient length were easily applied and tightened in tissue.

  • 7.
    Li, Zhenguang
    et al.
    Tokyo Univ Agr & Technol, Grad Sch Bioapplicat & Syst Engn, Tokyo 1848588, Japan.
    Mindemark, Jonas
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Tominaga, Yoichi
    Tokyo Univ Agr & Technol, Grad Sch Bioapplicat & Syst Engn, Tokyo 1848588, Japan.
    A concentrated poly(ethylene carbonate)/poly(trimethylene carbonate) blend electrolyte for all-solid-state Li battery2019In: Polymer journal, ISSN 0032-3896, E-ISSN 1349-0540, Vol. 51, no 8, p. 753-760Article in journal (Refereed)
    Abstract [en]

    Electrochemical and ion-transport properties of polymer blend electrolytes comprising poly(ethylene carbonate) (PEC), poly (trimethylene carbonate) (PTMC) and lithium bis(fluorosulfonyl) imide (LiFSI) were studied in this work, and the electrolyte with the best blend composition was applied in all-solid-state Li batteries. The ionic conductivity of both PEC and PTMC single-polymer electrolytes increased with increasing Li salt concentration. All PEC and PTMC blend electrolytes show ionic conductivities on the order of 10(-5) S cm(-1) at 50 degrees C, and the ionic conductivities increase slightly with increasing PEC contents. The PEC6PTMC4-LiFSI 150 mol% electrolyte demonstrated better Li/electrolyte electrochemical and interfacial stability than that of PEC and PTMC single-polymer electrolytes and maintained a polarization as low as 5 mV for up to 200 h during Li metal plating and stripping. A Li vertical bar SPE vertical bar LFP cell with the PEC6PTMC4-LiFSI 150 mol% electrolyte exhibited reversible charge/discharge capacities close to 150 mAh g(-1) at 50 degrees C and a C/10 rate, which is 88% of the theoretical value (170 mAh g(-1)).

  • 8.
    Li, Zhenguang
    et al.
    Tokyo Univ Agr & Technol, Grad Sch Bioapplicat & Syst Engn, 2-24-16 Naka Cho, Koganei, Tokyo 1848588, Japan.
    Mogensen, Ronnie
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Mindemark, Jonas
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Bowden, Tim
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Polymer Chemistry.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry. Uppsala Univ, Dept Chem, Angstrom Lab, SE-75121 Uppsala, Sweden.
    Tominaga, Yoichi
    Tokyo Univ Agr & Technol, Grad Sch Bioapplicat & Syst Engn, 2-24-16 Naka Cho, Koganei, Tokyo 1848588, Japan.
    Ion-Conductive and Thermal Properties of a Synergistic Poly(ethylene carbonate)/Poly(trimethylene carbonate) Blend Electrolyte2018In: Macromolecular rapid communications, ISSN 1022-1336, E-ISSN 1521-3927, Vol. 39, no 14, article id 1800146Article in journal (Refereed)
    Abstract [en]

    Electrolytes comprising poly(ethylene carbonate) (PEC)/poly(trimethylene carbonate) (PTM C) with lithium bis(trifluoromethane sulfonyl)imide (LiTFSI) are prepared by a simple solvent casting method. Although PEC and PTMC have similar chemical structures, they are immiscible and two glass transitions are present in the differential scanning calorimetry (DSC) measurements. Interestingly, these two polymers change to miscible blends with the addition of LiTFSI, and the ionic conductivity increases with increasing lithium salt concentration. The optimum composition of the blend electrolyte is achieved at PEC6PTMC4, with a conductivity as high as 10(-6) S cm(-1) at 50 degrees C. This value is greater than that for single PEC- and PTMC-based electrolytes. Moreover, the thermal stability of the blend-based electrolytes is improved as compared to PEC-based electrolytes. It is clear that the interaction between C=O groups and Li+ gives rise to a compatible amorphous phase of PEC and PTMC.

  • 9.
    Lindh, E. Mattias
    et al.
    Umeå Univ, Dept Phys, Organ Photon & Elect Grp, Umeå, Sweden.
    Lundberg, Petter
    Umeå Univ, Dept Phys, Organ Photon & Elect Grp, Umeå, Sweden.
    Lanz, Thomas
    Umeå Univ, Dept Phys, Organ Photon & Elect Grp, Umeå, Sweden.
    Mindemark, Jonas
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry. Umeå Univ, Dept Phys, Organ Photon & Elect Grp, Umeå, Sweden.
    Edman, Ludvig
    Umeå Univ, Dept Phys, Organ Photon & Elect Grp, Umeå, Sweden.
    Publisher Correction: The Weak Microcavity as an Enabler for Bright and Fault-tolerant Light-emitting Electrochemical Cells2018In: Scientific Reports, ISSN 2045-2322, E-ISSN 2045-2322, Vol. 8, article id 8697Article in journal (Other academic)
  • 10.
    Lindh, E. Mattias
    et al.
    Umeå Univ, Dept Phys, Organ Photon & Elect Grp, Umeå, Sweden.
    Lundberg, Petter
    Umeå Univ, Dept Phys, Organ Photon & Elect Grp, Umeå, Sweden.
    Lanz, Thomas
    Umeå Univ, Dept Phys, Organ Photon & Elect Grp, Umeå, Sweden.
    Mindemark, Jonas
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry. Umeå Univ, Dept Phys, Organ Photon & Elect Grp, Umeå, Sweden.
    Edman, Ludvig
    Umeå Univ, Dept Phys, Organ Photon & Elect Grp, Umeå, Sweden.
    The Weak Microcavity as an Enabler for Bright and Fault-tolerant Light-emitting Electrochemical Cells2018In: Scientific Reports, ISSN 2045-2322, E-ISSN 2045-2322, Vol. 8, article id 6970Article in journal (Refereed)
    Abstract [en]

    The light-emitting electrochemical cell (LEC) is functional at substantial active-layer thickness, and is as such heralded for being fit for low-cost and fault-tolerant solution-based fabrication. We report here that this statement should be moderated, and that in order to obtain a strong luminous output, it is fundamentally important to fabricate LEC devices with a designed thickness of the active layer. By systematic experimentation and simulation, we demonstrate that weak optical microcavity effects are prominent in a common LEC system, and that the luminance and efficiency, as well as the emission color and the angular intensity, vary in a periodic manner with the active-layer thickness. Importantly, we demonstrate that high-performance light-emission can be attained from LEC devices with a significant active-layer thickness of 300 nm, which implies that low-cost solution-processed LECs are indeed a realistic option, provided that the device structure has been appropriately designed from an optical perspective.

  • 11.
    Mindemark, Jonas
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Electrolytes for High-Performance Light-Emitting Electrochemical Cells: Going from Polyethers to Oligocarbonates2018Conference paper (Refereed)
  • 12.
    Mindemark, Jonas
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Polymer Chemistry.
    Functional Cyclic Carbonate Monomers and Polycarbonates: Synthesis and Biomaterials Applications2012Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    The present work describes a selection of strategies for the synthesis of functional aliphatic polycarbonates. Using an end-group functionalization strategy, a series of DNA-binding cationic poly(trimethylene carbonate)s was synthesized for application as vectors for non-viral gene delivery. As the end-group functionality was identical in all polymers, the differences observed in DNA binding and in vitro transfection studies were directly related to the length of the hydrophobic poly(trimethylene carbonate) backbone and the number of functional end-groups. This enabled the use of this polymer system to explore the effects of structural elements on the gene delivery ability of cationic polymers, revealing striking differences between different materials, related to functionality and cationic charge density.

    In an effort to achieve more flexibility in the synthesis of functional polymers, polycarbonates were synthesized in which the functionalities were distributed along the polymer backbone. Through polymerization of a series of alkyl halide-functional six-membered cyclic carbonates, semicrystalline chloro- and bromo-functional homopolycarbonates were obtained. The tendency of the materials to form crystallites was related to the presence of alkyl as well as halide functionalities and ranged from polymers that crystallized from the melt to materials that only crystallized on precipitation from a solution. Semicrystallinity was also observed for random 1:1 copolymers of some of the monomers with trimethylene carbonate, suggesting a remarkable ability of repeating units originating from these monomers to form crystallites.

    For the further synthesis of functional monomers and polymers, azide-functional cyclic carbonates were synthesized from the bromo-functional monomers. These were used as starting materials for the click synthesis of triazole-functional cyclic carbonate monomers through Cu(I)-catalyzed azide–alkyne cycloaddition. The click chemistry strategy proved to be a viable route to obtain structurally diverse monomers starting from a few azide-functional precursors. This paves the way for facile synthesis of a wide range of novel functional cyclic carbonate monomers and polycarbonates, limited only by the availability of suitable functional alkynes.

    List of papers
    1. Efficient DNA Binding and Condensation Using Low Molecular Weight, Low Charge Density Cationic Polymer Amphiphiles
    Open this publication in new window or tab >>Efficient DNA Binding and Condensation Using Low Molecular Weight, Low Charge Density Cationic Polymer Amphiphiles
    2010 (English)In: Macromolecular rapid communications, ISSN 1022-1336, E-ISSN 1521-3927, Vol. 31, no 15, p. 1378-1382Article in journal (Refereed) Published
    Abstract [en]

    A new class of biodegradable cationic macromolecules for DNA binding and condensation was developed by end-group-functionalization of poly(trimethylene carbonate). A series of one- and two-armed structures was synthesized and their interaction with DNA was evaluated. To aid data interpretation, a non-linear modeling method was applied to show efficient DNA binding that was intimately related to cationic charge density and macromolecular architecture. One-armed, low charge density structures were consistently found to bind to DNA at lower charge ratios than their two-armed, high charge density counterparts. This suggests that polymer backbone structure and characteristics are important considerations in the development of efficient cationic polymer systems for DNA condensation and delivery.

    Keywords
    DNA condensation, gene delivery, ionomers, polyplexes, self-assembly
    National Category
    Polymer Chemistry
    Research subject
    Chemistry with specialization in Polymer Chemistry
    Identifiers
    urn:nbn:se:uu:diva-135391 (URN)10.1002/marc.201000141 (DOI)000280944700011 ()
    Available from: 2010-12-07 Created: 2010-12-06 Last updated: 2017-12-11Bibliographically approved
    2. Low Charge Density Cationic Polymers for Gene Delivery: Exploring the Influence of Structural Elements on In Vitro Transfection
    Open this publication in new window or tab >>Low Charge Density Cationic Polymers for Gene Delivery: Exploring the Influence of Structural Elements on In Vitro Transfection
    2012 (English)In: Macromolecular Bioscience, ISSN 1616-5187, E-ISSN 1616-5195, Vol. 12, no 6, p. 840-848Article in journal (Refereed) Published
    Abstract [en]

    A series of end-functionalized poly(trimethylene carbonate) DNA carriers, characterized by low cationic charge density and pronounced hydrophobicity, was used to study structural effects on in vitro gene delivery. As the DNA-binding moieties were identical in all polymer structures, the differences observed between the different polymers were directly related to the functionality and length of the polymer backbone. The transfection efficiency and cytotoxicity of the polymer/DNA complexes were thus found to be dependent on a combination of polymer charge density and functionality, highlighting the importance of such structural considerations in the development of materials for efficient gene delivery.

    Place, publisher, year, edition, pages
    Wiley-VCH Verlagsgesellschaft, 2012
    Keywords
    amphiphiles, biodegradable, biological applications of polymers, gene delivery, transfection
    National Category
    Polymer Chemistry Biochemistry and Molecular Biology
    Research subject
    Chemistry with specialization in Polymer Chemistry
    Identifiers
    urn:nbn:se:uu:diva-169673 (URN)10.1002/mabi.201100480 (DOI)000304711200014 ()
    Available from: 2012-03-05 Created: 2012-03-05 Last updated: 2017-12-07Bibliographically approved
    3. Synthesis and polymerization of alkyl halide-functional cyclic carbonates
    Open this publication in new window or tab >>Synthesis and polymerization of alkyl halide-functional cyclic carbonates
    2011 (English)In: Polymer, ISSN 0032-3861, E-ISSN 1873-2291, Vol. 52, no 25, p. 5716-5722Article in journal (Refereed) Published
    Abstract [en]

    To increase the diversity in functional aliphatic polycarbonates, a series of novel chloro- and bromo-functional six-membered cyclic carbonate monomers were synthesized. Despite asymmetry in the monomer functionalities, homopolymerization of the monomers afforded semicrystalline polycarbonates with a high tendency to crystallize from the melt and/or on precipitation from a THF solution. Melting points were found in the 90-105 degrees C or 120-155 degrees C range for polymers comprising methyl or ethyl moieties, respectively, in the backbone. The monomers were further copolymerized with trimethylene carbonate to form random copolymers. Even among some of these random copolymers elements of semicrystallinity were found as confirmed by melting endotherms in DSC. The results clearly show that the incorporation of alkyl halide functionalities in aliphatic polycarbonates may lead to materials with a high ability to form crystallites, even in random copolymers, likely driven by polar interactions due to the presence of the halide functionalities.

    Keywords
    Cyclic carbonate monomers, Polycarbonates, Semicrystalline polymers
    National Category
    Chemical Sciences Polymer Chemistry
    Research subject
    Chemistry with specialization in Polymer Chemistry
    Identifiers
    urn:nbn:se:uu:diva-165694 (URN)10.1016/j.polymer.2011.10.027 (DOI)000297539000004 ()
    Available from: 2012-01-10 Created: 2012-01-09 Last updated: 2017-12-08Bibliographically approved
    4. Diversity in cyclic carbonates: Synthesis of triazole-functional monomers using click chemistry
    Open this publication in new window or tab >>Diversity in cyclic carbonates: Synthesis of triazole-functional monomers using click chemistry
    2012 (English)In: Polymer Chemistry, ISSN 1759-9962, Vol. 3, no 6, p. 1399-1401Article in journal (Refereed) Published
    Abstract [en]

    Triazole-functional cyclic carbonates are presented as a new class of functional monomers for ring-opening polymerisation. Starting from bromo-functional six-membered cyclic carbonates, a series of triazole-functional monomers was synthesised using click chemistry. This synthetic strategy allows for facile synthesis of a great number of structurally diverse monomers from just a few azide-functional precursors.

    Place, publisher, year, edition, pages
    Royal Society of Chemistry, 2012
    National Category
    Polymer Chemistry
    Research subject
    Chemistry with specialization in Polymer Chemistry
    Identifiers
    urn:nbn:se:uu:diva-169676 (URN)10.1039/C2PY20152F (DOI)000303773600005 ()
    Available from: 2012-03-13 Created: 2012-03-05 Last updated: 2013-01-08Bibliographically approved
  • 13.
    Mindemark, Jonas
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Polymer Chemistry.
    Bowden, Tim
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Polymer Chemistry.
    Diversity in cyclic carbonates: Synthesis of triazole-functional monomers using click chemistry2012In: Polymer Chemistry, ISSN 1759-9962, Vol. 3, no 6, p. 1399-1401Article in journal (Refereed)
    Abstract [en]

    Triazole-functional cyclic carbonates are presented as a new class of functional monomers for ring-opening polymerisation. Starting from bromo-functional six-membered cyclic carbonates, a series of triazole-functional monomers was synthesised using click chemistry. This synthetic strategy allows for facile synthesis of a great number of structurally diverse monomers from just a few azide-functional precursors.

  • 14.
    Mindemark, Jonas
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Materials Chemistry, Polymer Chemistry.
    Bowden, Tim
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Materials Chemistry, Polymer Chemistry.
    Efficient DNA Binding and Condensation Using Low Molecular Weight, Low Charge Density Cationic Polymer Amphiphiles2010In: Macromolecular rapid communications, ISSN 1022-1336, E-ISSN 1521-3927, Vol. 31, no 15, p. 1378-1382Article in journal (Refereed)
    Abstract [en]

    A new class of biodegradable cationic macromolecules for DNA binding and condensation was developed by end-group-functionalization of poly(trimethylene carbonate). A series of one- and two-armed structures was synthesized and their interaction with DNA was evaluated. To aid data interpretation, a non-linear modeling method was applied to show efficient DNA binding that was intimately related to cationic charge density and macromolecular architecture. One-armed, low charge density structures were consistently found to bind to DNA at lower charge ratios than their two-armed, high charge density counterparts. This suggests that polymer backbone structure and characteristics are important considerations in the development of efficient cationic polymer systems for DNA condensation and delivery.

  • 15.
    Mindemark, Jonas
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Materials Chemistry, Polymer Chemistry.
    Bowden, Tim
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Materials Chemistry, Polymer Chemistry.
    Low molecular weight, low charge density cationic polymers for gene delivery2009In: Frontiers in Polymer Science, Mainz, Tyskland 7–9 juni 2009, 2009Conference paper (Refereed)
  • 16.
    Mindemark, Jonas
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Materials Chemistry, Polymer Chemistry.
    Bowden, Tim
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Materials Chemistry, Polymer Chemistry.
    Novel Alkyl Halide-functional Polycarbonates and the Synthesis of Functional Cyclic Carbonate Monomers using Click Chemistry2011Conference paper (Refereed)
  • 17.
    Mindemark, Jonas
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Materials Chemistry, Polymer Chemistry.
    Bowden, Tim
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Materials Chemistry, Polymer Chemistry.
    Synthesis and polymerization of alkyl halide-functional cyclic carbonates2011In: Polymer, ISSN 0032-3861, E-ISSN 1873-2291, Vol. 52, no 25, p. 5716-5722Article in journal (Refereed)
    Abstract [en]

    To increase the diversity in functional aliphatic polycarbonates, a series of novel chloro- and bromo-functional six-membered cyclic carbonate monomers were synthesized. Despite asymmetry in the monomer functionalities, homopolymerization of the monomers afforded semicrystalline polycarbonates with a high tendency to crystallize from the melt and/or on precipitation from a THF solution. Melting points were found in the 90-105 degrees C or 120-155 degrees C range for polymers comprising methyl or ethyl moieties, respectively, in the backbone. The monomers were further copolymerized with trimethylene carbonate to form random copolymers. Even among some of these random copolymers elements of semicrystallinity were found as confirmed by melting endotherms in DSC. The results clearly show that the incorporation of alkyl halide functionalities in aliphatic polycarbonates may lead to materials with a high ability to form crystallites, even in random copolymers, likely driven by polar interactions due to the presence of the halide functionalities.

  • 18.
    Mindemark, Jonas
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry. Umea Univ, Dept Phys, Organ Photon & Elect Grp, SE-90187 Umea, Sweden..
    Edman, L.
    Umea Univ, Dept Phys, Organ Photon & Elect Grp, SE-90187 Umea, Sweden..
    Illuminating the electrolyte in light-emitting electrochemical cells2016In: Journal of Materials Chemistry C, ISSN 2050-7526, E-ISSN 2050-7534, Vol. 4, no 3, p. 420-432Article, review/survey (Refereed)
    Abstract [en]

    Light-emitting electrochemical cells (LECs) convert electric current to light within an active material comprising an electroluminescent organic semiconductor and an electrolyte. It is well established that it is the presence of this electrolyte that enabled the recent development of low-cost fabrication methods of functional LECs as well as the realisation of unique device architectures. At the same time, it should be acknowledged that the current lower performance of LECs in comparison to the more commonplace organic light-emitting diode, at least in part, is intimately linked to the utilisation of non-ideal electrolytes. In this review, we present the tasks that the electrolyte should fulfil during the various stages of LEC operation, and how the characteristics of the electrolyte can affect the LEC performance, specifically the turn-on time, the efficiency and the operational stability. We thereafter introduce the different classes of electrolytes that have been implemented in LEC devices up to date, and discuss how these electrolytes have been able to meet the specific requirements of the LEC technology.

  • 19.
    Mindemark, Jonas
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Materials Chemistry, Polymer Chemistry.
    Hilborn, Jöns
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Materials Chemistry, Polymer Chemistry.
    Bowden, Tim
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Materials Chemistry, Polymer Chemistry.
    End-Group-Catalyzed Ring-Opening Polymerization of Trimethylene Carbonate2007In: Macromolecules, ISSN 0024-9297, E-ISSN 1520-5835, Vol. 40, no 10, p. 3515-3517Article in journal (Refereed)
    Abstract [en]

    A controlled self-catalyzed polymerization reaction yielding well-defined heterotelechelic polymer chains and eliminating low molecular weight catalyst residues in the final polymer product were analyzed by utilizing a ternary amine. The molecular weights were kept relatively low for end-group analysis by Nuclear Magnetic Resonance spectroscopy (NMR) and linear correlation between the degree of polarization and monomer were found. NMR results show that the polydispersities remained low at high monomer conversions and longer reaction times after full conversion led to a larger molecular weight distribution. The results also show that the ternary amine catalyst are attached to the growing polymer chains that is shown by a downfield shift from 2.44 to 2.56 ppm. The benzoic acid ester of the ternary amine is found to be potent catalyst of Ring-Opening Polymerization (ROP).

  • 20.
    Mindemark, Jonas
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Imholt, Laura
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry. Uppsala Univ, Dept Chem, Angstrom Lab, SE-75121 Uppsala, Sweden..
    Synthesis of high molecular flexibility polycarbonates for solid polymer electrolytes2015In: Electrochimica Acta, ISSN 0013-4686, E-ISSN 1873-3859, Vol. 175, p. 247-253Article in journal (Refereed)
    Abstract [en]

    A new self-plasticizing aliphatic polycarbonate comprising flexible alkyl and alkyl ether side groups was designed and synthesized from six-membered cyclic carbonate monomers with the aim of producing a material with high molecular flexibility (low T-g)and concomitant high ionic conductivity when used as a polymer electrolyte. The T-g of the novel polycarbonate was determined to be -49.4 degrees C at a molecular weight of 34 400 g mol(-1), which is the lowest reported T-g to date for a substituted poly(trimethylene carbonate). UV-crosslinked polymer electrolytes were produced based on this novel material together with LiTFSI salt and showed ionic conductivities in the range of 2 x 10(-8) to 2 x 10(-7) S cm(-1) at room temperature and 1 x 10(-6) to 1 x 10(-5) S cm(-1) at 100 degrees C. The limited ionic conductivities of these electrolytes indicate that high molecular flexibility alone does not guarantee fast ion transport in solid polymer electrolytes and that other factors, such as the polarity of the polymer host material, will also influence the transport properties of the electrolyte.

  • 21.
    Mindemark, Jonas
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Lacey, Matthew J.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Bowden, Tim
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Polymer Chemistry.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Beyond PEO-Alternative host materials for Li+-conducting solid polymer electrolytes2018In: Progress in polymer science, ISSN 0079-6700, E-ISSN 1873-1619, Vol. 81, p. 114-143Article, review/survey (Refereed)
    Abstract [en]

    The bulk of the scientific literature on Li-conducting solid (solvent-free) polymer electrolytes (SPEs) for applications such as Li-based batteries is focused on polyether-based materials, not least the archetypal poly(ethylene oxide) (PEO). A significant number of alternative polymer hosts have, however, been explored over the years, encompassing materials such as polycarbonates, polyesters, polynitriles, polyalcohols and polyamines. These display fundamentally different properties to those of polyethers, and might therefore be able to resolve the key issues restricting SPEs from realizing their full potential, for example in terms of ionic conductivity, chemical or electrochemical stability and temperature sensitivity. It is further interesting that many of these polymer materials complex Li-ions less strongly than PEO and facilitate ion transport through different mechanisms than polyethers, which is likely critical for true advancement in the area. In this review, >30 years of research on these 'alternative' Li-ion-conducting SPE host materials are summarized and discussed in the perspective of their potential application in electrochemical devices, with a clear focus on Li batteries. Key challenges and strategies forward and beyond the current PEO-based paradigm are highlighted.

  • 22.
    Mindemark, Jonas
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Mogensen, Ronnie
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Smith, Michael J.
    Univ Minho, Ctr Quim, P-4710057 Braga, Portugal..
    Silva, Maria Manuela
    Univ Minho, Ctr Quim, P-4710057 Braga, Portugal..
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Polycarbonates as alternative electrolyte host materials for solid-state sodium batteries2017In: Electrochemistry communications, ISSN 1388-2481, E-ISSN 1873-1902, Vol. 77, p. 58-61Article in journal (Refereed)
    Abstract [en]

    This paper describes the first implementation of the aliphatic polycarbonate PTMC- that has previously been successfully applied to lithium polymer batteries- as a non-polyether host matrix in solid-state sodium batteries. Despite higher glass transition temperatures of PTMC-NaTFSI and PTMC-NaClO4 electrolytes than their Li-containing counterparts, the ionic conductivities were found to be similar to the equivalent Li salt electrolytes. Finally, the functionality of PTMC-NaTESI was demonstrated through cycling of Na/Prussian blue half-cells displaying high discharge capacities and limited polarization at C/10 and 60 degrees C.

  • 23.
    Mindemark, Jonas
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Sobkowiak, Adam
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Oltean, Gabriel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Gustafsson, Torbjörn
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Mechanical Stabilization of Solid Polymer Electrolytes through Gamma Irradiation2017In: Electrochimica Acta, ISSN 0013-4686, E-ISSN 1873-3859, Vol. 230, p. 189-195Article in journal (Refereed)
    Abstract [en]

    Attaining sufficient mechanical stability is a challenge for high-performance solid polymer electrolytes, particularly at elevated temperatures. We have here characterized the viscoelastic properties of the nonpolyether host material poly(epsilon-caprolactone-co-trimethylene carbonate) with and without incorporated LiTFSI salt. While this electrolyte material performs well at room temperature, at 80 degrees C the material is prone to viscous flow. Through gamma-irradiation at a dose of 25 kGy, the material stabilizes such that it behaves as a rubbery solid even at low rates of deformation while retaining a high ionic conductivity necessary for use in solid-state Li batteries. The performance of the irradiated electrolyte was investigated in Li polymer half-cells (Li vs. LiFePO4) at both 80 degrees C and room temperature. In Contrast with the notably stable battery performance at low temperatures using the non-irradiated material, during cycling of the irradiated electrolytes detrimental instabilities were noted at both 80 degrees C and room temperature. The possible effects of both radiation damage to the electrolyte and impaired interfacial contacts due to the crosslinking indicate that a different procedure may be necessary in order to stabilize these electrolytes for use in battery cells capable of stable long-term operation.

  • 24.
    Mindemark, Jonas
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Sun, Bing
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Aliphatic Polycarbonates as Solid State Electrolytes for Lithium Ion Batteries2013Conference paper (Refereed)
    Abstract
  • 25.
    Mindemark, Jonas
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Sun, Bing
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Development of functional polycarbonate-based electrolytes for lithium-ion batteries2014Conference paper (Refereed)
    Abstract
  • 26.
    Mindemark, Jonas
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Sun, Bing
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Hydroxyl-functionalized poly(trimethylene carbonate) electrolytes for 3D-electrode configurations2015In: Polymer Chemistry, ISSN 1759-9954, E-ISSN 1759-9962, Vol. 6, no 26, p. 4766-4774Article in journal (Refereed)
    Abstract [en]

    Polymer electrolytes were prepared from an aliphatic polycarbonate with 10 mol% of repeating units having a hydroxyl-functional side group, with the addition of LiTFSI salt. The hydrogen bond-interacting side groups were found to be beneficial for improving adhesion to 2D planar electrode material surfaces. These favorable surface properties proved to be valid also for 3D-structured systems since thin, conformal coatings could be cast on 3D-microstructured electrodes. In addition, the electrolytes were found to have reasonable ionic conductivity (up to 2.7 x 10(-8) S cm(-1) at 25 degrees C and 2.3 x 10(-6) S cm(-1) at 60 degrees C) that was almost independent of salt concentration. This demonstrates how a hydroxyl-functional polymer approach is suitable for the creation of 3D-structured electrode-electrolyte assemblies for microbattery applications.

  • 27.
    Mindemark, Jonas
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Sun, Bing
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Long-term stability of polycarbonate-based solid polymer electrolytes: 1-year anniversary of the first PTMC Li-ion cel2013Conference paper (Refereed)
    Abstract
  • 28.
    Mindemark, Jonas
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Sun, Bing
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Progress towards all-solid lithium polymer batteries: Solid polymer electrolytes for battery cells operated at room temperature2015Conference paper (Other academic)
    Abstract
  • 29.
    Mindemark, Jonas
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Sun, Bing
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Törmä, Erik
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    High-performance solid polymer electrolytes for lithium batteries operational at ambient temperature2015In: Journal of Power Sources, ISSN 0378-7753, E-ISSN 1873-2755, Vol. 298, p. 166-170Article in journal (Refereed)
    Abstract [en]

    Incorporation of carbonate repeating units in a poly(epsilon-caprolactone) (PCL) backbone used as a host material in solid polymer electrolytes is found to not only suppress crystallinity in the polyester material, but also give higher ionic conductivity in a wide temperature range exceeding the melting point of PCL crystallites. Combined with high cation transference numbers, this electrolyte material has sufficient lithium transport properties to be used in battery cells that are operational at temperatures down to below 23 degrees C, thus clearly demonstrating the potential of using non-polyether electrolytes in high-performance all-solid lithium polymer batteries.

  • 30.
    Mindemark, Jonas
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Polymer Chemistry.
    Tabata, Yasuhiko
    Department of Biomaterials, Institute for Frontier Medical Sciences, Kyoto University.
    Bowden, Tim
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Polymer Chemistry.
    Low Charge Density Cationic Polymers for Gene Delivery: Exploring the Influence of Structural Elements on In Vitro Transfection2012In: Macromolecular Bioscience, ISSN 1616-5187, E-ISSN 1616-5195, Vol. 12, no 6, p. 840-848Article in journal (Refereed)
    Abstract [en]

    A series of end-functionalized poly(trimethylene carbonate) DNA carriers, characterized by low cationic charge density and pronounced hydrophobicity, was used to study structural effects on in vitro gene delivery. As the DNA-binding moieties were identical in all polymer structures, the differences observed between the different polymers were directly related to the functionality and length of the polymer backbone. The transfection efficiency and cytotoxicity of the polymer/DNA complexes were thus found to be dependent on a combination of polymer charge density and functionality, highlighting the importance of such structural considerations in the development of materials for efficient gene delivery.

  • 31.
    Mindemark, Jonas
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Tang, Shi
    Umeå universitet.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Edman, Ludvig
    Umeå universitet.
    Improving the Performance of Light-Emitting Electrochemical Cells through Electrolyte End-Group Modification2014Conference paper (Refereed)
    Abstract
  • 32.
    Mindemark, Jonas
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry. Umea Univ, Dept Phys, Organ Photon & Elect Grp, SE-90187 Umea, Sweden..
    Tang, Shi
    Umea Univ, Dept Phys, Organ Photon & Elect Grp, SE-90187 Umea, Sweden.;LunaLEC AB, Tvistevagen 47, SE-90719 Umea, Sweden..
    Li, Hu
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Applied Materials Sciences.
    Edman, Ludvig
    Umea Univ, Dept Phys, Organ Photon & Elect Grp, SE-90187 Umea, Sweden.;LunaLEC AB, Tvistevagen 47, SE-90719 Umea, Sweden..
    Ion Transport beyond the Polyether Paradigm: Introducing Oligocarbonate Ion Transporters for Efficient Light-Emitting Electrochemical Cells2018In: Advanced Functional Materials, ISSN 1616-301X, E-ISSN 1616-3028, Vol. 28, no 32, article id 1801295Article in journal (Refereed)
    Abstract [en]

    The light-emitting electrochemical cell (LEC) is fundamentally dependent on mobile ions for its operation. In polymer LECs, the mobile ions are commonly provided by dissolving a salt in an ion transporter, with the latter almost invariably being an ether-based compound. Here, the synthesis, characterization, and application of a new class of carbonate-based ion transporters are reported. A polymer LEC, comprising a star-branched oligocarbonate endowed with aliphatic side groups as the ion transporter, features a current efficacy of 13.8 cd A(-1) at a luminance of 1060 cd m(-2), which is a record-high efficiency/luminance combination for a singlet-emitting LEC. It is further established that the design principles of a high-performance carbonate ion transporter constitute the selection of an oligomeric structure over a corresponding polymeric structure and the endowment of the oligomer with functional side chains to render it compatible with the polymeric emitter.

  • 33.
    Mindemark, Jonas
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry. Umea Univ, Dept Phys, Organ Photon & Elect Grp, SE-90187 Umea, Sweden..
    Tang, Shi
    Umea Univ, Dept Phys, Organ Photon & Elect Grp, SE-90187 Umea, Sweden..
    Wang, Jia
    Umea Univ, Dept Phys, Organ Photon & Elect Grp, SE-90187 Umea, Sweden..
    Kaihovirta, Nikolai
    Umea Univ, Dept Phys, Organ Photon & Elect Grp, SE-90187 Umea, Sweden..
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Edman, Ludvig
    Umea Univ, Dept Phys, Organ Photon & Elect Grp, SE-90187 Umea, Sweden..
    High-Performance Light-Emitting Electrochemical Cells by Electrolyte Design2016In: Chemistry of Materials, ISSN 0897-4756, E-ISSN 1520-5002, Vol. 28, no 8, p. 2618-2623Article in journal (Refereed)
    Abstract [en]

    Polymer light-emitting electrochemical cells (LECs) are inherently dependent on a suitable electrolyte for proper function. Here, we design and synthesize a series of alkyl carbonate-capped star-branched oligoether-based electrolytes with large electrochemical stability windows, facile ion release, and high compatibility with common light-emitting materials. LECs based on such designed electrolytes feature fast turn-on, a long operational lifetime of 1400 h at >100 cd m(-2) and a record-high power conversion efficiency of 18.1 lm W-1, when equipped with an external outcoupling film.

  • 34.
    Mindemark, Jonas
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Törmä, Erik
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Sun, Bing
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Copolymers of trimethylene carbonate and epsilon-caprolactone as electrolytes for lithium-ion batteries2015In: Polymer, ISSN 0032-3861, E-ISSN 1873-2291, Vol. 63, p. 91-98Article in journal (Refereed)
    Abstract [en]

    Random copolymers of trimethylene carbonate (TMC) and epsilon-caprolactone (CL) were synthesized through bulk ring-opening polymerization for use as host materials for solid polymer electrolytes. Amorphous electrolytes were solution-cast from the copolymers together with LiTFSI salt and showed lower T-g and higher ionic conductivity as the CL content was increased. The best-performing electrolyte, with a TMC:CL ratio of 60:40 with 28 wt% of LiTFSI, was found to have a conductivity of 1.6 x 10(-5) S cm(-1) at 60 degrees C (7.9 x 10(-7) S cm(-1) at 25 degrees C) and a T-g of -26 degrees C. This electrolyte was used in all-solid-state LiFePO4 half-cells that showed high capacity and coulombic efficiency at rates up to and including C/5.

  • 35.
    Qiu, Zhengfu
    et al.
    Shanghai Univ, Sch Mat Sci & Engn, Shanghai 200444, Peoples R China;Shanghai Univ, Res Ctr Nanosci & Nanotechnol, Shanghai 200444, Peoples R China.
    Shi, Liyi
    Shanghai Univ, Res Ctr Nanosci & Nanotechnol, Shanghai 200444, Peoples R China.
    Wang, Zhuyi
    Shanghai Univ, Res Ctr Nanosci & Nanotechnol, Shanghai 200444, Peoples R China.
    Mindemark, Jonas
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Zhu, Jie-Fang
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Edström, Kristina
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Zhao, Yin
    Shanghai Univ, Res Ctr Nanosci & Nanotechnol, Shanghai 200444, Peoples R China.
    Yuan, Shuai
    Shanghai Univ, Res Ctr Nanosci & Nanotechnol, Shanghai 200444, Peoples R China;Shanghai Univ, Emerging Ind Inst, Jinxing 314006, Zhejiang, Peoples R China.
    Surface activated polyethylene separator promoting Li+ ion transport in gel polymer electrolytes and cycling stability of Li-metal anode2019In: Chemical Engineering Journal, ISSN 1385-8947, E-ISSN 1873-3212, Vol. 368, p. 321-330Article in journal (Refereed)
    Abstract [en]

    This paper proposes a strategy to fabricate surface activated polyethylene (PE)-supported gel polymer electrolyte (GPE) with high ion transport ability, excellent electrolyte retention and mechanical properties to stabilize lithium (Li)-metal anodes. The inert outer and inner pore surface activation of polyethylene is demonstrated by coating an ultrathin zirconium oxide nanocrystal (ZrO2)/polyhedral oligomeric silsesquioxane (POSS) composite layer through a simple layer by layer (LBL) assembly method prior to the in situ polymerization. It is found that the activation layer may improve the Li+ ion transference number and induce the formation of GPE with a gradient structure by the interaction with the initiator system, giving rise to higher ion transport ability of final GPE. On the other hand, the GPE using the activated PE separator as support improves the Li/electrolyte interfacial stability during storage and repeated lithium plating/stripping cycling. A stable voltage profile with cycling for more than 800 h in a Li/Li symmetric cell was obtained by using surface activated PE-supported GPE. When it is assembled into the cells with metallic lithium anodes and lithium cobalt oxide (LiCoO2) cathodes, the cells show excellent rate capability and cycling performance, as well as effective dendrite inhibition.

  • 36. Saxena, Shalini
    et al.
    Ray, Alok R.
    Mindemark, Jonas
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Materials Chemistry, Polymer Chemistry.
    Hilborn, Jöns
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Materials Chemistry, Polymer Chemistry.
    Gupta, Bhuvanesh
    Plasma-Induced Graft Polymerization of Acrylic Acid onto Poly(propylene) Monofilament: Characterization2010In: Plasma Processes and Polymers, ISSN 1612-8850, Vol. 7, no 7, p. 610-618Article in journal (Refereed)
    Abstract [en]

    Poly(propylene) (PP) filaments were functionalized by plasma-grafting of acrylic acid and the characterization of the grafted filaments was carried out using various techniques. XPS content which causes a decrease in the analysis showed an increase in the oxygenated contact angle decreased from 88 for virgin PP to 28 for the filament with the maximum graft level. The storage of the samples leads to the loss in hydrophilicity. The grafts do not lead to any crystalline changes in the filament structure; significant changes however occur on the surface of the filaments as a function of the degree of grafting.

  • 37.
    Sun, Bing
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry. Paul Scherrer Inst, Electrochem Lab, Electrochem Energy Storage Sect, CH-5232 Villigen, Switzerland.
    Asfaw, Habtom Desta
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry. Imperial Coll London, Dept Chem, London SW7 2AZ, England.
    Rehnlund, David
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Inorganic Chemistry.
    Mindemark, Jonas
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Nyholm, Leif
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Inorganic Chemistry.
    Edström, Kristina
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Towards Solid-State 3D-Microbatteries using Functionalized Polycarbonate-based Polymer Electrolytes2018In: ACS Applied Materials and Interfaces, ISSN 1944-8244, E-ISSN 1944-8252, Vol. 10, no 3, p. 2407-2413Article in journal (Refereed)
    Abstract [en]

    3D-microbatteries (3D-MBs) impose new demands for theselection, fabrication and compatibility of the different battery components, notleast the electrolytes. Herein, solid polymer electrolytes (SPEs) based on poly(trimethylene carbonate) (PTMC) have been implemented in 3D-MB systems. 3D electrodes of two different architectures, LiFePO4-coated carbon foams and Cu2O-coated Cu nanopillars, have been coated with SPEs and used in Li-cells. Functionalized PTMC with hydroxyl end groups was found to enable uniform and well-covering coatings on LiFePO4-coated carbon foams, although the cell cycling performance was limited by the large SPE resistance. By employing a SPE prepared from a copolymer of TMC and caprolactone (CL), with higher ionic conductivity, Li-cells composed of Cu2O-coated Cu nanopillars were constructed and tested both at room temperature and 60 °C. The footprint areal capacity of the cells was ca. 0.02 mAh cm-2 for an area gain factor (AF) of 2.5, and 0.2 mAh cm-2 for a relatively dense nanopillar-array (AF=25) at a current density of 0.008 mA cm-2at ambient temperature (22±1 °C). These results provide new routes towards the realization of all-solid-state 3D-MBs.

  • 38.
    Sun, Bing
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Mindemark, Jonas
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Edström, Kristina
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Polycarbonate-based solid polymer electrolytes for Li-ion batteries2014In: Solid State Ionics, ISSN 0167-2738, E-ISSN 1872-7689, Vol. 262, p. 738-742Article in journal (Refereed)
    Abstract [en]

    This paper reports the synthesis and application of high-molecular-weight poly(trimethylene carbonate) (PTMC) as a new host material for solid polymer electrolyte-based Li-ion batteries. PTMC was synthesized through bulk ring-opening polymerization of the cyclic monomer to yield a high-molecular-weight polymer to serve as a base material for the electrolytes. The thermal properties and ionic conductivity of polymer electrolytes with different salt ratios were measured by TGA/DSC and electrochemical impedance spectroscopy, respectively. The most conductive systems were found at [Li+]:[carbonate] ratios of 1:13 and 1:8, which showed electrochemical stability up to 5.0 V vs. Li/Li+ and an ionic conductivity on the order of 10− 7 Scm(-1) at 60 °C. LiFePO4 half-cells using the electrolytes demonstrated a plateau in the specific discharge capacity around 153 mAhg(-1) after long-term cycling. The functionality of the electrolytes for three-dimensional microbatteries was also confirmed.

  • 39.
    Sun, Bing
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Mindemark, Jonas
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Edström, Kristina
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Realization of high performance polycarbonate-based Li polymer batteries2015In: Electrochemistry communications, ISSN 1388-2481, E-ISSN 1873-1902, Vol. 52, p. 71-74Article in journal (Refereed)
  • 40.
    Sun, Bing
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Mindemark, Jonas
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Morozov, Evgeny V.
    KTH Royal Inst Technol, Dept Chem, Div Appl Phys Chem, Teknikringen 36, SE-10044 Stockholm, Sweden.
    Costa, Luciano T.
    Univ Fed Fluminense, Inst Quim, Dept Quim Fis, Outeiro Sao Joao Batista S-N, BR-24020150 Niteroi, RJ, Brazil.
    Bergman, Martin
    Chalmers, Dept Phys, SE-41296 Gothenburg, Sweden.
    Johansson, Patrik
    Chalmers, Dept Phys, SE-41296 Gothenburg, Sweden.
    Fang, Yuan
    KTH Royal Inst Technol, Dept Chem, Div Appl Phys Chem, Teknikringen 36, SE-10044 Stockholm, Sweden.
    Furó, István
    KTH Royal Inst Technol, Dept Chem, Div Appl Phys Chem, Teknikringen 36, SE-10044 Stockholm, Sweden.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Ion transport in polycarbonate based solid polymer electrolytes: experimental and computational investigations2016In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 18, no 14, p. 9504-9513Article in journal (Refereed)
    Abstract [en]

    Among the alternative host materials for solid polymer electrolytes (SPEs), polycarbonates have recently shown promising functionality in all-solid-state lithium batteries from ambient to elevated temperatures. While the computational and experimental investigations of ion conduction in conventional polyethers have been extensive, the ion transport in polycarbonates has been much less studied. The present work investigates the ionic transport behavior in SPEs based on poly(trimethylene carbonate) (PTMC) and its co-polymer with epsilon-caprolactone (CL) via both experimental and computational approaches. FTIR spectra indicated a preferential local coordination between Li+ and ester carbonyl oxygen atoms in the P(TMC20CL80) co-polymer SPE. Diffusion NMR revealed that the co-polymer SPE also displays higher ion mobilities than PTMC. For both systems, locally oriented polymer domains, a few hundred nanometers in size and with limited connections between them, were inferred from the NMR spin relaxation and diffusion data. Potentiostatic polarization experiments revealed notably higher cationic transference numbers in the polycarbonate based SPEs as compared to conventional polyether based SPEs. In addition, MD simulations provided atomic-scale insight into the structure-dynamics properties, including confirmation of a preferential Li+-carbonyl oxygen atom coordination, with a preference in coordination to the ester based monomers. A coupling of the Li-ion dynamics to the polymer chain dynamics was indicated by both simulations and experiments.

  • 41.
    Sun, Bing
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Xu, Chao
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Mindemark, Jonas
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Bowden, Tim
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Novel solid polymer electrolytes for large and small Li-battery applications2013Conference paper (Other academic)
  • 42.
    Sun, Bing
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Xu, Chao
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Mindemark, Jonas
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Gustafsson, Torbjörn
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Edström, Kristina
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    At the polymer electrolyte interfaces: the role of the polymer host in interphase layer formation in Li-batteries2015In: Journal of Materials Chemistry A, ISSN 2050-7488, Vol. 3, no 26, p. 13994-14000Article in journal (Refereed)
    Abstract [en]

    In this study, X-ray photoelectron spectroscopy was applied for compositional analysis of the interphase layers formed in graphite and LiFePO4 Li-battery half cells containing solid polymer electrolytes (SPEs) consisting of poly(trimethylene carbonate) (PTMC) and LiTFSI salt. Decomposition of PTMC was observed at the anode/SPE interface, indicating different reaction products than those associated with the more conventional host material poly(ethylene oxide). Degradation mechanisms of the PTMC host material at low potentials are proposed. Compared to the LiFePO4/PEO interface, the absence of LiOH - a result of water contamination - was generally seen when using hydrophobic PTMC as the polymer host. A clear correlation of moisture content with the constitution of interphase layers in Li polymer batteries could thus be concluded. At the SPE/LiFePO4 interface, good stability was seen regardless of the polymer host materials.

  • 43.
    Sångeland, Christofer
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Mindemark, Jonas
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Polymer Chemistry. Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Younesi, Reza
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Polycarbonate/Polyester-Based Polymer Electrolyte Used in All-Solid-State Sodium-Ion Batteries – How are Cells Constructed?2018Conference paper (Other academic)
  • 44.
    Sångeland, Christofer
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Mindemark, Jonas
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Polymer Chemistry. Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Younesi, Reza
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Polyester/polycarbonate-based polymer electrolyte for sodium ion battery applications2018Conference paper (Other academic)
  • 45.
    Sångeland, Christofer
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Mindemark, Jonas
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Polymer Chemistry. Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Younesi, Reza
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Variations in optimal salt content depending on polycaprolactone-polycarbonate composition in polymer electrolytes2017Conference paper (Other academic)
  • 46.
    Sångeland, Christofer
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Mogensen, Ronnie
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Mindemark, Jonas
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Stable Cycling of Sodium Metal All-Solid-State Batteries with Polycarbonate-Based Polymer Electrolytes2019In: ACS APPLIED POLYMER MATERIALS, ISSN 2637-6105, Vol. 1, no 4, p. 825-832Article in journal (Refereed)
    Abstract [en]

    Solid polymer electrolytes based on high-molecular-weight poly(trimethylene carbonate) (PTMC) in combination with NaFSI salt were investigated for application in sodium batteries. The polycarbonate host material proved to be able to dissolve large amounts of salt, at least up to a carbonate:Na+ ratio of 1:1. Combined DSC, conductivity, and FTIR data indicated the formation of a percolating network of salt clusters along with the transition to a percolation-type ion transport mechanism at the highest salt concentrations. While the highest total ionic conductivities were seen at the highest salt concentrations (up to a remarkable 5 x 10(-5) S cm(-1) at 25 degrees C at a 1:1 carbonate:Na+ ratio), the most stable battery performance was seen at a more moderate salt loading of 5:1 carbonate:Na+, reaching >80 cycles at a stable capacity of similar to 90 mAh g(-1) at 60 degrees C in a sodium metal/Prussian blue cell. The results highlight the importance of the choice of salt and salt concentration on electrolyte performance as well as demonstrate the potential of utilizing polycarbonate-based electrolytes in sodium-based energy storage systems.

  • 47.
    Sångeland, Christofer
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Younesi, Reza
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Mindemark, Jonas
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Towards room temperature operation of all-solid-state Na-ion batteries through polyester-polycarbonate-based polymer electrolytes2019In: ENERGY STORAGE MATERIALS, ISSN 2405-8297, Vol. 19, p. 31-38Article in journal (Refereed)
    Abstract [en]

    In an ambition to develop solid-state Na-ion batteries functional at ambient temperature, we here explore a novel electrolyte system. Polyester-polycarbonate (PCL-PTMC) copolymers were combined with sodium bis(fluorosulfonyl) imide salt (NaFSI) to form solid polymer electrolytes for Na-ion batteries. The PCL-PTMC:NaFSI system demonstrated glass transition temperatures ranging from -64 to -11 degrees C, increasing with increasing salt content from 0 to 35 wt%, and ionic conductivities ranging from 10(-8) to 10(-5) S cm(-1) at 25 degrees C. The optimal salt concentration was clearly dependent on the level of crystallinity, which was largely determined by the CL content. At 70 and 80 mol% CL, the PCL-PTMC:NaFSI system was fully amorphous and exhibited high conductivities at lower salt concentrations. When the CL content was increased to 100 mol%, high ionic conductivities were instead observed at high salt concentrations. A decent transference number of ca. 0.5 at 80 degrees C was obtained for a polymer film containing 20 mol% CL units and 25 wt% NaFSI. Finally, a HC vertical bar 80-20(25)vertical bar Na2-xFe(Fe(CN)(6)) all-solid-state polymer electrolyte full cell was assembled to demonstrate the practical application of the material and cycled for more than 120 cycles at similar to 22 degrees C.

  • 48. Tang, Shi
    et al.
    Mindemark, Jonas
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Araujo, Carlos Moyses Graca
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Theory.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Edman, Ludvig
    Identifying Key Properties of Electrolytes for Light-Emitting Electrochemical Cells2014In: Chemistry of Materials, ISSN 0897-4756, E-ISSN 1520-5002, Vol. 26, no 17, p. 5083-5088Article in journal (Refereed)
    Abstract [en]

    The electrolyte is a key component in light-emitting electrochemical cells (LECs), as it facilitates in situ electrochemical doping and associated attractive device features. LiCF3SO3 dissolved in hydroxyl-capped trimethylolpropane ethoxylate (TMPE-OH) constitutes an electrolyte with which we have attained high stability and efficiency for polymer LECs, but the turn-on time of such devices is unfortunately slow. By replacing hydroxyl with methoxy as the TMPE end-group, we produced LECs with a desired combination of high efficiency, good stability, and fast turn-on time. Specifically, we showed that the turn-on time to high luminance (300 cd/m(2)) at a current density of 7.7 mA/cm(2) is lowered from 1740 to 16 s, that the efficiency is improved by similar to 20%, and that the other device properties are either maintained or improved. In a parallel modeling and experimental effort, we demonstrated that the faster kinetics following the shift in the TMPE end-group is attributed to a marked decrease in the level of both inter- and intramolecular interactions of the electrolyte, as manifested in a lowered electrolyte viscosity, faster ion transport, and more facile ion release during doping.

  • 49.
    Xu, Chao
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry. Univ Cambridge, Dept Chem, Lensfield Rd, Cambridge CB2 1EW, England.
    Hernández, Guiomar
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Abbrent, Sabina
    Czech Acad Sci, Inst Macromol Chem, Heyrovskeho Nam 2, Prague 16206 6, Czech Republic.
    Kober, Libor
    Czech Acad Sci, Inst Macromol Chem, Heyrovskeho Nam 2, Prague 16206 6, Czech Republic.
    Konefal, Rafal
    Czech Acad Sci, Inst Macromol Chem, Heyrovskeho Nam 2, Prague 16206 6, Czech Republic.
    Brus, Jiri
    Czech Acad Sci, Inst Macromol Chem, Heyrovskeho Nam 2, Prague 16206 6, Czech Republic.
    Edström, Kristina
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Mindemark, Jonas
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Unraveling and Mitigating the Storage Instability of Fluoroethylene Carbonate-Containing LiPF6 Electrolytes To Stabilize Lithium Metal Anodes for High-Temperature Rechargeable Batteries2019In: ACS APPLIED ENERGY MATERIALS, ISSN 2574-0962, Vol. 2, no 7, p. 4925-4935Article in journal (Refereed)
    Abstract [en]

    Implementing Li metal anodes provides the potential of substantially boosting the energy density of current Li-ion battery technology. However, it suffers greatly from fast performance fading largely due to substantial volume change during cycling and the poor stability of the solid electrolyte interphase (SEI). Fluoroethylene carbonate (FEC) is widely acknowledged as an effective electrolyte additive for improving the cycling performance of batteries consisting of electrode materials that undergo large volume changes during cycling such as Li metal. In this study, we report that while FEC can form a robust SEI on the electrode, it also deteriorates the shelf life of electrolytes containing LiPF6. The degradation mechanism of LiPF6 in FEC solutions is unraveled by liquid-and solid-state NMR. Specifically, traces of water residues induce the hydrolysis of LiPF6, releasing HF and PF5 which further trigger ring-opening of FEC and its subsequent polymerization. These reactions are significantly accelerated at elevated temperatures leading to the formation of a three-dimensional fluorinated solid polymer network. Moisture scavenger additives, such as lithium 4,5-dicyano-2-(trifluoromethyl)imidazole (LiTDI), can delay the degradation reaction as well as improve the cycling stability of LiNi1/3Mn1/3Co1/3O2/Li metal batteries at 55 degrees C. This work highlights the poor shelf life of electrolytes containing FEC in combination with LiPF6 and thereby the great importance of developing proper storage methods as well as optimizing the content of FEC in practical cells.

  • 50.
    Åvall, Gustav
    et al.
    Chalmers Univ Technol, Dept Phys, SE-41296 Gothenburg, Sweden.
    Mindemark, Jonas
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Polymer Chemistry. Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Johansson, Patrik
    Chalmers Univ Technol, Dept Phys, SE-41296 Gothenburg, Sweden.
    Sodium-Ion Battery Electrolytes: Modeling and Simulations2018In: ADVANCED ENERGY MATERIALS, ISSN 1614-6832, Vol. 8, no 17, article id 1703036Article, review/survey (Refereed)
    Abstract [en]

    The authors review the efforts made from a modeling and simulation perspective in order to assist both the fundamental understanding as well as the development of higher performance sodium-ion battery (SIB) electrolytes. Depending on the type of the electrolyte studied, liquid, ionic liquid, polymer, glass, solid-state, etc., the simulation methods applied and the research questions in focus differ, but all contribute to more rational progress. Furthermore, the authors create cases of meta-analysis using literature data. A historical perspective is applied and the focus clearly is on more recent work and novel electrolyte materials. Finally, the authors outline a few prospective areas for where SIB electrolyte simulations can/should be extended for maximum impact in the field.

1 - 50 of 50
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