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  • 1.
    Abdellah, Mohamed
    et al.
    Lund Univ, Div Chem Phys, Box 124, S-22100 Lund, Sweden.;Lund Univ, NanoLund, Box 124, S-22100 Lund, Sweden.;South Valley Univ, Qena Fac Sci, Dept Chem, Qena 83523, Egypt..
    Poulsen, Felipe
    Univ Copenhagen, Dept Chem, DK-2100 Copenhagen, Denmark..
    Zhu, Qiushi
    Lund Univ, Div Chem Phys, Box 124, S-22100 Lund, Sweden.;Lund Univ, NanoLund, Box 124, S-22100 Lund, Sweden..
    Zhu, Nan
    Tech Univ Denmark, Dept Chem, Kemitorvet Bldg 207, DK-2800 Lyngby, Denmark.;Dalian Univ Technol, Zhang Dayu Sch Chem, Dalian 116024, Peoples R China..
    Zidek, Karel
    Acad Sci Czech Republ, Inst Plasma Phys, Reg Ctr Special Opt & Optoelect Syst TOPTEC, Za Slovankou 1782-3, Prague 18200 8, Czech Republic..
    Chabera, Pavel
    Lund Univ, Div Chem Phys, Box 124, S-22100 Lund, Sweden.;Lund Univ, NanoLund, Box 124, S-22100 Lund, Sweden..
    Corti, Annamaria
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Hansen, Thorsten
    Univ Copenhagen, Dept Chem, DK-2100 Copenhagen, Denmark..
    Chi, Qijin
    Tech Univ Denmark, Dept Chem, Kemitorvet Bldg 207, DK-2800 Lyngby, Denmark..
    Canton, Sophie E.
    DESY, Attosecond Sci Grp, Notkestr 85, D-22607 Hamburg, Germany.;ELI HU Nonprofit Ltd, ELI ALPS, Dugonics Ter 13, H-6720 Szeged, Hungary..
    Zheng, Kaibo
    Lund Univ, Div Chem Phys, Box 124, S-22100 Lund, Sweden.;Lund Univ, NanoLund, Box 124, S-22100 Lund, Sweden.;Qatar Univ, Coll Engn, Gas Proc Ctr, POB 2713, Doha, Qatar..
    Pullerits, Tonu
    Lund Univ, Div Chem Phys, Box 124, S-22100 Lund, Sweden.;Lund Univ, NanoLund, Box 124, S-22100 Lund, Sweden..
    Drastic difference between hole and electron injection through the gradient shell of CdxSeyZn1−xS1−y quantum dots2017In: Nanoscale, ISSN 2040-3364, E-ISSN 2040-3372, Vol. 9, no 34, 12503-12508 p.Article in journal (Refereed)
    Abstract [en]

    Ultrafast fluorescence spectroscopy was used to investigate the hole injection in CdxSeyZn1-xS1-y gradient core-shell quantum dot (CSQD) sensitized p-type NiO photocathodes. A series of CSQDs with a wide range of shell thicknesses was studied. Complementary photoelectrochemical cell measurements were carried out to confirm that the hole injection from the active core through the gradient shell to NiO takes place. The hole injection from the valence band of the QDs to NiO depends much less on the shell thickness when compared to the corresponding electron injection to n-type semiconductor (ZnO). We simulate the charge carrier tunneling through the potential barrier due to the gradient shell by numerically solving the Schrodinger equation. The details of the band alignment determining the potential barrier are obtained from X-ray spectroscopy measurements. The observed drastic differences between the hole and electron injection are consistent with a model where the hole effective mass decreases, while the gradient shell thickness increases.

  • 2.
    Agthe, Michael
    et al.
    Stockholm Univ, Arrhenius Lab, Dept Mat & Environm Chem, SE-10691 Stockholm, Sweden..
    Wetterskog, Erik
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Physics.
    Bergström, Lennart
    Stockholm Univ, Arrhenius Lab, Dept Mat & Environm Chem, SE-10691 Stockholm, Sweden..
    Following the Assembly of Iron Oxide Nanocubes by Video Microscopy and Quartz Crystal Microbalance with Dissipation Monitoring2017In: Langmuir, ISSN 0743-7463, E-ISSN 1520-5827, Vol. 33, no 1, 303-310 p.Article in journal (Refereed)
    Abstract [en]

    We have studied the growth of ordered arrays by evaporation-induced self-assembly of iron oxide nanocubes with edge lengths of 6.8 and 10.1 nm using video microscopy (VM) and quartz crystal microbalance with dissipation monitoring (QCM-D). Ex situ electron diffraction of the ordered arrays demonstrates that the crystal axes of the nanocubes are coaligned and confirms that the ordered arrays are mesocrystals. Time-resolved video microscopy shows that growth of the highly ordered arrays at slow solvent evaporation is controlled by particle diffusion and can be described by a simple growth model. The growth of each mesocrystal depends only on the number of nanoparticles within the accessible region irrespective of the relative time of formation. The mass of the dried mesocrystals estimated from the analysis of the bandwidth-shift-to-frequency-shift ratio correlates well with the total mass of the oleate-coated nanoparticles in the deposited dispersion drop.

  • 3.
    Ahlberg, Patrik
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Electronics.
    Johansson, Fredrik
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy.
    Zhang, Zhibin
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Electronics.
    Jansson, Ulf
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Inorganic Chemistry.
    Zhang, Shi-Li
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Electronics.
    Lindblad, Andreas
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy.
    Nyberg, Tomas
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Electronics.
    Defect formation in graphene during low-energy ion bombardment2016In: APL Materials, ISSN 2166-532X, Vol. 4, no 4, 046104Article in journal (Refereed)
    Abstract [en]

    This letter reports on a systematic investigation of sputter induced damage in graphene caused by low energy Ar+ ion bombardment. The integral numbers of ions per area (dose) as well as their energies are varied in the range of a few eV's up to 200 eV. The defects in the graphene are correlated to the dose/energy and different mechanisms for the defect formation are presented. The energetic bombardment associated with the conventional sputter deposition process is typically in the investigated energy range. However, during sputter deposition on graphene, the energetic particle bombardment potentially disrupts the crystallinity and consequently deteriorates its properties. One purpose with the present study is therefore to demonstrate the limits and possibilities with sputter deposition of thin films on graphene and to identify energy levels necessary to obtain defect free graphene during the sputter deposition process. Another purpose is to disclose the fundamental mechanisms responsible for defect formation in graphene for the studied energy range.

  • 4.
    Ahmadi, Majid
    et al.
    University of Puerto Rico.
    Younesi, Reza
    Technical University of Denmark.
    Vegge, Tejs
    Technical University of Denmark.
    Guinel, Maxime J-F
    University of Puerto Rico.
    Nickel oxide crystalline nano flakes: synthesis, characterization and their use as anode in lithium-ion batteries2014In: Materials Research Express, ISSN 2053-1591, Vol. 1, no 2, 025501- p.Article in journal (Refereed)
  • 5.
    Aijaz, Asim
    et al.
    Linkoping Univ, Dept Phys Chem & Biol, IFM Mat Phys, SE-58183 Linkoping, Sweden.;Uppsala Univ, Dept Engn Sci, Angstrom Lab, POB 534, SE-75121 Uppsala, Sweden..
    Louring, Sascha
    Aarhus Univ, Interdisciplinary Nanosci Ctr iNANO, Ny Munkegade 120, DK-8000 Aarhus C, Denmark.;Danish Technol Inst, Tribol Ctr, Teknol Pk,Kongsvang Alle 29, DK-8000 Aarhus C, Denmark..
    Lundin, Daniel
    Univ Paris Saclay, Univ Paris Sud, LPGP, CNRS,UMR 8578, F-91405 Orsay, France..
    Kubart, Tomas
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Electronics.
    Jensen, Jens
    Linkoping Univ, Dept Phys Chem & Biol, IFM Mat Phys, SE-58183 Linkoping, Sweden..
    Sarakinos, Kostas
    Linkoping Univ, Dept Phys Chem & Biol, IFM Mat Phys, SE-58183 Linkoping, Sweden..
    Helmersson, Ulf
    Linkoping Univ, Dept Phys Chem & Biol, IFM Mat Phys, SE-58183 Linkoping, Sweden..
    Synthesis of hydrogenated diamondlike carbon thin films using neon-acetylene based high power impulse magnetron sputtering discharges2016In: Journal of Vacuum Science & Technology. A. Vacuum, Surfaces, and Films, ISSN 0734-2101, E-ISSN 1520-8559, Vol. 34, no 6, 061504Article in journal (Refereed)
    Abstract [en]

    Hydrogenated diamondlike carbon (DLC:H) thin films exhibit many interesting properties that can be tailored by controlling the composition and energy of the vapor fluxes used for their synthesis. This control can be facilitated by high electron density and/or high electron temperature plasmas that allow one to effectively tune the gas and surface chemistry during film growth, as well as the degree of ionization of the film forming species. The authors have recently demonstrated by adding Ne in an Ar-C high power impulse magnetron sputtering (HiPIMS) discharge that electron temperatures can be effectively increased to substantially ionize C species [Aijaz et al., Diamond Relat. Mater. 23, 1 (2012)]. The authors also developed an Ar-C2H2 HiPIMS process in which the high electron densities provided by the HiPIMS operation mode enhance gas phase dissociation reactions enabling control of the plasma and growth chemistry [Aijaz et al., Diamond Relat. Mater. 44, 117 (2014)]. Seeking to further enhance electron temperature and thereby promote electron impact induced interactions, control plasma chemical reaction pathways, and tune the resulting film properties, in this work, the authors synthesize DLC: H thin films by admixing Ne in a HiPIMS based Ar/C2H2 discharge. The authors investigate the plasma properties and discharge characteristics by measuring electron energy distributions as well as by studying discharge current characteristics showing an electron temperature enhancement in C2H2 based discharges and the role of ionic contribution to the film growth. These discharge conditions allow for the growth of thick (>1 mu m) DLC: H thin films exhibiting low compressive stresses (similar to 0.5 GPa), high hardness (similar to 25 GPa), low H content (similar to 11%), and density in the order of 2.2 g/cm(3). The authors also show that film densification and change of mechanical properties are related to H removal by ion bombardment rather than subplantation.

  • 6.
    Aktekin, Burak
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Lacey, Matthew
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Nordh, Tim
    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.
    Tengstedt, Carl
    Scania CV AB.
    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.
    Understanding the Rapid Capacity Fading of LNMO-LTO Lithium-ion Cells at Elevated Temperature2017Conference paper (Refereed)
    Abstract [en]

    The high voltage spinel LiNi0.5Mn1.5O4 (LNMO) has an average operating potential around 4.7 V vs. Li/Li+ and a gravimetric charge capacity of 146 mAh/g making it a promising high energy density positive electrode for Li-ion batteries. Additionally, the 3-D lithium transport paths available in the spinel structure enables fast diffusion kinetics, making it suitable for power applications [1]. However, the material displays large instability during cycling, especially at elevated temperatures. Therefore, significant research efforts have been undertaken to better understand and improve this electrode material.

    Electrolyte (LiPF6 in organic solvents) oxidation and transition metal dissolution are often considered as the main problems [2] for the systems based on this cathode material. These can cause a variety of problems (in different parts of the cell) eventually increasing internal cell resistance, causing active mass loss and decreasing the amount of cyclable lithium.

    Among these issues, cyclable lithium loss cannot be observed in half cells since lithium metal will provide almost unlimited capacity. Being a promising full cell chemistry for high power applications, there has also been a considerable interest on LNMO full cells with Li4Ti5O12 (LTO) used as the negative electrode. For this chemistry, for an optimized cell, quite stable cycling for >1000 cycles has been reported at room temperature while fast fading is still present at 55 °C [3]. This difference in performance (RT vs. 55 °C) is beyond most expectations and likely does not follow any Arrhenius-type of trend.

    In this study, a comprehensive analysis of LNMO-LTO cells has been performed at different temperatures (RT, 40 °C and 55 °C) to understand the underlying reasons behind stable cycling at room temperature and rapid fading at 55 °C. For this purpose, testing was made on regular cells (Figure 1a), 3-electrode cells (Figure 1b) and back-to-back cells [4] (Figure 1c). Electrode interactions (cross-talk) have been shown to exist in the LTO-LNMO system [5] and back-to-back cells have therefore been used to observe fading under conditions where cross-talk is impossible [4]. Galvanostatic cycling combined with short-duration intermittent current interruptions [6] was performed in order to separately observe changes in internal resistance for LNMO and LTO electrodes in a full cell. Ex-situ characterization of electrodes have also been performed using scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS) and X-ray absorption near edge spectroscopy (XANES).

    Our findings show how important the electrode interactions can be in full cells, as a decrease in lithium inventory was shown to be the major factor for the observed capacity fading at elevated temperature. In this presentation, the effect of other factors – active mass loss and internal cell resistance – will be discussed together with the consequences of cross-talk.

    References

    [1] A. Kraytsberg et al. Adv. Energy Mater., vol. 2, pp. 922–939,2012.

    [2] J. H. Kim et al., ChemPhysChem, vol. 15, pp. 1940–1954, 2014.

    [3] H. M. Wu et al. J. E. Soc., vol. 156, pp. A1047–A1050, 2009.

    [4] S. R. Li et al., J. E. Soc., vol. 160, no. 9, pp. A1524–A1528, 2013.

    [5] Dedryvère et al. J. Phys. C., vol. 114 (24), pp. 10999–11008, 2010.

    [6] M. J. Lacey, ChemElectroChem, pp. 1–9, 2017.

  • 7.
    Aktekin, Burak
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Lacey, Matthew
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Nordh, Tim
    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.
    Tengstedt, Carl
    Scania CV AB.
    Zipprich, Wolfgang
    Volkswagen AG.
    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.
    Understanding the Capacity Loss in LiNi0.5Mn1.5O4 - Li4Ti5O12 Lithium-Ion Cells at Ambient and Elevated Temperatures2017Conference paper (Refereed)
    Abstract [en]

    The high voltage spinel LiNi0.5Mn1.5O(LNMO) is an attractive positive electrode due to its operating voltage around 4.7 V (vs. Li/Li+) arising from the Ni2+/Ni4+ redox couple. In addition to high voltage operation, a second advantage of this material is its capability for fast lithium diffusion kinetics through 3-D transport paths in the spinel structure. However, the electrode material is prone to side reactions with conventional electrolytes, including electrolyte decomposition and transition metal dissolution, especially at elevated temperatures1. It is important to understand how undesired reactions originating from the high voltage spinel affect the aging of different cell components and overall cycle life. Half-cells are usually considered as an ideal cell configuration in order to get information only from the electrode of interest. However, this cell configuration may not be ideal to understand capacity fading for long-term cycling and the assumption of ‘stable’ lithium negative electrode may not be valid, especially at high current rates2. Also, among the variety of capacity fading mechanisms, the loss of “cyclable” lithium from the positive electrode (or gain of lithium from electrolyte into the negative electrode) due to side reactions in a full-cell can cause significant capacity loss. This capacity loss is not observable in a typical half-cell as a result of an excessive reserve of lithium in the negative electrode.

    In a full-cell, it is desired that the negative electrode does not contribute to side reactions in a significant way if the interest is more on the positive side. Among candidates on the negative side, Li4Ti5O12 (LTO) is known for its stability since its voltage plateau (around 1.5 V vs. Li/Li+) is in the electrochemical stability window of standard electrolytes and it shows a very small volume change during lithiation. These characteristics make the LNMO-LTO system attractive for a variety of applications (e.g. electric vehicles) but also make it a good model system for studying aging in high voltage spinel-based full cells.

    In this study, we aim to understand the fundamental mechanisms resulting in capacity fading for LNMO-LTO full cells both at room temperature and elevated temperature (55°C). It is known that electrode interactions occur in this system due to migration of reaction products from LNMO to the LTO side3, 4. For this purpose, three electrode cells have been cycled galvanostatically with short-duration intermittent current interruptionsin order to observe internal resistance for both LNMO and LTO electrodes in a full cell, separately. Change of voltage curves over cycling has also been observed to get an insight into capacity loss. For comparison purposes, back-to-back cells (a combination of LNMO and LTO cells connected electrically by lithium sides) were also tested similarly. Post-cycling of harvested electrodes in half cells was conducted to determine the degree of capacity loss due to charge slippage compared to other aging factors. Surface characterization of LNMO as well as LTO electrodes after cycling at room temperature and elevated temperature has been done via SEM, XPS, HAXPES and XANES.

    References

    1. A. Kraytsberg, Y. Ein-Eli, Adv. Energy Mater., vol. 2, pp. 922–939, 2012.

    2. Aurbach, D., Zinigrad, E., Cohen, Y., & Teller, H. Solid State Ionics, 148(3), 405-416, 2002.

    3. Li et al., Journal of The Electrochemical Society, 160 (9) A1524-A1528, 2013.

    4. Aktekin et al., Journal of The Electrochemical Society 164.4: A942-A948. 2017.

    5. Lacey, M. J., ChemElectroChem. Accepted Author Manuscript. doi:10.1002/celc.201700129, 2017. 

  • 8.
    Aktekin, Burak
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Lacey, Matthew
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Nordh, Tim
    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.
    Tengstedt, Carl
    Scania CV AB.
    Zipprich, Wolfgang
    Volkswagen.
    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.
    Understanding the capacity loss in LNMO-LTO lithium-ion cells at ambient and elevated temperaturesManuscript (preprint) (Other academic)
    Abstract
  • 9.
    Alfredsson, Sara
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Applied Materials Sciences.
    Varför svänger stenen?: En studie i curlingens komplexa tribosystem2010Independent thesis Advanced level (professional degree), 20 credits / 30 HE creditsStudent thesis
    Abstract [en]

    The tribo system ice-curling stone was investigated in order to understand the mechanisms behind the stones' behavior on the ice sheet. The problem with non-identical stones should also be addressed.The stone curls, that is, its sliding path deviates from a straight line to the right for a clock-wise rotation and to the left for a anti-clock-wise rotation. Several mechanisms to explain this behavior have been proposed over the years but none has been successful.By carrying out experiments at the local curling rink and studying silicon castings of ice- and stone-surfaces with scanning electron microscopy and vertical scanning interferometry, it has been decided that the curl is not due to dry friction, ice-debris or the difference in friction on the left and right side of the stone. The side force comes from the fact that the friction is higher at the back of the stone than at the front.The contact between stone and ice is never completely dry, nor in the hydrodynamic lubrication regime. It is probably a combination of hydrodynamic lubrication and a contribution from mechanical scratching of the ice. The coefficient of friction depends upon the velocity, from 0.01 for velocities around 1 m/s to higher values for lower velocities. It is not possible to make identical stones, that is identical glide band structures out of Blue Hone granite, since its composition is too inhomogeneous and its grain size is too course. It is recommended to use an amorphous or very fine grained material, at least in the surface of the glideband.

  • 10.
    Amorim, Rodrigo G.
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Theory. Univ Fed Fluminense, Dept Fis, ICEx, Volta Redonda, RJ, Brazil..
    Rocha, Alexandre R.
    Univ Estadual Paulista, UNESP, Inst Fis Teor, Sao Paulo, Brazil..
    Scheicher, Ralph H.
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Theory.
    Boosting DNA Recognition Sensitivity of Graphene Nanogaps through Nitrogen Edge Functionalization2016In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 120, no 34, 19384-19388 p.Article in journal (Refereed)
    Abstract [en]

    One of the challenges for next generation DNA sequencing is to have a robust, stable, and reproducible nanodevice. In this work, we propose how to improve the sensing of DNA nucleobase using functionalized graphene nanogap as a solid state device. Two types of edge functionalization, namely, either hydrogen or nitrogen, were considered. We showed that, independent of species involved in the edge passivation, the highest-to-lowest order of the nucleobase transmissions is not altered, but the intensity is affected by several orders of magnitude. Our results show that nitrogen edge tends to p-dope graphene, and most importantly, it contributes with resonance states close to the Fermi level, which can be associated with the increased conductance. Finally, the translocation process of nucleobases passing through the nanogap was also investigated by varying their position from a certain height (from +3 to -3 angstrom) with respect to the graphene sheet to show that nitrogen-terminated sheets have enhanced sensitivity, as moving the nucleobase by approximately 1 angstrom reduces the conductance by up to 3 orders of magnitude.

  • 11.
    Andersson, Jonas
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Synthesis of polycarbonate polymer electrolytes for lithium ion batteries and study of additives to raise the ionic conductivity2015Independent thesis Advanced level (professional degree), 20 credits / 30 HE creditsStudent thesis
    Abstract [en]

    Polymer electrolyte films based on poly(trimethylene carbonate) (PTMC) mixed with LiTFSI salt in different compositions were synthesized and investigated as electrolytes for lithium ion batteries, where the ionic conductivity is the most interesting material property. Electrochemical impedance spectroscopy (EIS) and DSC were used to measure the ionic conductivity and thermal properties, respectively. Additionally, FTIR and Raman spectroscopy were used to examine ion coordination in the material. Additives of nanosized TiO2 and powders of superionically conducting Li1.3Al0.3Ti1.7(PO4)3 were investigated as enhancers of ionic conductivity, but no positive effect could be shown. The most conductive composition was found at a [Li+]:[carbonate] ratio of 1, corresponding to a salt concentration of 74 percent by weight, which showed an ionic conductivity of 2.0 × 10–6 S cm–1 at 25 °C and 2.2 × 10–5 S cm–1 at 60 °C, whereas for even larger salt concentrations, the mechanical durability of the polymeric material was dramatically reduced, preventing use as a solid electrolyte material. Macroscopic salt crystallization was also observed for these concentrations. Ion coordination to carbonyls on the polymer chain was examined for high salt content compositions with FTIR spectroscopy, where it was found to be relatively similar between the samples, possibly indicating saturation. Moveover, with FTIR, the ion-pairing was found to increase with salt concentration. The ionic conductivity was found to be markedly lower after 7 weeks of aging of the materials with highest salt concentrations.

  • 12.
    Araujo, Rafael B.
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Theory.
    Islam, Muhammed Shafiqul
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Theory. Natl Univ Bangladesh, DSHE, Dhaka 1000, Bangladesh..
    Chakraborty, Sudip
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Theory.
    Ahuja, R.
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Theory. Royal Inst Technol KTH, Dept Mat & Engn, Appl Mat Phys, S-10044 Stockholm, Sweden..
    Predicting electrochemical properties and ionic diffusion in Na2+2xMn2-x(SO4)(3): crafting a promising high voltage cathode material2016In: Journal of Materials Chemistry A, ISSN 2050-7488, Vol. 4, no 2, 451-457 p.Article in journal (Refereed)
    Abstract [en]

    Sodium ion batteries have emerged as a good alternative to lithium based systems due to their low cost of production. In this scenario, the search for higher voltage, sodium cathodes results in a new promising alluaudite structure Na2+2xMn2-x(SO4)(3). The structural, electronic and Na diffusion properties along with defects have been reported in this investigation within the framework of density functional theory. A band gap of 3.61 eV has been computed and the average deintercalation potential is determined to be 4.11 V vs. Na/Na+. A low concentration of anti-site defects is predicted due to their high formation energy. The biggest issue for the ionic diffusion in the Na2+2xMn2-x(SO4)(3) crystal structure is revealed to be the effect of Mn vacancies increasing the activation energy of Na+ ions that hop along the [001] equilibrium positions. This effect leads to activation energies of almost the same high values for the ionic hop through the [010] direction characterizing a 2D like ionic diffusion mechanism in this system.

  • 13.
    Asfaw, Habtom D.
    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.
    Valvo, Mario
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Maibach, Julia
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Ångström, Jonas
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Tai, Cheuk-Wai
    Bacsik, Zoltan
    Sahlberg, Martin
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Inorganic 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.
    Boosting the thermal stability of emulsion–templated polymers via sulfonation: an efficient synthetic route to hierarchically porous carbon foams2016In: ChemistrySelect, ISSN 2365-6549, Vol. 1, no 4, 784-792 p.Article in journal (Refereed)
    Abstract [en]

    Hierarchically porous carbon foams with specific surface areas exceeding 600 m2 g−1 can be derived from polystyrene foams that are synthesized via water-in-oil emulsion templating. However, most styrene-based polymers lack strong crosslinks and are degraded to volatile products when heated above 400 oC. A common strategy employed to avert depolymerization is to introduce potential crosslinking sites such as sulfonic acids by sulfonating the polymers. This article unravels the thermal and chemical processes leading up to the conversion of sulfonated high internal phase emulsion polystyrenes (polyHIPEs) to sulfur containing carbon foams. During pyrolysis, the sulfonic acid groups (-SO3H) are transformed to sulfone (-C-SO2-C-) and then to thioether (-C−S-C-) crosslinks. These chemical transformations have been monitored using spectroscopic techniques: in situ IR, Raman, X-ray photoelectron and X-ray absorption near edge structure spectroscopy. Based on thermal analyses, the formation of thioether links is associated with increased thermal stability and thus a substantial decrease in volatilization of the polymers.

  • 14.
    Asfaw, Habtom Desta
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Multifunctional Carbon Foams by Emulsion Templating: Synthesis, Microstructure, and 3D Li-ion Microbatteries2017Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    Carbon foams are among the existing electrode designs proposed for use in 3D Li-ion microbatteries. For such electrodes to find applications in practical microbatteries, however, their void sizes, specific surface areas and pore volumes need be optimized. This thesis concerns the synthesis of highly porous carbon foams and their multifunctional applications in 3D microbatteries. The carbon foams are derived from polymers that are obtained by polymerizing high internal phase water-in-oil emulsions (HIPEs).

    In general, the carbonization of the sulfonated polymers yielded hierarchically porous structures with void sizes ranging from 2 to 35 µm and a BET specific surface area as high as 630 m2 g-1. Thermogravimetric and spectroscopic evidence indicated that the sulfonic acid groups, introduced during sulfonation, transformed above 250 oC to thioether (-C-S-) crosslinks which were responsible for the thermal stability and charring tendency of the polymer precursors. Depending on the preparation of the HIPEs, the specific surface areas and void-size distributions were observed to vary considerably. In addition, the pyrolysis temperature could also affect the microstructures, the degree of graphitization, and the surface chemistry of the carbon foams.

    Various potential applications were explored for the bespoke carbon foams. First, their use as freestanding active materials in 3D microbatteries was studied. The carbon foams obtained at 700 to 1500 oC suffered from significant irreversible capacity loss during the initial discharge. In an effort to alleviate this drawback, the pyrolysis temperature was raised to 2200 oC. The resulting carbon foams were observed to deliver high, stable areal capacities over several cycles. Secondly, the possibility of using these structures as 3D current collectors for various active materials was investigated in-depth. As a proof-of-concept demonstration, positive active materials like polyaniline and LiFePO4 were deposited on the 3D architectures by means of electrodeposition and sol-gel approach, respectively. In both cases, the composite electrodes exhibited reasonably high cyclability and rate performance at different current densities. The syntheses of niobium and molybdenum oxides and their potential application as electrodes in microbatteries were also studied. In such applications, the carbon foams served dual purposes as 3D scaffolds and as reducing reactants in the carbothermal reduction process. Finally, a facile method of coating carbon substrates with oxide nanosheets was developed. The approach involved the exfoliation of crystalline VO2 to prepare dispersions of hydrated V2O5, which were subsequently cast onto CNT paper to form oxide films of different thicknesses.

    List of papers
    1. Boosting the thermal stability of emulsion–templated polymers via sulfonation: an efficient synthetic route to hierarchically porous carbon foams
    Open this publication in new window or tab >>Boosting the thermal stability of emulsion–templated polymers via sulfonation: an efficient synthetic route to hierarchically porous carbon foams
    Show others...
    2016 (English)In: ChemistrySelect, ISSN 2365-6549, Vol. 1, no 4, 784-792 p.Article in journal (Refereed) Published
    Abstract [en]

    Hierarchically porous carbon foams with specific surface areas exceeding 600 m2 g−1 can be derived from polystyrene foams that are synthesized via water-in-oil emulsion templating. However, most styrene-based polymers lack strong crosslinks and are degraded to volatile products when heated above 400 oC. A common strategy employed to avert depolymerization is to introduce potential crosslinking sites such as sulfonic acids by sulfonating the polymers. This article unravels the thermal and chemical processes leading up to the conversion of sulfonated high internal phase emulsion polystyrenes (polyHIPEs) to sulfur containing carbon foams. During pyrolysis, the sulfonic acid groups (-SO3H) are transformed to sulfone (-C-SO2-C-) and then to thioether (-C−S-C-) crosslinks. These chemical transformations have been monitored using spectroscopic techniques: in situ IR, Raman, X-ray photoelectron and X-ray absorption near edge structure spectroscopy. Based on thermal analyses, the formation of thioether links is associated with increased thermal stability and thus a substantial decrease in volatilization of the polymers.

    Keyword
    Emulsion-templated polymer, sulfonation, pyrolysis, spectroscopy, carbon foam
    National Category
    Materials Chemistry
    Research subject
    Chemistry with specialization in Materials Chemistry
    Identifiers
    urn:nbn:se:uu:diva-283174 (URN)10.1002/slct.201600139 (DOI)000395395900026 ()
    Projects
    3D microbatteries
    Available from: 2016-04-11 Created: 2016-04-11 Last updated: 2017-10-30Bibliographically approved
    2. Emulsion-templated bicontinuous carbon network electrodes for use in 3D microstructured batteries
    Open this publication in new window or tab >>Emulsion-templated bicontinuous carbon network electrodes for use in 3D microstructured batteries
    2013 (English)In: Journal of Materials Chemistry, ISSN 0959-9428, E-ISSN 1364-5501, Vol. 1, no 44, 13750-13758 p.Article in journal (Refereed) Published
    Abstract [en]

    High surface area carbon foams were prepared and characterized for use in 3D structured batteries. Twopotential applications exist for these foams: firstly as an anode and secondly as a current collector supportfor electrode materials. The preparation of the carbon foams by pyrolysis of a high internal phase emulsionpolymer (polyHIPE) resulted in structures with cage sizes of 25 mm and a surface area enhancement pergeometric area of approximately 90 times, close to the optimal configuration for a 3D microstructuredbattery support. The structure was probed using XPS, SEM, BET, XRD and Raman techniques; revealingthat the foams were composed of a disordered carbon with a pore size in the <100 nm range resultingin a BET measured surface area of 433 m2 g-1. A reversible capacity exceeding 3.5 mA h cm2 at acurrent density of 0.37 mA cm-2 was achieved. SEM images of the foams after 50 cycles showed thatthe structure suffered no degradation. Furthermore, the foams were tested as a current collector bydepositing a layer of polyaniline cathode over their surface. High footprint area capacities of500 mA h cm-2 were seen in the voltage range 3.8 to 2.5 V vs. Li and a reasonable rate performancewas observed.

    Place, publisher, year, edition, pages
    United Kingdom: , 2013
    Keyword
    Carbon foam, High internal phase emulsion polymer, microbattery, 3D microbattery, Lithium ion
    National Category
    Chemical Sciences Materials Chemistry
    Research subject
    Materials Science; Chemistry; Materials Science; Physical Chemistry
    Identifiers
    urn:nbn:se:uu:diva-210659 (URN)10.1039/C3TA12680C (DOI)000326463400009 ()
    Projects
    STEM-VR-Microbattery
    Funder
    Swedish Energy AgencySwedish Research Council
    Available from: 2013-11-12 Created: 2013-11-12 Last updated: 2017-12-06Bibliographically approved
    3. Emulsion-templated graphitic carbon foams with optimum porosity for 3D Li-ion microbatteries
    Open this publication in new window or tab >>Emulsion-templated graphitic carbon foams with optimum porosity for 3D Li-ion microbatteries
    (English)Manuscript (preprint) (Other academic)
    Keyword
    carbon, foam, graphitic, anode, three-dimensional, microbattery, lithium
    National Category
    Polymer Technologies Chemical Process Engineering Materials Chemistry Polymer Chemistry Inorganic Chemistry Physical Chemistry
    Identifiers
    urn:nbn:se:uu:diva-312893 (URN)
    Funder
    Swedish Research Council, 2012–4681StandUp
    Available from: 2017-01-14 Created: 2017-01-14 Last updated: 2017-12-30
    4. Nanosized LiFePO4-decorated emulsion-templated carbon foam for 3D micro batteries: a study of structure and electrochemical performance
    Open this publication in new window or tab >>Nanosized LiFePO4-decorated emulsion-templated carbon foam for 3D micro batteries: a study of structure and electrochemical performance
    Show others...
    2014 (English)In: Nanoscale, ISSN 2040-3364, E-ISSN 2040-3372, Vol. 6, no 15, 8804-8813 p.Article in journal (Refereed) Published
    Abstract [en]

    In this article, we report a novel 3D composite cathode fabricated from LiFePO4 nanoparticles deposited conformally on emulsion-templated carbon foam by a sol–gel method. The carbon foam is synthesized via a facile and scalable method which involves the carbonization of a high internal phase emulsion (polyHIPE) polymer template. Various techniques (XRD, SEM, TEM and electrochemical methods) are used to fully characterize the porous electrode and confirm the distribution and morphology of the cathode active material. The major benefits of the carbon foam used in our work are closely connected with its high surface area and the plenty of space suitable for sequential coating with battery components. After coating with a cathode material (LiFePO4nanoparticles), the 3D electrode presents a hierarchically structured electrode in which a porous layer of the cathode material is deposited on the rigid and bicontinuous carbon foam. The composite electrodes exhibit impressive cyclability and rate performance at different current densities affirming their importance as viable power sources in miniature devices. Footprint area capacities of 1.72 mA h cm−2 at 0.1 mA cm−2 (lowest rate) and 1.1 mA h cm−2 at 6 mA cm−2(highest rate) are obtained when the cells are cycled in the range 2.8 to 4.0 V vs. lithium.

    Place, publisher, year, edition, pages
    Royal Society of Chemistry: , 2014
    National Category
    Physical Chemistry Polymer Chemistry Materials Chemistry Inorganic Chemistry
    Identifiers
    urn:nbn:se:uu:diva-228630 (URN)10.1039/C4NR01682C (DOI)000339861500051 ()
    Projects
    STEM-VR-Microbattery
    Available from: 2014-07-18 Created: 2014-07-18 Last updated: 2017-12-05Bibliographically approved
    5. Surface-oxidized NbO2 nanoparticles for high performance lithium microbatteries
    Open this publication in new window or tab >>Surface-oxidized NbO2 nanoparticles for high performance lithium microbatteries
    (English)Manuscript (preprint) (Other academic)
    Keyword
    niobium, oxide, nanoparticle, power, energy, carbon, foam, lithium, microbattery
    National Category
    Natural Sciences Inorganic Chemistry Materials Chemistry Physical Chemistry Condensed Matter Physics Materials Engineering Chemical Engineering
    Research subject
    Chemistry with specialization in Materials Chemistry
    Identifiers
    urn:nbn:se:uu:diva-312894 (URN)
    Projects
    3D Lithium-ion microbattery
    Funder
    Swedish Research Council, 2012–4681StandUp
    Available from: 2017-01-14 Created: 2017-01-14 Last updated: 2017-12-30
    6. A one-step water based strategy for synthesizing hydrated vanadium pentoxide nanosheets from VO2(B) as free-standing electrodes for lithium battery applications
    Open this publication in new window or tab >>A one-step water based strategy for synthesizing hydrated vanadium pentoxide nanosheets from VO2(B) as free-standing electrodes for lithium battery applications
    Show others...
    2016 (English)In: Journal of Materials Chemistry A, ISSN 2050-7488, Vol. 4, no 46, 17988-18001 p.Article in journal (Refereed) Published
    Abstract [en]

    The synthesis of two dimensional (2D) materials from transition metal oxides, chalcogenides, and carbides mostly involve multiple exfoliation steps in which hazardous solvents and reagents are used. In this study, hydrated vanadium pentoxide (V2O5[middle dot]nH2O) nanosheets with a thickness of a few nanometers were prepared via a facile environmentally friendly water based exfoliation technique. The exfoliation process involved refluxing the precursor, vanadium dioxide (VO2(B)), in water for a few days at 60 [degree]C. The proposed exfoliation mechanism is based on the intercalation/insertion of water molecules into the VO2(B) crystals and the subsequent cleavage of the covalent bonds holding the layers of VO2(B) together. The thermal and chemical analyses showed that the approximate chemical composition of the nanosheets is H0.4V2O5[middle dot]0.55H2O, and the percentage of VV content to that of VIV in the nanosheets is about 80(3)% to 20(3)%. The exfoliated aqueous suspension of the V2O5[middle dot]0.55H2O nanosheets was successfully deposited onto multi-walled carbon nanotube (MW-CNT) paper to form free-standing electrodes with a thickness of the V2O5[middle dot]0.55H2O layer ranging between 45 and 4 [small mu ]m. A series of electrochemical tests were conducted on the electrodes to determine the cyclability and rate capability of lithium insertion into V2O5[middle dot]0.55H2O nanosheets. The electrodes with the thinnest active material coating ([similar]4 [small mu ]m) delivered gravimetric capacities of up to 480 and 280 mA h g-1 when cycled at current densities of 10 and 200 mA g-1, respectively.

    Keyword
    2D materials, vanadium oxides, free-standing, battery, lithium
    National Category
    Materials Chemistry
    Identifiers
    urn:nbn:se:uu:diva-311357 (URN)10.1039/C6TA06571F (DOI)000388505400010 ()
    Funder
    Swedish Research Council, 2012-4681Swedish Energy AgencyBerzelii Centre EXSELENTStandUp
    Available from: 2016-12-24 Created: 2016-12-24 Last updated: 2017-12-30
  • 15.
    Asfaw, Habtom Desta
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Roberts, Matthew R.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström.
    Tai, Cheuk-Wai
    Stockholm University.
    Younesi, Reza
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry. DTU.
    Valvo, Mario
    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.
    Nanosized LiFePO4-decorated emulsion-templated carbon foam for 3D micro batteries: a study of structure and electrochemical performance2014In: Nanoscale, ISSN 2040-3364, E-ISSN 2040-3372, Vol. 6, no 15, 8804-8813 p.Article in journal (Refereed)
    Abstract [en]

    In this article, we report a novel 3D composite cathode fabricated from LiFePO4 nanoparticles deposited conformally on emulsion-templated carbon foam by a sol–gel method. The carbon foam is synthesized via a facile and scalable method which involves the carbonization of a high internal phase emulsion (polyHIPE) polymer template. Various techniques (XRD, SEM, TEM and electrochemical methods) are used to fully characterize the porous electrode and confirm the distribution and morphology of the cathode active material. The major benefits of the carbon foam used in our work are closely connected with its high surface area and the plenty of space suitable for sequential coating with battery components. After coating with a cathode material (LiFePO4nanoparticles), the 3D electrode presents a hierarchically structured electrode in which a porous layer of the cathode material is deposited on the rigid and bicontinuous carbon foam. The composite electrodes exhibit impressive cyclability and rate performance at different current densities affirming their importance as viable power sources in miniature devices. Footprint area capacities of 1.72 mA h cm−2 at 0.1 mA cm−2 (lowest rate) and 1.1 mA h cm−2 at 6 mA cm−2(highest rate) are obtained when the cells are cycled in the range 2.8 to 4.0 V vs. lithium.

  • 16.
    Asfaw, Habtom Desta
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Roberts, Matthew R.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry. St. Andrews.
    Younesi, Reza
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry. DTU.
    Edström, Kristina
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Emulsion-templated bicontinuous carbon network electrodes for use in 3D microstructured batteries2013In: Journal of Materials Chemistry, ISSN 0959-9428, E-ISSN 1364-5501, Vol. 1, no 44, 13750-13758 p.Article in journal (Refereed)
    Abstract [en]

    High surface area carbon foams were prepared and characterized for use in 3D structured batteries. Twopotential applications exist for these foams: firstly as an anode and secondly as a current collector supportfor electrode materials. The preparation of the carbon foams by pyrolysis of a high internal phase emulsionpolymer (polyHIPE) resulted in structures with cage sizes of 25 mm and a surface area enhancement pergeometric area of approximately 90 times, close to the optimal configuration for a 3D microstructuredbattery support. The structure was probed using XPS, SEM, BET, XRD and Raman techniques; revealingthat the foams were composed of a disordered carbon with a pore size in the <100 nm range resultingin a BET measured surface area of 433 m2 g-1. A reversible capacity exceeding 3.5 mA h cm2 at acurrent density of 0.37 mA cm-2 was achieved. SEM images of the foams after 50 cycles showed thatthe structure suffered no degradation. Furthermore, the foams were tested as a current collector bydepositing a layer of polyaniline cathode over their surface. High footprint area capacities of500 mA h cm-2 were seen in the voltage range 3.8 to 2.5 V vs. Li and a reasonable rate performancewas observed.

  • 17.
    Asfaw, Habtom Desta
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Tai, Cheuk-Wai
    Stockholm University.
    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.
    Emulsion-templated graphitic carbon foams with optimum porosity for 3D Li-ion microbatteriesManuscript (preprint) (Other academic)
  • 18.
    Asfaw, Habtom Desta
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Tai, Cheuk-Wai
    Stockholm University.
    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.
    Surface-oxidized NbO2 nanoparticles for high performance lithium microbatteriesManuscript (preprint) (Other academic)
  • 19.
    Asfaw, Habtom
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström.
    Tai, Cheuk-Wai
    Stockholm University.
    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.
    Surface-oxidized NbO2 nanoparticles for high performance lithium microbatteriesManuscript (preprint) (Other academic)
  • 20.
    Aulin, Cecilia
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Materials Chemistry.
    Extracellular Matrix Based Materials for Tissue Engineering2010Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    The extracellular matrix is (ECM) is a network of large, structural proteins and polysaccharides, important for cellular behavior, tissue development and maintenance. Present thesis describes work exploring ECM as scaffolds for tissue engineering by manipulating cells cultured in vitro or by influencing ECM expression in vivo. By culturing cells on polymer meshes under dynamic culture conditions, deposition of a complex ECM could be achieved, but with low yields. Since the major part of synthesized ECM diffused into the medium the rate limiting step of deposition was investigated. This quantitative analysis showed that the real rate limiting factor is the low proportion of new proteins which are deposited as functional ECM. It is suggested that cells are pre-embedded in for example collagen gels to increase the steric retention and hence functional deposition.

    The possibility to induce endogenous ECM formation and tissue regeneration by implantation of growth factors in a carrier material was investigated. Bone morphogenetic protein-2 (BMP-2) is a growth factor known to be involved in growth and differentiation of bone and cartilage tissue. The BMP-2 processing and secretion was examined in two cell systems representing endochondral (chondrocytes) and intramembranous (mesenchymal stem cells) bone formation. It was discovered that chondrocytes are more efficient in producing BMP-2 compared to MSC. The role of the antagonist noggin was also investigated and was found to affect the stability of BMP-2 and modulate its effect. Finally, an injectable gel of the ECM component hyaluronan has been evaluated as delivery vehicle in cartilage regeneration. The hyaluronan hydrogel system showed promising results as a versatile biomaterial for cartilage regeneration, could easily be placed intraarticulary and can be used for both cell based and cell free therapies.

    List of papers
    1. Extracellular matrix-polymer hybrid materials produced in a pulsed-flow bioreactor system
    Open this publication in new window or tab >>Extracellular matrix-polymer hybrid materials produced in a pulsed-flow bioreactor system
    2009 (English)In: Journal of Tissue Engineering and Regenerative Medicine, ISSN 1932-6254, Vol. 3, no 3, 188-195 p.Article in journal (Refereed) Published
    Abstract [en]

    Cell adhesion, interaction with material, cell proliferation and the production of an extracellular matrix (ECM) are all important factors determining the successful performance of an engineered scaffold. Scaffold design should aim at creating structures which can guide cells into forming new, functional tissue. In this study, the concept of in situ deposition of ECM by human dermal fibroblasts onto a compliant, knitted poly (ethyleneterephtalate) support is demonstrated, creating in vitro produced ECM polymer hybrid materials for tissue engineering. Comparison of cells cultured under static and dynamic conditions were examined, and the structure and morphology of the materials so formed were evaluated, along with the amount collagen deposited by the seeded cells. In vitro produced ECM polymer hybrid scaffolds could be created in this way, with the dynamic culture conditions increasing ECM deposition. Histological analysis indicated a homogenous distribution of cells in the 1 mm thick scaffold, surrounded by a matrix-like structure. ECM deposition was observed throughout the materials wigh 81.6 µg/cm2 of collagen deposited after 6 weeks. Cell produced bundles of ECM fibres bridged the polymer filaments and anchored cells to the support. These findings open hereto unknown possibilities of producing materials with structure designed by engineering together with biochemical composition given by cells.

    Place, publisher, year, edition, pages
    John Wiley & Sons, Ltd, 2009
    Keyword
    extracellular matrix, scaffold, polymer support, fibroblasts, bioreactor, dynamic culture conditions
    National Category
    Chemical Sciences
    Research subject
    Inorganic Chemistry
    Identifiers
    urn:nbn:se:uu:diva-106096 (URN)10.1002/term.152 (DOI)000265268400003 ()
    Available from: 2009-06-15 Created: 2009-06-15 Last updated: 2010-08-02Bibliographically approved
    2. Bulk collagen incorporation rates into knitted stiff fibre polymer in tissue-engineered scaffolds: the rate-limiting step
    Open this publication in new window or tab >>Bulk collagen incorporation rates into knitted stiff fibre polymer in tissue-engineered scaffolds: the rate-limiting step
    Show others...
    2008 (English)In: Journal of Tissue Engineering and Regenerative Medicine, ISSN 1932-6254, Vol. 2, no 8, 507-514 p.Article in journal (Refereed) Published
    Abstract [en]

    Fabrication of tissue-engineered constructs in vitro relies on sufficient synthesis of extracellular matrix (ECM) by cells to form a material suitable for normal function in vivo. Collagen synthesis by human dermal fibroblasts grown in vitro on two polymers, polyethylene terephthalate (PET) and polyglycolic acid (PGA), was measured by high-performance liquid chromatography (HPLC). Cells were either cultured in a dynamic environment, where meshes were loaded onto a pulsing tube in a bioreactor, or in a static environment without pulsing. Collagen synthesis by cells cultured on a static mesh increased by six-fold compared to monolayer culture, and increased by up to a further 5.4-fold in a pulsed bioreactor. However, little of the collagen synthesized was deposited onto the meshes, almost all being lost to the medium. The amount of collagen deposited onto meshes was highest when cells were cultured dynamically on PET meshes (17.6 µg), but deposition still represented only 1.4% of the total synthesized. Although total collagen synthesis was increased by the use of 3D culture and the introduction of pulsing, the results suggest that the limiting factor for fabrication of a tissue-engineered construct within practical timescales is not the amount of collagen synthesized but the quantity retained (i.e. deposited) within the construct during culture. This may be enhanced by systems which promote or assemble true 3D multi-layers of cells.

    Place, publisher, year, edition, pages
    John Wiley & Sons, Ltd., 2008
    Keyword
    collagen synthesis, collagen deposition, tissue engineering, polyethylene terephthalate, 3D culture, bioreactors
    National Category
    Chemical Sciences
    Research subject
    Inorganic Chemistry
    Identifiers
    urn:nbn:se:uu:diva-99347 (URN)10.1002/term.126 (DOI)000262272900007 ()
    Available from: 2009-03-12 Created: 2009-03-12 Last updated: 2010-08-04Bibliographically approved
    3. Comparative studies on BMP-2 processing and secretion in chondrocytes and mesenchymal cells and the effect of noggin
    Open this publication in new window or tab >>Comparative studies on BMP-2 processing and secretion in chondrocytes and mesenchymal cells and the effect of noggin
    (English)Manuscript (preprint) (Other academic)
    Keyword
    bone formation, BMP-2, noggin, chondrocytes, mesenchymal stem cells
    Identifiers
    urn:nbn:se:uu:diva-110746 (URN)
    Available from: 2009-11-24 Created: 2009-11-24
    4. Evaluation of an injectable hyaluronan hydrogel for cartilage regeneration
    Open this publication in new window or tab >>Evaluation of an injectable hyaluronan hydrogel for cartilage regeneration
    Show others...
    (English)Manuscript (preprint) (Other academic)
    Keyword
    hyaluronan, chondrocytes, mesenchymal stem cells, cartilage, injectable, bone morphogenetic protein-2, rabbit model
    Identifiers
    urn:nbn:se:uu:diva-110750 (URN)
    Available from: 2009-11-24 Created: 2009-11-24
  • 21.
    Backholm, Jonas
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Physics.
    Georén, Peter
    Niklasson, Gunnar A.
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Physics.
    Determination of solid phase chemical diffusion coefficient and density of states by electrochemical methods: Application to iridium oxide-based thin films2008In: Journal of Applied Physics, ISSN 0021-8979, E-ISSN 1089-7550, Vol. 103, no 2, 023702- p.Article in journal (Refereed)
    Abstract [en]

    Potentiostatic intermittent titration technique (PITT) and electrochemical impedance spectroscopy (EIS) were investigated as methods to determine solid phase chemical diffusion coefficient (D) and electronic density of states (DOS). These techniques were then applied to iridium oxide (IrOx) and iridium-tantalum oxide (IrTaOx) thin films prepared by sputter deposition. The experiments, performed in 1M propionic acid between -0.2 and 0.8 V vs Ag/AgCl, showed effects of interfacial side reactions, whose contribution to the electrochemical response could be identified and corrected for in the case of PITT as well as EIS. It was found that D is strongly underestimated when using PITT with the common Cottrell formalism, which follows from non-negligible interfacial charge transfer and Ohmic resistances. EIS indicated an anomalous diffusion mechanism, and D was determined to be in the 10(-11)-10(-10) cm(2)/s range for IrOx and IrTaOx. Both PITT and EIS showed that the intercalated charge as a function of potential exhibits a shape that resembles the theoretical DOS of crystalline iridium oxide, especially for IrTaOx.

  • 22.
    Baloukas, Bill
    et al.
    Polytech Montreal, Dept Engn Phys, Montreal.
    Arvizu, Miguel A
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Physics.
    Wen, Rui-Tao
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Physics.
    Niklasson, Gunnar A.
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Physics.
    Granqvist, Claes Göran
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Physics.
    Vernhes, Richard
    Polytech Montreal, Dept Engn Phys, Montreal.
    Klemberg-Sapieha, Jolanta E.
    Polytech Montreal, Dept Engn Phys, Montreal.
    Martinu, Ludvik
    Polytech Montreal, Dept Engn Phys, Montreal.
    Galvanostatic Rejuvenation of Electrochromic WO3 Thin Films: Ion Trapping and Detrapping Observed by Optical Measurements and by Time-of-Flight Secondary Ion Mass Spectrometry2017In: ACS Applied Materials and Interfaces, ISSN 1944-8244, E-ISSN 1944-8252, Vol. 9, no 20, 16996-17002 p.Article in journal (Refereed)
    Abstract [en]

    Electrochromic (EC) smart windows are able to decrease our energy footprint while enhancing indoor comfort and convenience. However, the limited durability of these windows, as well as their cost, result in hampered market introduction. Here, we investigate thin films of the most widely studied EC material, WO3. Specifically, we combine optical measurements (using spectrophotometry in conjunction with variable-angle spectroscopic ellipsometry) with time-of-flight secondary ion mass spectrometry and atomic force microscopy. Data were taken on films in their as-deposited state, after immersion in a Li-ion-conducting electrolyte, after severe degradation by harsh voltammetric cycling and after galvanostatic rejuvenation to regain the original EC performance. Unambiguous evidence was found for the trapping and detrapping of Li ions in the films, along with a thickness increase or decrease during degradation and rejuvenation, respectively. It was discovered that (i) the trapped ions exhibited a depth gradient; (ii) following the rejuvenation procedure, a small fraction of the Li ions remained trapped in the film and gave rise to a weak short-wavelength residual absorption; and (iii) the surface roughness of the film was larger in the degraded state than in its virgin and rejuvenated states. These data provide important insights into the degradation mechanisms of EC devices and into means of achieving improved durability.

  • 23.
    Bamford, Erik
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Applied Materials Sciences.
    Tool wear in turning of titanium alloy Ti–6Al–4V: Challenges and potential solutions for crater wear, diffusion and chip formation2016Independent thesis Advanced level (professional degree), 20 credits / 30 HE creditsStudent thesis
    Abstract [en]

    Titanium alloys are major materials used in the airplane industry, and prospects show that airplane production will double in the next 20 years. Consequently, the demand for cutting tools for machining of titanium alloys will increase. The primary problem when machining titanium alloys is their low thermal conductivity. Crater wear is the main factor limiting tool life, and is generally caused by thermal diffusion due to high temperatures in the tool-chip interface.

    This master’s thesis was performed in collaboration with Sandvik Coromant, with the prospect to increase knowledge of how diffusion and chip formation influences crater wear progression. The aim was to study tool wear of cutting tools when turning Ti–6Al–4V. This was done by testing two different rake face geometries, both coated and uncoated, at cutting speeds of 30–115 m/min. Diffusion was investigated to learn about the impact it has on crater wear. Chips were examined to investigate chip formation and shear strain.

    The coated modified rake face insert showed less crater wear only for the initial few seconds of machining. Uncoated inserts with a modified rake face showed higher diffusion rate and faster crater wear progression than did standard inserts. The standard inserts showed twice as long tool life as did the modified inserts. No significant differences in the chip formation mechanism were found between modified and standard inserts. Cracks were found within shear bands that were thinner than usual, which suggest that the generation of cracks allows less shear deformation.

  • 24.
    Barker, Paul Michael
    et al.
    Laboratory for Nanoscale Materials Science, Empa, Dübendorf, Switzerland.
    Konstantinidis, Stephanos
    Chimie des Interactions Plasma-Surface (ChIPS), Université de Mons, Belgium.
    Lewin, Erik
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Inorganic Chemistry.
    Britun, Nikolay
    Chimie des Interactions Plasma-Surface (ChIPS), Université de Mons, Belgium.
    Patscheider, Jörg
    Laboratory for Nanoscale Materials Science, Empa, Dübendorf, Switzerland.
    An investigation of c-HiPIMS discharges during titanium deposition2014In: Surface & Coatings Technology, ISSN 0257-8972, E-ISSN 1879-3347, Vol. 258, 631-638 p.Article in journal (Refereed)
    Abstract [en]

    Abstract A modified version of high power impulse magnetron sputtering (HiPIMS) has been used to deposit titanium films at higher deposition rates than for conventional HiPIMS whilst maintaining similar pulse voltages and peak currents. This process, named chopped-HiPIMS (c-HiPIMS) utilises pulses decomposed into several short single pulses instead of single HiPIMS pulses. Experiments show that manipulating the pulse sequence during c-HiPIMS, i.e. the tÎŒon and tÎŒoff times (explained in the glossary) allows for an increase of the deposition rate; increases of up to 150% are reported here for selected conditions. Further, deposition rates higher than those measured using direct current magnetron sputtering are also shown. Investigations by optical emission and optical absorption spectroscopy at the substrate show that the increase of deposition rate is not a consequence of different ion concentrations arriving at the substrate when changing the micro-pulse-off times of c-HiPIMS. Thus alternative reasons for the enhanced deposition rate during c-HiPIMS deposition of metal films are discussed. It is demonstrated that film micro-structure maintains the void free, dense nature typically demonstrated by HiPIMS deposited coatings whilst at enhanced deposition rates. Thus c-HiPIMS allows for the preparation of dense films with the benefit of faster growth rates.

  • 25. Beinik, Igor
    et al.
    Hellström, Matti
    Jensen, Thomas
    Broqvist, Peter
    Lauritsen, Jeppe
    Cu wets the polar ZnO(0001)-Zn surface because of interaction with subsurface defectsArticle in journal (Refereed)
  • 26.
    Beinik, Igor
    et al.
    Aarhus Univ, Interdisciplinary Nanosci Ctr iNANO, DK-8000 Aarhus, Denmark..
    Hellström, Matti
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström.
    Jensen, Thomas N.
    Aarhus Univ, Interdisciplinary Nanosci Ctr iNANO, DK-8000 Aarhus, Denmark..
    Broqvist, Peter
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Lauritsen, Jeppe V.
    Aarhus Univ, Interdisciplinary Nanosci Ctr iNANO, DK-8000 Aarhus, Denmark..
    Enhanced wetting of Cu on ZnO by migration of subsurface oxygen vacancies2015In: Nature Communications, ISSN 2041-1723, E-ISSN 2041-1723, Vol. 6, 8845Article in journal (Refereed)
    Abstract [en]

    Metal adhesion on metal oxides is strongly controlled by the oxide surface structure and composition, but lack of control over the surface conditions often limits the possibilities to exploit this in opto- and micro-electronics applications and heterogeneous catalysis where nanostructural control is of utmost importance. The Cu/ZnO system is among the most investigated of such systems in model studies, but the presence of subsurface ZnO defects and their important role for adhesion on ZnO have been unappreciated so far. Here we reveal that the surface- directed migration of subsurface defects affects the Cu adhesion on polar ZnO(0001) in the technologically interesting temperature range up to 550 K. This leads to enhanced adhesion and ultimately complete wetting of ZnO(0001) by a Cu overlayer. On the basis of our experimental and computational results we demonstrate a mechanism which implies that defect concentrations in the bulk are an important, and possibly controllable, parameter for the metal-on-oxide growth.

  • 27.
    Bergh, Magnus
    et al.
    Swedish Def Res Agcy, S-16490 Stockholm, Sweden..
    Caleman, Carl
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics. DESY, Ctr Free Electron Laser Sci, Hamburg, Germany..
    A Validation Study of the General Amber Force Field Applied to Energetic Molecular Crystals2016In: Journal of Energetic Materials, ISSN 0737-0652, E-ISSN 1545-8822, Vol. 34, no 1, 62-75 p.Article in journal (Refereed)
    Abstract [en]

    Molecula dynamics is a well-established tool to computationally study molecules. However, to reach predictive capability at the level required for applied research and design, extensive validation of the available force fields is pertinent. Here we present a study of density, isothermal compressibility and coefficients of thermal expansion of four energetic materials (FOX-7, RDX, CL-20 and HMX) based on molecular dynamics simulations with the General Amber Force Field (GAFF), and compare the results to experimental measurements from the literature. Furthermore, we quantify the accuracy of the calculated properties through hydrocode simulation of a typical impact scenario. We find that molecular dynamics simulations with generic and computationally efficient force fields may be used to understand and estimate important physical properties of nitramine-like energetic materials.

  • 28.
    Berts, Ida
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström.
    Relating the Bulk and Interface Structure of Hyaluronan to Physical Properties of Future Biomaterials2013Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    This dissertation describes a structural investigation of hyaluronan (HA) with neutron scattering techniques. HA is a natural biopolymer and one of the major components of the extracellular matrix, synovial fluid, and vitreous humor.  It is used in several biomedical applications like tissue engineering, drug delivery, and treatment of osteoarthritis. Although HA is extensively studied, very little is known about its three-dimensional conformation and how it interacts with ions and other molecules. The study aims to understand the bulk structure of a cross-linked HA hydrogel, as well as the conformational arrangement of HA at solid-liquid interfaces. In addition, the structural changes of HA are investigated by simulation of physiological environments, such as changes in ions, interactions with nanoparticles, and proteins etc. Small-angle neutron scattering and neutron reflectivity are the two main techniques applied to investigate the nanostructure of hyaluronan in its original, hydrated state.

    The present study on hydrogels shows that they possess inhomogeneous structures best described with two correlation lengths, one of the order of a few nanometers and the other in the order of few hundred nanometers. These gels are made up of dense polymer-rich clusters linked to each other. The polymer concentration and mixing governs the connectivity between these clusters, which in turn determines the viscoelastic properties of the gels. Surface-tethered HA at a solid-liquid interface is best described with a smooth varying density profile. The shape of this profile depends on the immobilization chemistry, the deposition protocol, and the ionic interactions. HA could be suitably modified to enhance adherence to metal surfaces, as well as incorporation of proteins like growth factors with tunable release properties. This could be exploited for surface coating of implants with bioactive molecules. The knowledge gained from this work would significantly help to develop future biomaterials and surface coatings of implants and biomedical devices.

    List of papers
    1. Structure of polymer and particle aggregates in hydrogel composites
    Open this publication in new window or tab >>Structure of polymer and particle aggregates in hydrogel composites
    2013 (English)In: Journal of Polymer Science Part B: Polymer Physics, ISSN 0887-6266, E-ISSN 1099-0488, Vol. 51, no 6, 421-429 p.Article in journal (Refereed) Published
    Abstract [en]

    Knowledge of the structure of a biomaterial is usually vital to control its function. This article provides a structural characterization of a hyaluronan scaffold that has demonstrated good biocompatibility and is used to induce bone regeneration. Hyaluronan hydrogels are appealing materials that can function as a matrix to incorporate both organic and inorganic substances to enhance tissue growth. Because of the intrinsic properties of this swollen matrix, one needs a very sensitive technique that can be applied in situ to determine the organization of the polymers in a gel. Small-angle neutron scattering is used to determine the characteristics of the inhomogeneous structure of the hydrogel both with and without added particles. The results are interpreted using models of structure with two length scales that are beyond the traditional picture of homogeneous gels. The observed structure and the dimensions can explain the previously reported rheological properties of gels containing different amount of polymers. Hydroxyapatite nanoparticles added to the gel are frozen in the gel matrix. We are able to determine the distribution and shape of these particles as they aggregate around the polymer chains. We have also concluded, in this case, that the particle structure is concentration independent. Information about the nanostructure for an applicable biomaterial guides the formulation, preparation, and use that should lead to further understanding of its exploitation.

    Keyword
    biopolymers, correlation length, hyaluronan, hydrogels, nanocomposites, neutron scattering
    National Category
    Natural Sciences
    Identifiers
    urn:nbn:se:uu:diva-197038 (URN)10.1002/polb.23230 (DOI)000315050800005 ()
    Available from: 2013-03-19 Created: 2013-03-18 Last updated: 2017-12-06Bibliographically approved
    2. Tuning the density profile of surface-grafted hyaluronan and the effect of counter-ions
    Open this publication in new window or tab >>Tuning the density profile of surface-grafted hyaluronan and the effect of counter-ions
    2013 (English)In: European Physical Journal E, ISSN 1292-8941, Vol. 36, no 7, 70- p.Article in journal (Refereed) Published
    Abstract [en]

    The present paper investigates the structure and composition of grafted sodium hyaluronanat a solid-liquid interface using neutron reflection. The solvated polymer at the surface could be described with a density profile that decays exponentially towards the bulk solution. The density profileof the polymer varied depending on the deposition protocol. A single-stage deposition resulted in denser polymer layers, while layers created with a two-stage deposition process were more diffuse and had an overall lower density. Despite the diffuse density profile, two-stage deposition leads to a highersurface excess. Addition of calcium ions causes a strong collapse of the sodium hyaluronan chains, increasing the polymer density near the surface. This effect is more pronounced on the sample prepared by two-stage deposition due to the initial less dense profile. This study provides an understanding at a molecular level of how surface functionalization alters the structure and howsurface layers respond to changes in calcium ions in the solvent.

    National Category
    Polymer Technologies Polymer Chemistry
    Identifiers
    urn:nbn:se:uu:diva-197814 (URN)10.1140/epje/i2013-13070-7 (DOI)000322872700002 ()
    Available from: 2013-04-04 Created: 2013-04-04 Last updated: 2014-02-17Bibliographically approved
    3. Adsorption and co-adsorption of human serum albumin and myoglobin with hyaluronan on different substrates
    Open this publication in new window or tab >>Adsorption and co-adsorption of human serum albumin and myoglobin with hyaluronan on different substrates
    Show others...
    (English)Manuscript (preprint) (Other academic)
    National Category
    Polymer Chemistry Materials Chemistry
    Identifiers
    urn:nbn:se:uu:diva-197815 (URN)
    Available from: 2013-04-12 Created: 2013-04-04 Last updated: 2013-05-06
    4. Polymeric Smart Coating Strategy for Titanium Implants
    Open this publication in new window or tab >>Polymeric Smart Coating Strategy for Titanium Implants
    Show others...
    2014 (English)In: Advanced Engineering Materials, ISSN 1438-1656, E-ISSN 1527-2648, Vol. 16, no 11, 1340-1350 p.Article in journal (Refereed) Published
    Abstract [en]

    Hyaluronan based hydrogel coatings can mimic extracellular matrix components and incorporate growth factors that can be released during a progressive degradation while new tissue regenerates. This paper describes a structural characterization of a hydrogel coating made of modified hyaluronan polymers and how these coatings interact with bone morphogenetic protein-2 (BMP-2). Quartz crystal microbalance and neutron reflectivity measurements were used for in-situ, real-time measurements of the adsorption properties of polymers and proteins on smooth titanium oxide surfaces that mimic implant products in orthopedics. The adsorption of BMP-2 on a bare titanium oxide surface is compared to that on titanium oxide coated with different chemically modified hyaluronan, the most important being hyaluronan with bisphosphonate groups (HA-BP). The subsequent release of the BMP-2 from these hydrogel coatings could be triggered by calcium ions. The amount of adsorbed protein on the surfaces as well as the amount of released protein both depend on the type of hyaluronan coating. We conclude that HA-BP coated titanium oxide surfaces provide an excellent material for growth factor delivery in-vivo.

    National Category
    Biomaterials Science Polymer Chemistry Polymer Technologies Materials Chemistry
    Identifiers
    urn:nbn:se:uu:diva-197816 (URN)10.1002/adem.201400009 (DOI)000344790000004 ()
    Available from: 2013-04-16 Created: 2013-04-04 Last updated: 2017-12-06Bibliographically approved
  • 29.
    Berts, Ida
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström.
    Fragneto, Giovanna
    Institut Laue-Langevin.
    Porcar, Lionel
    Institut Laue-Langevin.
    Hellsing, Maja S.
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy.
    Rennie, Adrian. R
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy.
    Adsorption and co-adsorption of human serum albumin and myoglobin with hyaluronan on different substratesManuscript (preprint) (Other academic)
  • 30.
    Berts, Ida
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström. Uppsala University, Science for Life Laboratory, SciLifeLab.
    Ossipov, Dmitri
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström. Uppsala University, Science for Life Laboratory, SciLifeLab.
    Fragneto, Giovanna
    Institut Laue-Langevin.
    Frisk, Andreas
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Physics.
    Rennie, Adrian. R
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Physics.
    Polymeric Smart Coating Strategy for Titanium Implants2014In: Advanced Engineering Materials, ISSN 1438-1656, E-ISSN 1527-2648, Vol. 16, no 11, 1340-1350 p.Article in journal (Refereed)
    Abstract [en]

    Hyaluronan based hydrogel coatings can mimic extracellular matrix components and incorporate growth factors that can be released during a progressive degradation while new tissue regenerates. This paper describes a structural characterization of a hydrogel coating made of modified hyaluronan polymers and how these coatings interact with bone morphogenetic protein-2 (BMP-2). Quartz crystal microbalance and neutron reflectivity measurements were used for in-situ, real-time measurements of the adsorption properties of polymers and proteins on smooth titanium oxide surfaces that mimic implant products in orthopedics. The adsorption of BMP-2 on a bare titanium oxide surface is compared to that on titanium oxide coated with different chemically modified hyaluronan, the most important being hyaluronan with bisphosphonate groups (HA-BP). The subsequent release of the BMP-2 from these hydrogel coatings could be triggered by calcium ions. The amount of adsorbed protein on the surfaces as well as the amount of released protein both depend on the type of hyaluronan coating. We conclude that HA-BP coated titanium oxide surfaces provide an excellent material for growth factor delivery in-vivo.

  • 31.
    Bhunia, Asamanjoy
    et al.
    Univ Ghent, Ctr Ordered Mat Organomet & Catalysis, Dept Inorgan & Phys Chem, Krijgslaan 281-S3, B-9000 Ghent, Belgium.;Univ Dusseldorf, Inst Anorgan Chem & Strukturchem, D-40204 Dusseldorf, Germany..
    Esquivel, Dolores
    Univ Ghent, Ctr Ordered Mat Organomet & Catalysis, Dept Inorgan & Phys Chem, Krijgslaan 281-S3, B-9000 Ghent, Belgium.;Univ Cordoba, Fac Sci, Dept Organ Chem, Nanochem & Fine Chem Res Inst IUIQFN, Campus Rabanales,Marie Curie Bldg,Ctra Nal 4, E-14071 Cordoba, Spain..
    Dey, Subarna
    Univ Dusseldorf, Inst Anorgan Chem & Strukturchem, D-40204 Dusseldorf, Germany..
    Fernandez-Teran, Ricardo
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Goto, Yasutomo
    Toyota Cent Res & Dev Labs Inc, Nagakute, Aichi 4801192, Japan..
    Inagaki, Shinji
    Toyota Cent Res & Dev Labs Inc, Nagakute, Aichi 4801192, Japan..
    Van der Voort, Pascal
    Univ Ghent, Ctr Ordered Mat Organomet & Catalysis, Dept Inorgan & Phys Chem, Krijgslaan 281-S3, B-9000 Ghent, Belgium..
    Janiak, Christoph
    Univ Dusseldorf, Inst Anorgan Chem & Strukturchem, D-40204 Dusseldorf, Germany..
    A photoluminescent covalent triazine framework: CO2 adsorption, light-driven hydrogen evolution and sensing of nitroaromatics2016In: Journal of Materials Chemistry A, ISSN 2050-7488, Vol. 4, no 35, 13450-13457 p.Article in journal (Refereed)
    Abstract [en]

    A highly photoluminescent (PL) porous covalent triazine-based framework (PCTF-8) is synthesized from tetra(4-cyanophenyl) ethylene by using trifluoromethanesulfonic acid as the catalyst at room temperature. Due to triazine units in the framework, the PCTF-8 exhibits excellent thermal stability (>400 degrees C). The Brunauer-Emmett-Teller (BET) specific surface area of PCTF-8 is 625 m(2) g(-1) which is lower than the one obtained from the synthesis under Lewis acid conditions (ZnCl2). At 1 bar and 273 K, the PCTF-8 adsorbs a significant amount of CO2 (56 cm(3) g(-1)) and CH4 (17 cm(3) g(-1)) which is highly comparable to nanoporous 1,3,5-triazine frameworks (NOP-1-6, 29-56 cm(3) g(-1)). This nitrogen rich framework exhibits good ideal selectivity (61 : 1 (85% N-2 : 15% CO2) at 273 K, 1 bar). Thus, it can be used as a promising candidate for potential applications in post-combustion CO2 capture and sequestration technologies. In addition, photoluminescence properties as well as the sensing behaviour towards nitroaromatics have been demonstrated. The fluorescence emission intensity of PCTF-8 is quenched by ca. 71% in the presence of 2,4,6-trinitrophenol (TNP). From time-resolved studies, a static quenching behaviour was found. This high photoluminescence property is used for hydrogen evolving organic photocatalysis from water in the presence of a sacrificial electron donor and a cocatalyst.

  • 32.
    Bielecki, Johan
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Biology, Department of Cell and Molecular Biology, Molecular biophysics. Chalmers, Dept Appl Phys, SE-41296 Gothenburg, Sweden..
    Parker, Stewart F.
    Rutherford Appleton Lab, STFC, ISIS Facil, Didcot OX11 0QX, Oxon, England..
    Mazzei, Laura
    Chalmers, Dept Appl Phys, SE-41296 Gothenburg, Sweden..
    Börjesson, Lars
    Chalmers, Dept Appl Phys, SE-41296 Gothenburg, Sweden..
    Karlsson, Maths
    Chalmers, Dept Appl Phys, SE-41296 Gothenburg, Sweden..
    Structure and dehydration mechanism of the proton conducting oxide Ba2In2O5(H2O)(x)2016In: Journal of Materials Chemistry A, ISSN 2050-7488, Vol. 4, no 4, 1224-1232 p.Article in journal (Refereed)
    Abstract [en]

    The structure and dehydration mechanism of the proton conducting oxide Ba2In2O5(H2O)(x) are investigated by means of variable temperature (20-600 degrees C) Raman spectroscopy together with thermal gravimetric analysis and inelastic neutron scattering. At room temperature, Ba2In2O5(H2O)(x) is found to be fully hydrated (x = 1) and to have a perovskite-like structure, which dehydrates gradually with increasing temperature and at around 600 degrees C the material is essentially dehydrated (x approximate to 0.2). The dehydrated material exhibits a brownmillerite structure, which is featured by alternating layers of InO6 octahedra and InO4 tetrahedra. The transition from a perovskite-like to a brownmillerite-like structure upon increasing temperature occurs through the formation of an intermediate phase at ca. 370 degrees C, corresponding to a hydration degree of approximately 50%. The structure of the intermediate phase is similar to the structure of the dehydrated material, but with the difference that it exhibits a non-centrosymmetric distortion of the InO6 octahedra that is not present in the dehydrated material. The dehydration process upon heating is a two-stage mechanism; for temperatures below the hydrated-to-intermediate phase transition, dehydration is characterized by a homogenous release of protons over the entire oxide lattice, whereas above the transition a preferential desorption of protons originating in the nominally tetrahedral layers is observed. Furthermore, our spectroscopic results point towards the co-existence of two structural phases, which relate to the two lowest-energy proton configurations in the material. The relative contributions of the two proton configurations depend on how the sample is hydrated.

  • 33.
    Biendicho, Jordi Jacas
    et al.
    The ISIS Facility, STFC Rutherford Appleton Laboratory, Oxfordshire 11 0QX, United Kingdom; and Department of Materials and Environmental Chemistry, Stockholm University, Stockholm 106 91, Sweden.
    Roberts, Matthew
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Noreus, Dag
    Department of Materials and Environmental Chemistry, Stockholm University, Stockholm 106 91, Sweden.
    Lagerqvist, Ulrika
    Nilar Svenska AB, Gavle 800 08, Sweden.
    Smith, Ronald I.
    The ISIS Facility, STFC Rutherford Appleton Laboratory, Oxfordshire 11 0QX, UK.
    Svensson, Gunnar
    Department of Materials and Environmental Chemistry, Stockholm University, Stockholm 106 91, Sweden.
    Norberg, Stefan T.
    Department of Chemical and Biological Engineering, Chalmers University of Technology, Sweden 412 96, Sweden.
    Eriksson, Sten G.
    Department of Chemical and Biological Engineering, Chalmers University of Technology, Sweden 412 96, Sweden.
    Hull, Stephen
    The ISIS Facility, STFC Rutherford Appleton Laboratory, Oxfordshire 11 0QX, UK.
    In situ investigation of commercial Ni(OH)(2) and LaNi5-based electrodes by neutron powder diffraction2015In: Journal of Materials Research, ISSN 0884-2914, E-ISSN 2044-5326, Vol. 30, no 3, 407-416 p.Article in journal (Refereed)
    Abstract [en]

    Electrochemical reactions at both positive and negative electrodes in a nickel metal hydride (Ni-MH) battery during charge have been investigated by in situ neutron powder diffraction. Commercially available beta-Ni(OH)(2) and LaNi5-based powders were used in this experiment as positive and negative electrodes, respectively. Exchange of hydrogen by deuterium for the beta-Ni(OH)(2) electrode was achieved by ex situ cycling of the cell prior to in situ measurements. Neutron diffraction data collected in situ show that the largest amount of deuterium contained at the positive electrode is de-intercalated from the electrode with no phase transformation involved up to similar to 100 mA h/g and, in addition, the 110 peak width for the positive electrode increases on charge. The negative electrode of composition MmNi(3.6)Al(0.4)Mn(0.3)Co(0.7), where Mm = Mischmetal, exhibits a phase transformation to an intermediate hydride gamma phase first and then to the beta phase on charge. Unit cell dimensions and phase fractions have been investigated by Rietveld refinement of the crystal structure.

  • 34.
    Blidberg, Andreas
    et al.
    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.
    Tengstedt, Carl
    Björefors, Fredrik
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Brant, William R.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Monitoring LixFeSO4F (x = 1, 0.5, 0) Phase Distributions in Operando To Determine Reaction Homogeneity in Porous Battery Electrodes2017In: Chemistry of Materials, ISSN 0897-4756, E-ISSN 1520-5002, Vol. 29, no 17, 7159-7169 p.Article in journal (Refereed)
  • 35.
    Blidberg, Andreas
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry. Uppsala universitet.
    Sobkowiak, Adam
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Tengstedt, Carl
    Scania CV AB.
    Valvo, Mario
    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.
    Björefors, Fredrik
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Battery Performance of PEDOT Coated LiFeSO4F Cathodes with Controlled PorosityManuscript (preprint) (Other academic)
  • 36.
    Blidberg, Andreas
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström.
    Sobkowiak, Adam
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström.
    Tengstedt, Carl
    Valvo, Mario
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström.
    Gustafsson, Torbjörn
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström.
    Björefors, Fredrik
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström.
    Insight Into the Electrochemcal Performance of PEDOT-coated Tavorite LiFeSO4F for Li-ion BatteriesManuscript (preprint) (Other academic)
  • 37.
    Borges, J.
    et al.
    Czech Tech Univ, Fac Elect Engn, Dept Control Engn, Tech 2, CR-16635 Prague 6, Czech Republic..
    Rodrigues, M. S.
    Univ Minho, Ctr Fis, P-4710057 Braga, Portugal.;Inst Pedro Nunes, Lab Ensaios Desgaste & Mat, P-3030199 Coimbra, Portugal..
    Kubart, Tomas
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Electronics.
    Kumar, S.
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Electronics.
    Leifer, Klaus
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Applied Materials Sciences.
    Evaristo, M.
    Univ Coimbra, Dept Mech Engn, SEG CEMUC, P-3030788 Coimbra, Portugal..
    Cavaleiro, A.
    Univ Coimbra, Dept Mech Engn, SEG CEMUC, P-3030788 Coimbra, Portugal..
    Apreutesei, M.
    INSA Lyon, MATEIS Lab, F-69621 Villeurbanne, France..
    Pereira, R. M. S.
    Univ Minho, Ctr Fis, P-4710057 Braga, Portugal.;Univ Minho, Ctr Matemat, Braga, Portugal..
    Vasilevskiy, M. I.
    Univ Minho, Ctr Fis, P-4710057 Braga, Portugal..
    Polcar, T.
    Czech Tech Univ, Fac Elect Engn, Dept Control Engn, Tech 2, CR-16635 Prague 6, Czech Republic.;Univ Southampton, Natl Ctr Adv Tribol Southampton nCATS, Southampton SO17 1BJ, Hants, England..
    Vaz, F.
    Univ Minho, Ctr Fis, P-4710057 Braga, Portugal..
    Thin films composed of gold nanoparticles dispersed in a dielectric matrix: The influence of the host matrix on the optical and mechanical responses2015In: Thin Solid Films, ISSN 0040-6090, E-ISSN 1879-2731, Vol. 596, 8-17 p.Article in journal (Refereed)
    Abstract [en]

    Gold nanoparticles were dispersed in two different dielectric matrices, TiO2 and Al2O3, using magnetron sputtering and a post-deposition annealing treatment. The main goal of the present work was to study how the two different host dielectric matrices, and the resulting microstructure evolution (including both the nanoparticles and the host matrix itself) promoted by thermal annealing, influenced the physical properties of the films. In particular, the structure and morphology of the nanocomposites were correlated with the optical response of the thin films, namely their localized surface plasmon resonance (LSPR) characteristics. Furthermore, and in order to scan the future application of the two thin film system in different types of sensors (namely biological ones), their functional behaviour (hardness and Young's modulus change) was also evaluated. Despite the similar Au concentrations in both matrices (similar to 11 at.%), very different microstructural features were observed, which were found to depend strongly on the annealing temperature. The main structural differences included: (i) the early crystallization of the TiO2 host matrix, while the Al2O3 one remained amorphous up to 800 degrees C; (ii) different grain size evolution behaviours with the annealing temperature, namely an almost linear increase for the Au:TiO2 system (from 3 to 11 nm), and the approximately constant values observed in the Au:Al2O3 system (4-5 nm). The results from the nanoparticle size distributions were also found to be quite sensitive to the surrounding matrix, suggesting different mechanisms for the nanoparticle growth (particle migration and coalescence dominating in TiO2 and Ostwald ripening in Al2O3). These different clustering behaviours induced different transmittance-LSPR responses and a good mechanical stability, which opens the possibility for future use of these nanocomposite thin film systems in some envisaged applications (e.g. LSPR-biosensors).

  • 38. Boschloo, Gerrit
    et al.
    Edvinsson, Tomas
    Hagfeldt, Anders
    Dye-sensitized nanostructured ZnO Electrodes for solar cell applications2007In: Nanostructured materials for solar energy conversion / [ed] Tetsuo Soga, Amsterdam: Elsevier Science , 2007Chapter in book (Refereed)
  • 39.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    A renaissance for Li-batterysolid polymer electrolytes2015Conference paper (Refereed)
  • 40.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    A Renaissance for SolidPolymer Electrolyte through Alternative Host Materials: Polycarbonates2015Conference paper (Refereed)
  • 41.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    EV batteries –challenges for power, capacity, lifetime, cost and sustainability2016Conference paper (Other academic)
  • 42.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Functionalized PolymerElectrolytes for Large and Small Li-Battery Applications: Experiments andModelling2014Conference paper (Refereed)
  • 43.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Molecular Dynamics ModellingSingel-Ion Conducting Polymer Electrolytes2013Conference paper (Refereed)
  • 44.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Novel solid polymerelectrolytes for large and small Li-ion battery applications2013Conference paper (Refereed)
  • 45.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Organic Batteries2016Conference paper (Other academic)
  • 46.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    PES/XPS Studies of the Interface Chemistry in PEO-Based Polymer Electrolyte Lithium-IonBatteries2012Conference paper (Refereed)
  • 47.
    Brandell, Daniel
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Ultrathin Solid Polymer Electrolytes forMicrobatteries2012Conference paper (Refereed)
  • 48.
    Brandell, Daniel
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Costa, Luciano
    MD simulating ternarybattery electrolyte systems: polymer, salt and ionic liquids2014Conference paper (Refereed)
  • 49.
    Brandell, Daniel
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Jeschull, Fabian
    How water-soluble bindercontrol the surface chemistry in Li-ion battery anodes2017Conference paper (Refereed)
  • 50.
    Brandell, Daniel
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Structural Chemistry.
    Jeschull, Fabian
    Tailoring the surfacechemistry of Li-ion battery anodes through the use of water-soluble functional functionalbinders2017Conference paper (Refereed)
1234567 1 - 50 of 510
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