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  • 1.
    Ahlström, Olle
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Characterizing the state of water in an amorphous magnesium carbonate using Dielectric spectroscopy2013Independent thesis Advanced level (professional degree), 20 credits / 30 HE creditsStudent thesis
    Abstract [en]

    In the industry of today, materials which can adsorb and hold large amounts of water are playing an important role. Here, the free and bound water carrying capacity of an amorphous magnesium carbonate is investigated. It is also determined how these parameters depend on the relative humidity of the surrounding environment. To do this, the technique of dielectric spectroscopy is employed. Along with the water binding properties, the concentration of charge carriers and the diffusion coefficient was determined. A smaller part of around 10-30 % of the water adsorbed was shown to behave as free water in the material. The concentration of charge carriers was calculated to be in an order of magnitude of 1018-1022 m-3 for the higher relative humidity environments. The diffusion coefficient was shown to be about 5*10-9 m2/s for the adsorption spectrum. This value is in good agreement with the value for OH- ions in water.

  • 2. Ahrentorp, Fredrik
    et al.
    Blomgren, Jacob
    Gómez de La Torre, Teresa Zardán
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Strömme, Maria
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Johansson, Christer
    Development of a sensitive induction based magnetic nanoparticlebiodetection method2018In: 12th International Conference on the Scientific and Clinical Applications of Magnetic Carriers, 2018Conference paper (Refereed)
  • 3. Ahrentorp, Fredrik
    et al.
    Blomgren, Jakob
    Jonasson, Christian
    Sarwe, Anna
    Sepehri, Sobhan
    Eriksson, Emil
    Kalaboukhov, Alexei
    Jesorka, Aldo
    Winkler, Dag
    Schneiderman, Justin F.
    Nilsson, Mats
    Albert, Jan
    Gómez de La Torre, Teresa Zardán
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Strömme, Maria
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Johansson, Christer
    Sensitive magnetic biodetection using magnetic multi-core nanoparticles and RCA coils2017In: Journal of Magnetism and Magnetic Materials, ISSN 0304-8853, E-ISSN 1873-4766, Vol. 427, no Supplement C, p. 14-18Article in journal (Refereed)
    Abstract [en]

    Abstract We use functionalized iron oxide magnetic multi-core particles of 100nm in size (hydrodynamic particle diameter) and AC susceptometry (ACS) methods to measure the binding reactions between the magnetic nanoparticles (MNPs) and bio-analyte products produced from DNA segments using the rolling circle amplification (RCA) method. We use sensitive induction detection techniques in order to measure the ACS response. The DNA is amplified via RCA to generate RCA coils with a specific size that is dependent on the amplification time. After about 75min of amplification we obtain an average RCA coil diameter of about 1µm. We determine a theoretical limit of detection (LOD) in the range of 11 attomole (corresponding to an analyte concentration of 55 fM for a sample volume of 200µL) from the ACS dynamic response after the MNPs have bound to the RCA coils and the measured ACS readout noise. We also discuss further possible improvements of the LOD.

  • 4. Ahrentorp, Fredrik
    et al.
    Blomgren, Jakob
    Jonasson, Christian
    Sarwe, Anna
    Sepehri, Sobhan
    Eriksson, Emil
    Kalaboukhov, Alexei
    Jesorka, Aldo
    Winkler, Dag
    Schneiderman, Justin F.
    Nilsson, Mats
    Albert, Jan
    Zardán Gómez de la Torre, Teresa
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Strømme, Maria
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Johansson, Christer
    Sensitive magnetic biodetection using magnetic multi-core nanoparticles and RCA coils2016In: Journal of Magnetism and Magnetic Materials, ISSN 0304-8853, E-ISSN 1873-4766, Vol. 427, p. 14-18Article in journal (Refereed)
    Abstract [en]

    We use functionalized iron oxide magnetic multi-core particles of 100 nm in size (hydrodynamic particle diameter) and AC susceptometry (ACS) methods to measure the binding reactions between the magnetic nanoparticles (MNPs) and bio-analyte products produced from DNA segments using the rolling circle amplification (RCA) method. We use sensitive induction detection techniques in order to measure the ACS response. The DNA is amplified via RCA to generate RCA coils with a specific size that is dependent on the amplification time. After about 75 min of amplification we obtain an average RCA coil diameter of about 1 µm. We determine a theoretical limit of detection (LOD) in the range of 11 attomole (corresponding to an analyte concentration of 55 fM for a sample volume of 200 µL) from the ACS dynamic response after the MNPs have bound to the RCA coils and the measured ACS readout noise. We also discuss further possible improvements of the LOD.

  • 5.
    Akhtar, Sultan
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Experimental Physics.
    Leifer, Klaus
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Experimental Physics.
    Strömberg, Mattias
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Strømme, Maria
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    TEM investigations of attachment of functionalized magnetic nanoparticles to DNA-coils acting as a biosensor2010In: Scandem 2010, Stockholm, Sweden, June 8-11, 2010Conference paper (Refereed)
  • 6.
    Akhtar, Sultan
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Experimental Physics.
    Rubino, Stefano
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Experimental Physics.
    Jansson, Ulf
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Materials Chemistry.
    Yang, W.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Biochemistry and Organic Chemistry.
    Grennberg, Helena
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Biochemistry and Organic Chemistry.
    Strömberg, Mattias
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Strömme, Maria
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Leifer, Klaus
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Experimental Physics.
    Visualization of functionalization of nano-particles and graphene in the TEM2010In: Advanced Materials Workshop 2010, 2010Conference paper (Refereed)
    Abstract [en]

    Recently, the activity on functionalized nano-objects has strongly increased. Yet, there are, to our knowledge no techniques available that visualize the attachment of molecules to nano-entities such as nanoparticles and graphene. In this work, we show a methodology to analyse the attachment of molecules to nanoparticles and graphene. The difficulty of such transmission electron microscopy (TEM) characterization consists in the high beam sensitivity of these nanoobjects. We employed a high resolution- as well as diffraction contrast-imaging methods to characterize graphene. First, we have developed a method to measure the thickness of free-standing graphene-like layers. The refinement of these imaging techniques enabled the imaging of functionalized C60 (fullerene) on top of a few-layer graphene flake by TEM. We also developed a methodology to visualize the attachment of functionalized gold and magnetic nanoparticles (different sizes) to nonstained and unlabeled single strand DNA-coils. This technique can be used to understand the interaction of a large variety of functionalized nanoparticles with their solution environment and/or macromolecular structures for their large applications.

  • 7.
    Akhtar, Sultan
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Experimental Physics.
    Strömberg, Mattias
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Zardán Gómez de la Torre, Teresa
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Russell, Camilla
    Uppsala University, Disciplinary Domain of Medicine and Pharmacy, Faculty of Medicine, Department of Genetics and Pathology.
    Gunnarsson, Klas
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Physics.
    Nilsson, Mats
    Uppsala University, Disciplinary Domain of Medicine and Pharmacy, Faculty of Medicine, Department of Genetics and Pathology.
    Svedlindh, Peter
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Physics.
    Strömme, Maria
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Leifer, Klaus
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Experimental Physics.
    Real-Space Transmission Electron Microscopy Investigations of Attachment of Functionalized Magnetic Nanoparticles to DNA-Coils Acting as a Biosensor2010In: Journal of Physical Chemistry B, ISSN 1520-6106, E-ISSN 1520-5207, Vol. 114, no 41, p. 13255-13262Article in journal (Refereed)
    Abstract [en]

    The present work provides the first real-space analysis of nanobead-DNA coil interactions. Immobilization of oligonucleotide-functionalized magnetic nanobeads in rolling circle amplified DNA-coils was studied by complex magnetization measurements and transmission electron microscopy (TEM), and a statistical analysis of the number of beads hybridized to the DNA-coils was performed. The average number of beads per DNAcoil using the results from both methods was found to be around 6 and slightly above 2 for samples with 40 and 130 nm beads, respectively. The TEM analysis supported an earlier hypothesis that 40 nm beads are preferably immobilized in the interior of DNA-coils whereas 130 nm beads, to a larger extent, are immobilized closer to the exterior of the coils. The methodology demonstrated in the present work should open up new possibilities for characterization of interactions of a large variety of functionalized nanoparticles with macromolecules, useful for gaining more fundamental understanding of such interactions as well as for optimizing a number of biosensor applications.

  • 8.
    Alvebratt, Caroline
    et al.
    Uppsala University, Disciplinary Domain of Medicine and Pharmacy, Faculty of Pharmacy, Department of Pharmacy.
    Cheung, Ocean
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Strömme, Maria
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Bergström, Christel A S
    A Modified In Situ Method to Determine Release from a Complex Drug Carrier in Particle-Rich Suspensions.2018In: AAPS PharmSciTech, ISSN 1530-9932, E-ISSN 1530-9932Article in journal (Refereed)
    Abstract [en]

    Effective and compound-sparing methods to evaluate promising drug delivery systems are a prerequisite for successful selection of formulations in early development stages. The aim of the study was to develop a small-scale in situ method to determine drug release and supersaturation in highly concentrated suspensions of enabling formulations. Mesoporous magnesium carbonate (MMC), which delivers the drug in an amorphous form, was selected as a drug carrier. Five model compounds were loaded into the MMC at a 1:10 ratio using a solvent evaporation technique. The μDiss Profiler was used to study the drug release from MMC in fasted-state simulated intestinal fluid. To avoid extensive light scattering previously seen in particle-rich suspensions in the μDiss Profiler, an in-house-designed protective nylon filter was placed on the in situ UV probes. Three types of release experiments were conducted for each compound: micronized crystalline drug with MMC present, drug-loaded MMC, and drug-loaded MMC with 0.01% w/w hydroxypropyl methyl cellulose. The nylon filters effectively diminished interference with the UV absorption; however, the release profiles obtained were heavily compound dependent. For one of the compounds, changes in the UV spectra were detected during the release from the MMC, and these were consistent with degradation of the compound. To conclude, the addition of protective nylon filters to the probes of the μDiss Profiler is a useful contribution to the method, making evaluations of particle-rich suspensions feasible. The method is a valuable addition to the current ones, allowing for fast and effective evaluation of advanced drug delivery systems.

  • 9.
    Alvebratt, Caroline
    et al.
    Uppsala University, Disciplinary Domain of Medicine and Pharmacy, Faculty of Pharmacy, Department of Pharmacy.
    Petersson, E.
    Strömme, Maria
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Bergström, Christel
    Uppsala University, Disciplinary Domain of Medicine and Pharmacy, Faculty of Pharmacy, Department of Pharmacy.
    A small scale method to determine release rate from complexcarrier-mediated systems. 2016In: AAPS Annual Meeting and Exposition. Denver, November 13-17, 2016. / [ed] AAPS, 2016Conference paper (Refereed)
  • 10.
    Alvebratt, Caroline
    et al.
    Uppsala University, Disciplinary Domain of Medicine and Pharmacy, Faculty of Pharmacy, Department of Pharmacy.
    Petersson, E.
    Strömme, Maria
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Bergström, Christel
    Uppsala University, Disciplinary Domain of Medicine and Pharmacy, Faculty of Pharmacy, Department of Pharmacy.
    Dissolution studies of solid formulations - Applicability of µDiss inmonitoring supersaturation, nucleation and crystallization behavior; Casestudy: Carrier-based formulation.2016In: pION Fiber Optic Advanced Training Course. Uppsala, June 14-15, 2016., 2016Conference paper (Refereed)
  • 11.
    Alvebratt, Caroline
    et al.
    Uppsala University, Disciplinary Domain of Medicine and Pharmacy, Faculty of Pharmacy, Department of Pharmacy.
    Petersson, Erik
    Strömme, Maria
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Bergström, Christel
    A small scale method to determine release rate from complex carrier-mediated systems2016In: Emerging Technologies in Drug Discovery and Development. Zhuhai, August 23-26, 2016., 2016Conference paper (Refereed)
  • 12.
    Alvebratt, Caroline
    et al.
    Uppsala University, Disciplinary Domain of Medicine and Pharmacy, Faculty of Pharmacy, Department of Pharmacy.
    Strömme, Maria
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Bergström, Christel
    Uppsala University, Disciplinary Domain of Medicine and Pharmacy, Faculty of Pharmacy, Department of Pharmacy.
    A new method that enables in situ measurement of drug release from complex carrier-mediated systems2017In: 6th FIP Pharmaceutical Sciences World Congress2017., 2017Conference paper (Refereed)
  • 13.
    Araujo, Rafael B.
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Theory.
    Banerjee, Amitava
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Theory.
    Panigrahi, Puspamitra
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Theory. Hindustan Univ, Ctr Clean Energy & Nanoconvergence, Madras, Tamil Nadu, India.
    Yang, Li
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Sjödin, Martin
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Strömme, Maria
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Araujo, C. Moyses
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Theory.
    Ahuja, Rajeev
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Theory. Royal Inst Technol KTH, Dept Mat, Appl Mat Phys, S-10044 Stockholm, Sweden.; Royal Inst Technol KTH, Dept Engn, S-10044 Stockholm, Sweden.
    Assessing Electrochemical Properties of Polypyridine and Polythiophene for Prospective Application in Sustainable Organic Batteries2017In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 19, no 4, p. 3307-3314Article in journal (Refereed)
    Abstract [en]

    Conducting polymers are being considered promising candidates for sustainable organic batteries mainly due to their fast electron transport properties and high recyclability. In this work, key properties of polythiophene and polypyridine have been assessed through a combined theoretical and experimental study focusing on such applications. A theoretical protocol has been developed to calculate redox potentials in solution within the framework of the density functional theory and using continuous solvation models. Here, the evolution of the electrochemical properties of solvated oligomers as a function of the length of the chain is analyzed and then the polymer properties are estimated via linear regressions using ordinary least square. The predicted values were verified against our electrochemical experiments. This protocol can now be employed to screen a large database of compounds in order to identify organic electrodes with superior properties.

  • 14.
    Araujo, Rafael B.
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Theory.
    Banerjee, Amitava
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Theory.
    Panigrahi, Puspamitra
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Theory. Hindustan Univ, Ctr Clean Energy & Nanoconvergence, Chennai, Tamil Nadu, India.
    Yang, Li
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Strömme, Maria
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Sjödin, Martin
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Araujo, C. Moyses
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Theory.
    Ahuja, Rajeev
    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.
    Designing strategies to tune reduction potential of organic molecules for sustainable high capacity batteries application2017In: Journal of Materials Chemistry A, ISSN 2050-7488, Vol. 5, no 9, p. 4430-4454Article in journal (Refereed)
    Abstract [en]

    Organic compounds evolve as a promising alternative to the currently used inorganic materials in rechargeable batteries due to their low-cost, environmentally friendliness and flexibility. One of the strategies to reach acceptable energy densities and to deal with the high solubility of known organic compounds is to combine small redox active molecules, acting as capacity carrying centres, with conducting polymers. Following this strategy, it is important to achieve redox matching between the chosen molecule and the polymer backbone. Here, a synergetic approach combining theory and experiment has been employed to investigate this strategy. The framework of density functional theory connected with the reaction field method has been applied to predict the formal potential of 137 molecules and identify promising candidates for the referent application. The effects of including different ring types, e.g. fused rings or bonded rings, heteroatoms, [small pi] bonds, as well as carboxyl groups on the formal potential, has been rationalized. Finally, we have identified a number of molecules with acceptable theoretical capacities that show redox matching with thiophene-based conducting polymers which, hence, are suggested as pendent groups for the development of conducting redox polymer based electrode materials.

  • 15.
    Asper, M.
    et al.
    Charles River Biopharmaceut Serv GmbH, D-51105 Cologne, Germany..
    Hanrieder, T.
    Charles River Biopharmaceut Serv GmbH, D-51105 Cologne, Germany..
    Quellmalz, Arne
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Mihranyan, Albert
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Removal of xenotropic murine leukemia virus by nanocellulose based filter paper2015In: Biologicals (Print), ISSN 1045-1056, E-ISSN 1095-8320, Vol. 43, no 6, p. 452-456Article in journal (Refereed)
    Abstract [en]

    The removal of xenotrpic murine leukemia virus (xMuLV) by size-exclusion filter paper composed of 100% naturally derived cellulose was validated. The filter paper was produced using cellulose nanofibers derived from Cladophora sp. algae. The filter paper was characterized using atomic force microscopy, scanning electron microscopy, helium pycnometry, and model tracer (100 nm latex beads and 50 nm gold nanoparticles) retention tests. Following the filtration of xMuLV spiked solutions, LRV >= 5.25 log(10) TCID50 was observed, as limited by the virus titre in the feed solution and sensitivity of the tissue infectivity test. The results of the validation study suggest that the nanocellulose filter paper is useful for removal of endogenous rodent retroviruses and retrovirus-like particles during the production of recombinant proteins.

  • 16.
    Atluri, Rambabu
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Novel Syntheses, Structures and Functions of Mesoporous Silica Materials2010Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    The field of mesoporous silica has been studied for about 20 years but it is still an area attracting a lot of attention. The use of novel templating molecules and several issues related to the synthesis and fine structural details are still poorly understood. These aspects are of special relevance to the theme of this thesis, which includes novel work on three fronts; the synthesis, characterization and applications of mesoporous materials.

    The work described in this thesis aims to contribute to the mesoporous field by developing novel methods of mesoporous silica synthesis without relying on surfactant micelles as the templating agent but focusing instead on the stacking arrangement of aromatic molecules such as folic acid. The novel route presented here leads to 2D hexagonal structures with p6mm symmetry possessing high mesoporosity and large surface areas. The versatility of this route at various synthesis temperatures and using hydrothermal treatments has also been investigated.

    A novel strategy is also proposed for the synthesis of mesocaged materials with Pm3n symmetry structures. The mechanism relies on the penetration of the neutral propylamino moiety of a co-structure directing agent into the hydrophobic core of the surfactant micelles. Beside these novel pathways, the effect of hydrothermal treatment (HT) at 100 oC on the 3D cubic Ia3d structure (AMS-6) over a long period of time was also examined, and the results show a phase transformation from a 3D cubic Ia3d to a 2D hexagonal p6mm structure and a return to the 3D cubic Ia3d structure at a later stage in the synthesis. This unexpected result is discussed.

    In this work, the detailed structural characterization of mesoporous materials using electron microscopy techniques is an important task. In particular, to extend previous knowledge, the fine structural details of mesocaged materials possessing Pm3n symmetry prepared with various amphiphilic surfactants under acidic and alkaline conditions has been investigated using electron crystallography and sorption studies. The results show subtle fine structural differences with materials prepared under alkaline conditions exhibiting the largest mesocage sizes. The cage and window sizes are primarily determined by the charge density of the surfactant and the thickness of the hydration layer surrounding the surfactant micelles.

    The relationship between the mesoporous structure and its function has been investigated by evaluating the rate of release of amphiphilic molecules, used as model molecules, from the internal pore structures of mesoporous materials with different pore geometries. In a similar study, the rate of proton diffusion from a liquid surrounding the mesoporous nanoparticles into the pore system of AMS-n was also assessed. The results show that the diffusion coefficients for the proton absorption process are higher than those for the release of the surfactant template molecules, with more complex 3D mesocaged particles showing the highest diffusion coefficients in both cases.

    Finally, the quantity of CO2 adsorption was measured by modifying the internal surfaces of mesocaged material with n-propylamino groups. Results show that the cage-connecting window sizes limit the surface coverage of n-propylamino groups by pore blocking and affect the volume of CO2 adsorption. In addition, at the molecular level, CO2 adsorption shows physisorption or chemisorption depending on the localized distribution of n-propylamino groups, as studied by in-situ infrared spectroscopy.

    List of papers
    1. Structural variations in mesoporous materials with cubic Pm3n symmetry
    Open this publication in new window or tab >>Structural variations in mesoporous materials with cubic Pm3n symmetry
    2010 (English)In: Microporous and Mesoporous Materials, ISSN 1387-1811, E-ISSN 1873-3093, Vol. 133, no 1-3, p. 27-35Article in journal (Refereed) Published
    Abstract [en]

    The fine structural details of mesoporous materials possessing Pm3n symmetry prepared with varying amphiphilic surfactants under acid and alkaline conditions are investigated using electron crystallography and sorption studies. The structural data derived is used to understand the parameters that govern the formation of cavity-windows and to propose synthetic strategies in order to control independently the size of the cavities and cavity-windows. Results support that whilst attainment of Pm3n cubic packing is due to the overall surfactant geometry, the formation of cavity-windows is associated with the hydration layer formed at the interphase between the surfactant and the silica wall.  The charge density at the micelle surface may be tailored using two strategies: (i) using dicationic gemini surfactants at low pHs resulting in an increase in the hydration layer; or (ii) by using co-structure directing agents such as organoalkoxysilanes which reduce the hydration layer surrounding the micelles. The latter leads to the formation of higher cavity sizes and may be useful for tuning fine structural details of mesoporous materials when considering their use in important applications such as gas separation.

    Keywords
    Amphiphilic surfactants, Mesoporous materials, Electron microscopy, Structural solutions, Gas separation
    National Category
    Materials Engineering
    Research subject
    Materials Science
    Identifiers
    urn:nbn:se:uu:diva-121984 (URN)10.1016/j.micromeso.2010.04.007 (DOI)000279061000004 ()
    Available from: 2010-04-06 Created: 2010-04-03 Last updated: 2017-12-12Bibliographically approved
    2. Nonsurfactant Supramolecular Synthesis of Ordered Mesoporous Silica
    Open this publication in new window or tab >>Nonsurfactant Supramolecular Synthesis of Ordered Mesoporous Silica
    2009 (English)In: Journal of the American Chemical Society, ISSN 0002-7863, E-ISSN 1520-5126, Vol. 131, no 9, p. 3189-3191Article in journal (Refereed) Published
    Abstract [en]

    Hoogsteen-bonded tetrads and pentamers are formed by a large variety of organic molecules through H-donor and acceptor groups capable of inducing self-organization to form columnar and hexagonal mesophases. The biological importance of such macromolecular structures is exemplified by the assembly of guanosine-rich groups of telomere units and their implication in chromosomal replication. Folic acid is composed of a pterin group, chemically and structurally similar to guanine, conjugated to an l-glutamate moiety via a p-amino benzoic acid. Our aim has been to develop a delivery vehicle for folic acid and at the same time provide a novel synthetic route for ordered mesoporous materials without the use of amphiphilic surfactants. We present a new nonsurfactant route for the synthesis of highly ordered mesoporous materials, based on the supramolecular templating of stacked arrays of the tetramer-forming pterin groups of folic acid under a variety of synthetic conditions. This method leads to hexagonally ordered mesoporous structures with gyroid, spherical, and chiral morphologies with pores on the order of 25−30 Å in diameter and surface areas above 1000 m2/g. More importantly circular dichroism studies reveal that the folate template possesses a chiral signature within the pores in the as-synthesized solid and that chirality is transferred from the folate template to the pore surface via the aminopropyl triethoxysilane costructure directing agent used in the supramolecular assembly. This novel templating approach for ordered mesoporous materials breaks the hegemony of surfactant micellar systems for the preparation of these exciting high surface area solids and opens new opportunities for structural control, design of pore geometry, and novel applications.

    National Category
    Engineering and Technology
    Research subject
    Engineering Science with specialization in Nanotechnology and Functional Materials
    Identifiers
    urn:nbn:se:uu:diva-99093 (URN)10.1021/ja8096477 (DOI)000264792400033 ()19220057 (PubMedID)
    Available from: 2009-03-06 Created: 2009-03-06 Last updated: 2017-12-13Bibliographically approved
    3. Hydrothermal Phase Transformation of Bicontinuous Cubic Mesoporous Material AMS-6
    Open this publication in new window or tab >>Hydrothermal Phase Transformation of Bicontinuous Cubic Mesoporous Material AMS-6
    2008 (English)In: Chemistry of Materials, ISSN 0897-4756, E-ISSN 1520-5002, Vol. 20, no 12, p. 3857-3866Article in journal (Refereed) Published
    Abstract [en]

    The controlled synthesis of ordered anionic surfactant templated mesoporous silica with cubic Ia3 structure (AMS-6) is reported via prolonged periods of hydrothermal treatment (HT). The cubic Ia3 mesophase transforms to hexagonal p6mm after 8 days of HT at 100 °C. Surprisingly, the hexagonal phase is stable only for a limited period after which a reversal to the cubic Ia3 mesostructure is observed. Characterization methods such as powder X-ray diffraction (XRD), electron microscopy (SEM, TEM), N2-isotherms, magic-angle spinning (MAS) 29Si NMR spectroscopy, and thermogravimetric analysis (TGA) have been employed to follow structural and textural changes of the materials prepared. Data show that the resultant mesostructure and its textural properties are highly dependent on the period of HT with less unit-cell shrinkage on calcination after extensive HT. Furthermore, evidence of two different solid−solid phase mechanisms during HT is presented. The initial transition is consistent with a restructuring of the surfactant packing and a depletion of the organic moieties from the organo-silica wall as evident from 29Si NMR spectroscopy. The return to the bicontinuous cubic phase is driven by changes in charge matching at the organic−inorganic interface as a result of increases in the polymerization of the silica wall. The textural properties, and in particular the presence or absence of surface porosity, has been controlled through variations in hydrothermal treatment. These are associated with specific growth directions of cubic AMS-6 crystals. The synthetic method described allows us to easily prepare phase pure and intermediate mesostructured nanoparticles.

    National Category
    Other Materials Engineering
    Research subject
    Engineering Science with specialization in Nanotechnology and Functional Materials
    Identifiers
    urn:nbn:se:uu:diva-98531 (URN)10.1021/cm702440n (DOI)000256854800015 ()
    Available from: 2009-02-25 Created: 2009-02-25 Last updated: 2017-12-13Bibliographically approved
    4. Co-Structure Directing Agent Induced Phase Transformation of Mesoporous Materials
    Open this publication in new window or tab >>Co-Structure Directing Agent Induced Phase Transformation of Mesoporous Materials
    2009 (English)In: Langmuir, ISSN 0743-7463, E-ISSN 1520-5827, Vol. 25, no 5, p. 3189-3195Article in journal (Refereed) Published
    Abstract [en]

    The synthesis of cubic Pmn mesocaged solid templated by cetyltrimethyl ammonium bromide (C16TMABr) surfactant by direct cocondensation of (3-aminopropyl)triethoxysilanes (APES) under strong alkaline conditions is reported. The novel route gives direct incorporation of amino functional groups on the porous silica wall, and the structural formation has been followed by means of in situ SAXS studies performed at a synchrotron beam line. Data shows that a molar ratio of C16TMABr/APES = 0.6 favors the formation of 3D cubic mesocaged solid with Pmn symmetry which transforms to a cylindrical mesoporous phase with p6mm symmetry at higher molar ratios. Further structural evaluation has been performed by means electron crystallography (EC). Reconstructed 3D models based on EC show the presence of spherical cages (A-cages, 45 Å) and ellipsoidal cages (B-cages, 48 × 43 Å) whereby every cage in the unit cell is connected to 14 nearest cages with a window size of 18 Å. Finally, a mechanism is proposed, denoted S+NoI, in which penetration of the neutral aminopropyl moiety within the micellar corona is responsible for the formation of the Pmn phase, accounting for the formation of the hexagonal phase at higher molar ratios and higher temperatures. In comparison to other mesocaged materials with the same symmetry this structure possesses a more open porous network which will help assess its potential in a variety of applications discussed herein.

    National Category
    Other Materials Engineering
    Research subject
    Engineering Science with specialization in Nanotechnology and Functional Materials
    Identifiers
    urn:nbn:se:uu:diva-99092 (URN)10.1021/la803727u (DOI)000263770800097 ()
    Available from: 2009-03-06 Created: 2009-03-06 Last updated: 2017-12-13Bibliographically approved
    5. Temperature-Induced Uptake of CO2 and Formation of Carbamates in Mesocaged Silica Modified with n-Propylamines
    Open this publication in new window or tab >>Temperature-Induced Uptake of CO2 and Formation of Carbamates in Mesocaged Silica Modified with n-Propylamines
    2010 (English)In: Langmuir, ISSN 0743-7463, E-ISSN 1520-5827, Vol. 26, no 12, p. 10013-10024Article in journal (Refereed) Published
    Abstract [en]

    Adsorption-mediated CO2 separation can reduce the costs of carbon capture and storage. The reduction in cost requires adsorbents with high capacities for CO2 sorption and high CO2-over-N2 selectivity. Amine-modified sorbents are promising candidates for carbon capture. To investigate the details of CO2 adsorption in such materials, we studied mesocaged (cubic, Pm3n symmetry) silica adsorbents with tethered propylamines using Fourier transform infrared (FTIR) spectroscopy and volumetric uptake experiments. The degree of heterogeneity in these coatings was varied by either co-synthesizing or post-synthetically introducing the propylamine modification. In situ FTIR spectroscopy revealed the presence of both physisorbed and chemisorbed CO2 in the materials. We present the first direct molecular evidence for physisorption using FTIR spectroscopy in mesoporous silica sorbents modified with propylamines. Physisorption reduced the CO2-over-N2 selectivity in amine-rich sorbents. Samples with homogenous coatings showed typical CO2 adsorption trends and large quantities of IR-observable physisorbed CO2. The uptake of CO2 in mesocaged materials with heterogeneous propylamine coatings was higher at high temperatures than at low temperatures. At higher temperatures and low pressures, the post-synthetically modified materials adsorbed more CO2 than did the extracted ones, even though the surface area after modification was clearly reduced and the coverage of primary amine groups was lower. The principal mode of CO2 uptake in post-synthetically modified mesoporous silica was chemisorption. The chemisorbed moieties were present mainly as carbamate–ammonium ion pairs, resulting from the quantitative transformation of primary amine groups during CO2 adsorption as established by NIR spectroscopy. The heterogeneity in the coatings promoted the formation of these ion pairs. The average propylamine–propylamine distance must be small to allow the formation of carbamate–propylammonium ion pairs.

    Keywords
    carbon dioxide, propylamine, adsorption, IR, FTIR, silica, mesoporous
    National Category
    Materials Engineering
    Research subject
    Materials Science
    Identifiers
    urn:nbn:se:uu:diva-121987 (URN)10.1021/la1001495 (DOI)000278427600114 ()
    Available from: 2010-04-06 Created: 2010-04-03 Last updated: 2017-12-12Bibliographically approved
    6. Sustained Release from Mesosporous Nanoparticles: evaluation of structural properties associated with controlled release rate
    Open this publication in new window or tab >>Sustained Release from Mesosporous Nanoparticles: evaluation of structural properties associated with controlled release rate
    2008 (English)In: Current Drug Delivery, ISSN 1567-2018, E-ISSN 1875-5704, Vol. 5, no 3, p. 177-185Article in journal (Refereed) Published
    Abstract [en]

    We present here a detailed study of the controlled release of amino acid derived amphiphilic molecules from the internal pore structure of mesoporous nanoparticle drug delivery systems with different structural properties; namely cubic and hexagonal structures of various degrees of complexity. The internal pore surface of the nanomaterials presented has been functionalised with amine moieties through a one pot method. Release profiles obtained by Alternating Ionic Current measurements are interpreted in terms of specific structural and textural parameters of the porous nanoparticles such as pore geometry and connectivity. Results indicate that diffusion coefficients are lower by as much as four orders of magnitude in 2-dimensional structures in comparison to 3-dimensional mesoporous solids. A fast release in turn is observed from mesocaged materials AMS-9 and AMS-8 where the presence of structural defects is thought to lead to a slightly lower diffusion coefficient in the latter. Amount of pore wall functionalisation and number of binding sites on the model drug are found to have little effect on the drug release rate.

    National Category
    Nano Technology
    Research subject
    Engineering Science with specialization in Nanotechnology and Functional Materials
    Identifiers
    urn:nbn:se:uu:diva-17498 (URN)10.2174/156720108784911686 (DOI)18673261 (PubMedID)
    Available from: 2008-08-07 Created: 2008-08-07 Last updated: 2017-12-08Bibliographically approved
    7. Proton Absorption in As-Synthesized Mesoporous Silica Nanoparticles as a Structure-Function Relationship Probing Mechanism
    Open this publication in new window or tab >>Proton Absorption in As-Synthesized Mesoporous Silica Nanoparticles as a Structure-Function Relationship Probing Mechanism
    Show others...
    2009 (English)In: Langmuir, ISSN 0743-7463, E-ISSN 1520-5827, Vol. 25, no 8, p. 4306-4310Article in journal (Refereed) Published
    Abstract [en]

    A new method to investigate the effect of pore geometry on diffusion processes in mesoporous silica nanoparticles and other types of micro- and mesoporous structures is put forward. The method is based onthe study of proton diffusion from a liquid surrounding the mesoporous particles into the particle pore system. The proton diffusion properties are assessed for a variety of as-synthesized mesoporous nano- and microparticles with two-dimensional and three-dimensional connectivity. Results show that the diffusion coefficients are higher for the proton absorption process than for the release of surfactant template molecules, and that they overall follow the same trend with the more complex three-dimensional mesocaged particles showing the highest diffusion coefficients. The pore geometry (cylindrical pores versus cage-type pores) and structure connectivity are found to play a key role for the effects observed. The results put forward in the present work should offer a valuable tool in the development of porous nanomaterials in a range of applications including the use as catalysis and separation enhancers in the petrochemical industry, as scaffolds for hydrogen storage, and as drug delivery vehicles for sustained release and gene transfection.

    National Category
    Engineering and Technology
    Research subject
    Engineering Science with specialization in Nanotechnology and Functional Materials
    Identifiers
    urn:nbn:se:uu:diva-100974 (URN)10.1021/la900105u (DOI)000265281700015 ()19281159 (PubMedID)
    Available from: 2009-04-15 Created: 2009-04-15 Last updated: 2017-12-13Bibliographically approved
  • 17.
    Atluri, Rambabu
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Bacsik, Zoltán
    Stockholm University.
    Hedin, Niklas
    Stockholm University.
    Garcia-Bennett, Alfonso E.
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Structural variations in mesoporous materials with cubic Pm3n symmetry2010In: Microporous and Mesoporous Materials, ISSN 1387-1811, E-ISSN 1873-3093, Vol. 133, no 1-3, p. 27-35Article in journal (Refereed)
    Abstract [en]

    The fine structural details of mesoporous materials possessing Pm3n symmetry prepared with varying amphiphilic surfactants under acid and alkaline conditions are investigated using electron crystallography and sorption studies. The structural data derived is used to understand the parameters that govern the formation of cavity-windows and to propose synthetic strategies in order to control independently the size of the cavities and cavity-windows. Results support that whilst attainment of Pm3n cubic packing is due to the overall surfactant geometry, the formation of cavity-windows is associated with the hydration layer formed at the interphase between the surfactant and the silica wall.  The charge density at the micelle surface may be tailored using two strategies: (i) using dicationic gemini surfactants at low pHs resulting in an increase in the hydration layer; or (ii) by using co-structure directing agents such as organoalkoxysilanes which reduce the hydration layer surrounding the micelles. The latter leads to the formation of higher cavity sizes and may be useful for tuning fine structural details of mesoporous materials when considering their use in important applications such as gas separation.

  • 18.
    Atluri, Rambabu
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Garcia Bennett, Alfonso
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Synthesis and Structural control of novel mesoporous material AMS-62007Conference paper (Refereed)
    Abstract [en]

    An in-depth study of the synthesis and growth of bicontinuous cubic mesoporous AMS-6 material in the presence of polymeric dispersant P123 is presented, resulting in controlled particle shape attainable over a small range of synthesis conditions. Unlike previous syntheses a remarkable effect on facet formation of the Iad silica particles with cubic morphologies is observed. Trapezoidal icositetrahedra, spherical and elongated morphologies have been prepared with increased faceting on addition of higher concentration of dispersant. Particles are characterised extensively by powder X-ray diffraction, transmission electron microscopy, scanning electron microscopy and nitrogen sorption isotherms. Mesoporous materials produced in this study show textural features suggesting a secondary porous network formed on the external surface of the particle and the origin of this secondary porosity is discussed. Based on the reduced dynamics generated by the presence of the P123 dispersant, we suggest possible growth models for the formation of mainly two different morphologies—the thermodynamically favoured trapezoidal icositetrahedron and elongated particles, the latter not following the expected point group symmetry, mm.

  • 19.
    Atluri, Rambabu
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Garcia-Bennett, Alfonso
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Comparative Structural study on Mesocaged porous materials with Pm3n Symmetry2008Conference paper (Refereed)
  • 20.
    Atluri, Rambabu
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Garcia-Bennett, Alfonso
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Controlling the phase transformation of AMS-6 mesoporous material via hydrothermal treatment2007Conference paper (Refereed)
  • 21.
    Atluri, Rambabu
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Garcia-Bennett, Alfonso
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Structural solution of complex low symmetry structure AMS-92008Conference paper (Refereed)
  • 22.
    Atluri, Rambabu
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Garcia-Bennett, Alfonso E.
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Structural variations in mesocaged materials with Pm3n symmetry2009Conference paper (Refereed)
  • 23.
    Atluri, Rambabu
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Garcia-Bennett, Alfonso
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Hedin, Niklas
    Hydrothermal Phase Transformation of Bicontinuous Cubic Mesoporous Material AMS-62008In: Chemistry of Materials, ISSN 0897-4756, E-ISSN 1520-5002, Vol. 20, no 12, p. 3857-3866Article in journal (Refereed)
    Abstract [en]

    The controlled synthesis of ordered anionic surfactant templated mesoporous silica with cubic Ia3 structure (AMS-6) is reported via prolonged periods of hydrothermal treatment (HT). The cubic Ia3 mesophase transforms to hexagonal p6mm after 8 days of HT at 100 °C. Surprisingly, the hexagonal phase is stable only for a limited period after which a reversal to the cubic Ia3 mesostructure is observed. Characterization methods such as powder X-ray diffraction (XRD), electron microscopy (SEM, TEM), N2-isotherms, magic-angle spinning (MAS) 29Si NMR spectroscopy, and thermogravimetric analysis (TGA) have been employed to follow structural and textural changes of the materials prepared. Data show that the resultant mesostructure and its textural properties are highly dependent on the period of HT with less unit-cell shrinkage on calcination after extensive HT. Furthermore, evidence of two different solid−solid phase mechanisms during HT is presented. The initial transition is consistent with a restructuring of the surfactant packing and a depletion of the organic moieties from the organo-silica wall as evident from 29Si NMR spectroscopy. The return to the bicontinuous cubic phase is driven by changes in charge matching at the organic−inorganic interface as a result of increases in the polymerization of the silica wall. The textural properties, and in particular the presence or absence of surface porosity, has been controlled through variations in hydrothermal treatment. These are associated with specific growth directions of cubic AMS-6 crystals. The synthetic method described allows us to easily prepare phase pure and intermediate mesostructured nanoparticles.

  • 24.
    Atluri, Rambabu
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Garcia-Bennett, Alfonso
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Hedin, Niklas
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Nonsurfactant Supramolecular Synthesis of Ordered Mesoporous Silica2009In: Journal of the American Chemical Society, ISSN 0002-7863, E-ISSN 1520-5126, Vol. 131, no 9, p. 3189-3191Article in journal (Refereed)
    Abstract [en]

    Hoogsteen-bonded tetrads and pentamers are formed by a large variety of organic molecules through H-donor and acceptor groups capable of inducing self-organization to form columnar and hexagonal mesophases. The biological importance of such macromolecular structures is exemplified by the assembly of guanosine-rich groups of telomere units and their implication in chromosomal replication. Folic acid is composed of a pterin group, chemically and structurally similar to guanine, conjugated to an l-glutamate moiety via a p-amino benzoic acid. Our aim has been to develop a delivery vehicle for folic acid and at the same time provide a novel synthetic route for ordered mesoporous materials without the use of amphiphilic surfactants. We present a new nonsurfactant route for the synthesis of highly ordered mesoporous materials, based on the supramolecular templating of stacked arrays of the tetramer-forming pterin groups of folic acid under a variety of synthetic conditions. This method leads to hexagonally ordered mesoporous structures with gyroid, spherical, and chiral morphologies with pores on the order of 25−30 Å in diameter and surface areas above 1000 m2/g. More importantly circular dichroism studies reveal that the folate template possesses a chiral signature within the pores in the as-synthesized solid and that chirality is transferred from the folate template to the pore surface via the aminopropyl triethoxysilane costructure directing agent used in the supramolecular assembly. This novel templating approach for ordered mesoporous materials breaks the hegemony of surfactant micellar systems for the preparation of these exciting high surface area solids and opens new opportunities for structural control, design of pore geometry, and novel applications.

  • 25.
    Atluri, Rambabu
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Garcia-Bennett, Alfonso.E
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Sakamoto, Yasuhiro
    Co-Structure Directing Agent Induced Phase Transformation of Mesoporous Materials2009In: Langmuir, ISSN 0743-7463, E-ISSN 1520-5827, Vol. 25, no 5, p. 3189-3195Article in journal (Refereed)
    Abstract [en]

    The synthesis of cubic Pmn mesocaged solid templated by cetyltrimethyl ammonium bromide (C16TMABr) surfactant by direct cocondensation of (3-aminopropyl)triethoxysilanes (APES) under strong alkaline conditions is reported. The novel route gives direct incorporation of amino functional groups on the porous silica wall, and the structural formation has been followed by means of in situ SAXS studies performed at a synchrotron beam line. Data shows that a molar ratio of C16TMABr/APES = 0.6 favors the formation of 3D cubic mesocaged solid with Pmn symmetry which transforms to a cylindrical mesoporous phase with p6mm symmetry at higher molar ratios. Further structural evaluation has been performed by means electron crystallography (EC). Reconstructed 3D models based on EC show the presence of spherical cages (A-cages, 45 Å) and ellipsoidal cages (B-cages, 48 × 43 Å) whereby every cage in the unit cell is connected to 14 nearest cages with a window size of 18 Å. Finally, a mechanism is proposed, denoted S+NoI, in which penetration of the neutral aminopropyl moiety within the micellar corona is responsible for the formation of the Pmn phase, accounting for the formation of the hexagonal phase at higher molar ratios and higher temperatures. In comparison to other mesocaged materials with the same symmetry this structure possesses a more open porous network which will help assess its potential in a variety of applications discussed herein.

  • 26. Atluri, Rambabu
    et al.
    Iqbal, Muhammad Naeem
    Bacsik, Zoltan
    Hedin, Niklas
    Villaescusa, Luis Angel
    Garcia-Bennett, Alfonso E
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Self-assembly mechanism of folate-templated mesoporous silica.2013In: Langmuir, ISSN 0743-7463, E-ISSN 1520-5827, Vol. 29, no 38, p. 12003-12Article in journal (Refereed)
    Abstract [en]

    A method to form ordered mesoporous silica based on the use of folate supramolecular templates has been developed. Evidence based on in situ small-angle X-ray scattering (SAXS), electron microscopy, infrared spectroscopy, and in situ conductivity measurements are used to investigate the organic-inorganic interactions and synthesis mechanism. The behavior of folate molecules in solution differs distinctively from that of surfactants commonly used for the preparation of ordered mesoporous silica phases, notably with the absence of a critical micellar concentration. In situ SAXS studies reveal fluctuations in X-ray scattering intensities consistent with the condensation of the silica precursor surrounding the folate template and the growth of the silica mesostructure in the initial stages. High-angle X-ray diffraction shows that the folate template is well-ordered within the pores even after a few minutes of synthesis. Direct structural data for the self-assembly of folates into chiral tetramers within the pores of mesoporous silica provide evidence for the in register stacking of folate tetramers, resulting in a chiral surface of rotated tetramers, with a rotation angle of 30°. Additionally, the self-assembled folates within pores were capable of adsorbing a considerable amount of CO2 gas through the cavity space of the tetramers. The study demonstrates the validity of using a naturally occurring template to produce relevant and functional mesoporous materials.

  • 27.
    Axelsson, Linda
    et al.
    Uppsala University, Disciplinary Domain of Medicine and Pharmacy, Faculty of Pharmacy, Department of Medicinal Chemistry, Organic Pharmaceutical Chemistry.
    Veron, Jean-Baptiste
    Uppsala University, Disciplinary Domain of Medicine and Pharmacy, Faculty of Pharmacy, Department of Medicinal Chemistry, Organic Pharmaceutical Chemistry.
    Sävmarker, Jonas
    Uppsala University, Disciplinary Domain of Medicine and Pharmacy, Faculty of Pharmacy, Department of Medicinal Chemistry, Organic Pharmaceutical Chemistry.
    Lindh, Jonas
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Odell, Luke
    Uppsala University, Disciplinary Domain of Medicine and Pharmacy, Faculty of Pharmacy, Department of Medicinal Chemistry, Organic Pharmaceutical Chemistry.
    Larhed, Mats
    Uppsala University, Disciplinary Domain of Medicine and Pharmacy, Faculty of Pharmacy, Department of Medicinal Chemistry, Organic Pharmaceutical Chemistry.
    An Improved Palladium(II)-Catalyzed Method for the Synthesis of Aryl Ketones from Aryl Carboxylic Acids and Organonitriles2014In: Tetrahedron Letters, ISSN 0040-4039, E-ISSN 1359-8562, Vol. 55, no 15, p. 2376-2380Article in journal (Refereed)
    Abstract [en]

    A palladium(II)-catalyzed decarboxylative protocol for the synthesis of aryl ketones has been developed. The addition of TFA was shown to improve the reaction yield and employing THF as solvent enabled the use of solid nitriles and in only a small excess. Using this method, five different benzoic acids reacted with a wide range of nitriles to produce 29 diverse (hetero)aryl ketone derivatives in up to 94% yield.

  • 28.
    Bacsik, Zoltan
    et al.
    Department of Materials and Environmental Chemistry , Berzelii Center EXSELENT on Porous Materials, Arrhenius Laboratory, Stockholm University.
    Ahlsten, Nanna
    Department of Organic Chemistry, Berzelii Center EXSELENT on Porous Materials, Arrhenius Laboratory, Stockholm University.
    Ziadi, Asraa
    Department of Organic Chemistry, Berzelii Center EXSELENT on Porous Materials, Arrhenius Laboratory, Stockholm University.
    Zhao, Guoying
    Department of Materials and Environmental Chemistry , Berzelii Center EXSELENT on Porous Materials, Arrhenius Laboratory, Stockholm University.
    Garcia-Bennett, Alfonso E.
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Martin-Matute, Belen
    Department of Organic Chemistry, Berzelii Center EXSELENT on Porous Materials, Arrhenius Laboratory, Stockholm University.
    Hedin, Niklas
    Department of Materials and Environmental Chemistry , Berzelii Center EXSELENT on Porous Materials, Arrhenius Laboratory, Stockholm University.
    Mechanisms and Kinetics for Sorption of CO(2) on Bicontinuous Mesoporous Silica Modified with n-Propylamine2011In: Langmuir, ISSN 0743-7463, E-ISSN 1520-5827, Vol. 27, no 17, p. 11118-11128Article in journal (Refereed)
    Abstract [en]

    We studied equilibrium adsorption and uptake kinetics and identified molecular species that formed during sorption of carbon dioxide on amine-modified silica. Bicontinuous silicas (AMS-6 and MCM-48) were postsynthetically modified with (3-aminopropyl)triethoxysilane or (3-aminopropyl)methyldiethoxysilane, and amine-modified AMS-6 adsorbed more CO(2) than did amine-modified MCM-48. By in situ FTIR spectroscopy, we showed that the amine groups reacted with CO(2) and formed ammonium carbamate ion pairs as well as carbamic acids under both dry and moist conditions. The carbamic acid was stabilized by hydrogen bonds, and ammonium carbamate ion pairs formed preferably on sorbents with high densities of amine groups. Under dry conditions, silylpropylcarbamate formed, slowly, by condensing carbamic acid and silanol groups. The ratio of ammonium carbamate ion pairs to silylpropylcarbamate was higher for samples with high amine contents than samples with low amine contents. Bicarbonates or carbonates did not form under dry or moist conditions. The uptake of CO(2) was enhanced in the presence of water, which was rationalized by the observed release of additional amine groups under these conditions and related formation of ammonium carbamate ion pairs. Distinct evidence for a fourth and irreversibly formed moiety was observed under sorption of CO(2) under dry conditions. Significant amounts of physisorbed, linear CO(2) were detected at relatively high partial pressures of CO(2), such that they could adsorb only after the reactive amine groups were consumed.

  • 29.
    Bacsik, Zoltán
    et al.
    Stockholm University.
    Atluri, Rambabu
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Garcia-Bennett, Alfonso E.
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Hedin, Niklas
    Stockholm University.
    Temperature-Induced Uptake of CO2 and Formation of Carbamates in Mesocaged Silica Modified with n-Propylamines2010In: Langmuir, ISSN 0743-7463, E-ISSN 1520-5827, Vol. 26, no 12, p. 10013-10024Article in journal (Refereed)
    Abstract [en]

    Adsorption-mediated CO2 separation can reduce the costs of carbon capture and storage. The reduction in cost requires adsorbents with high capacities for CO2 sorption and high CO2-over-N2 selectivity. Amine-modified sorbents are promising candidates for carbon capture. To investigate the details of CO2 adsorption in such materials, we studied mesocaged (cubic, Pm3n symmetry) silica adsorbents with tethered propylamines using Fourier transform infrared (FTIR) spectroscopy and volumetric uptake experiments. The degree of heterogeneity in these coatings was varied by either co-synthesizing or post-synthetically introducing the propylamine modification. In situ FTIR spectroscopy revealed the presence of both physisorbed and chemisorbed CO2 in the materials. We present the first direct molecular evidence for physisorption using FTIR spectroscopy in mesoporous silica sorbents modified with propylamines. Physisorption reduced the CO2-over-N2 selectivity in amine-rich sorbents. Samples with homogenous coatings showed typical CO2 adsorption trends and large quantities of IR-observable physisorbed CO2. The uptake of CO2 in mesocaged materials with heterogeneous propylamine coatings was higher at high temperatures than at low temperatures. At higher temperatures and low pressures, the post-synthetically modified materials adsorbed more CO2 than did the extracted ones, even though the surface area after modification was clearly reduced and the coverage of primary amine groups was lower. The principal mode of CO2 uptake in post-synthetically modified mesoporous silica was chemisorption. The chemisorbed moieties were present mainly as carbamate–ammonium ion pairs, resulting from the quantitative transformation of primary amine groups during CO2 adsorption as established by NIR spectroscopy. The heterogeneity in the coatings promoted the formation of these ion pairs. The average propylamine–propylamine distance must be small to allow the formation of carbamate–propylammonium ion pairs.

  • 30. - Banerjee, Amitava
    et al.
    - Araujo, Rafael B.
    Sjödin, Martin
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    - Ahuja, Rajeev
    Identifying the tuning key of disproportionation redox reaction in terephthalate: A Li-based anode for sustainable organic batteries2018In: Nano Energy, ISSN 2211-2855, E-ISSN 2211-3282, ISSN - 2211-2855, Vol. - 47Article in journal (Refereed)
    Abstract [en]

    - The ever-increasing consumption of energy storage devices has pushed the scientific community to realize strategies toward organic electrodes with superior properties. This is owed to advantages such as economic viability and eco-friendliness. In this context, the family of conjugated dicarboxylates has emerged as an interesting candidate for the application as negative electrodes in advanced Li-ion batteries due to the revealed thermal stability, rate capability, high capacity and high cyclability. This work aims to rationalize the effects of small molecular modifications on the electrochemical properties of the terephthalate anode by means of first principles calculations. The crystal structure prediction of the investigated host compounds dilithium terephthalate (Li2TP) and diethyl terephthalate (Et2Li0TP) together with their crystal modification upon battery cycling enable us to calculate the potential profile of these materials. Distinct underlying mechanisms of the redox reactions were obtained where Li2TP comes with a disproportionation reaction while Et2Li0TP displays sequential redox reactions. This effect proved to be strongly correlated to the Li coordination number evolution upon the Li insertion into the host structures. Finally, the calculations of sublimation enthalpy inferred that polymerization techniques could easily be employed in Et2Li0TP as compared to Li2TP. Similar results are observed with methyl, propyl, and vinyl capped groups. That could be a strategy to enhance the properties of this compound placing it into the gallery of the new anode materials for state of art Li-batteries.

  • 31.
    Banerjee, Amitava
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Theory.
    Araujo, Rafael Barros
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Theory.
    Sjödin, Martin
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Ahuja, Rajeev
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Theory. Royal Inst Technol KTH, Appl Mat Phys, Dept Mat, S-10044 Stockholm, Sweden;Royal Inst Technol KTH, Appl Mat Phys, Dept Engn, S-10044 Stockholm, Sweden.
    Identifying the tuning key of disproportionation redox reaction in terephthalate: A Li-based anode for sustainable organic batteries2018In: Nano Energy, ISSN 2211-2855, E-ISSN 2211-3282, Vol. 47, p. 301-308Article in journal (Refereed)
    Abstract [en]

    The ever-increasing consumption of energy storage devices has pushed the scientific community to realize strategies toward organic electrodes with superior properties. This is owed to advantages such as economic viability and eco-friendliness. In this context, the family of conjugated dicarboxylates has emerged as an interesting candidate for the application as negative electrodes in advanced Li-ion batteries due to the revealed thermal stability, rate capability, high capacity and high cyclability. This work aims to rationalize the effects of small molecular modifications on the electrochemical properties of the terephthalate anode by means of first principles calculations. The crystal structure prediction of the investigated host compounds dilithium terephthalate (Li2TP) and diethyl terephthalate (Et2Li0TP) together with their crystal modification upon battery cycling enable us to calculate the potential profile of these materials. Distinct underlying mechanisms of the redox reactions were obtained where Li2TP comes with a disproportionation reaction while Et2Li0TP displays sequential redox reactions. This effect proved to be strongly correlated to the Li coordination number evolution upon the Li insertion into the host structures. Finally, the calculations of sublimation enthalpy inferred that polymerization techniques could easily be employed in Et2Li0TP as compared to Li2TP. Similar results are observed with methyl, propyl, and vinyl capped groups. That could be a strategy to enhance the properties of this compound placing it into the gallery of the new anode materials for state of art Li-batteries.

  • 32.
    Basu, Alex
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Ion-Crosslinked Nanocellulose Hydrogels for Advanced Wound Care Applications2018Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    A current trend in the field of wound care is the development of wound healing materials that are designed to address specific types of wounds or underlying pathologies to achieve improved healing. At the same time, there is a societal drive to replace synthetic materials with renewable alternatives. The work presented in this thesis was therefore carried out to investigate the use of wood nanocellulose, produced from the world’s most abundant biopolymer, cellulose, in advanced wound care applications.

    Wood-based nanofibrillated cellulose (NFC) was chemically functionalized and crosslinked using calcium to obtain a self-standing hydrogel. The NFC hydrogel was evaluated in terms of its physicochemical properties, biocompatibility, blood interactions, bacterial interactions, in vivo wound healing ability and, finally, as a protein carrier. Parallel with the assessment of the NFC hydrogel, modified versions of the material were tested to investigate the tunability of the above-mentioned characteristics.

    The ability of the hydrogel to maintain a moist wound bed was demonstrated. Evaluation of the biocompatibility showed that the material was cytocompatible and did not trigger inflammatory mechanisms. Furthermore, the NFC hydrogel supported cell proliferation, and was shown to possess hemostatic properties. It was also discovered that the material had a slight bacteriostatic effect and the ability to act as a barrier against bacteria. When tested in vivo, the hydrogel was found to significantly improve wound healing.

    Modifications through the incorporation of additives to the hydrogel matrix, as well as exchange of the crosslinking ion, were shown to influence the biological response to the material. Moreover, the results presented here demonstrate the possibility of using the NFC hydrogel as a protein carrier; the easily adjustable charge property being identified as a central parameter for manipulation to regulate the release profile.

    In conclusion, this work has demonstrated the extensive wound healing ability of the calcium-crosslinked NFC hydrogel, and represents an important milestone in the research on NFC towards advanced wound care applications. It is expected that the easily modifiable nature of the material can be exploited to further develop the NFC hydrogel to suit the treatment needs for a broad range of wound types.

    List of papers
    1. On the use of ion-crosslinked nanocellulose hydrogels for wound healing solutions: Physicochemical properties and application-oriented biocompatibility studies
    Open this publication in new window or tab >>On the use of ion-crosslinked nanocellulose hydrogels for wound healing solutions: Physicochemical properties and application-oriented biocompatibility studies
    Show others...
    2017 (English)In: Carbohydrate Polymers, ISSN 0144-8617, E-ISSN 1879-1344, Vol. 174, p. 299-308Article in journal (Refereed) Published
    Abstract [en]

    Calcium ion-crosslinked nanofibrillated cellulose (NFC) hydrogels were investigated as potential materials for wound healing dressings. The physicochemical properties of the hydrogels were examined by rheology and water retention tests. Skin cells and monocytes were selected for application-oriented bio-compatibility studies. The NFC hydrogels presented entangled fibrous networks and solid-like behavior. Water retention tests showed the material's potential to maintain a suitable moist environment for different type of wounds. The hydrogels did not affect dermal fibroblasts monolayer cultures upon directcontact, as cell monolayers remained intact after application, incubation and removal of the materials. Inflammatory response studies with blood-derived mononuclear cells revealed the inert nature of the hydrogels in terms of cytokine secretion and reactive oxygen species production. Results highlight the great potential of ion-crosslinked NFC hydrogels for the development of advanced wound dressings, where further functionalization of the material could lead to improved properties towards the healing of specific wound types.

    Keywords
    Nanofibrillated cellulose, Inflammation, Fibroblasts, Mononuclear cells
    National Category
    Nano Technology
    Research subject
    Engineering Science with specialization in Nanotechnology and Functional Materials
    Identifiers
    urn:nbn:se:uu:diva-332126 (URN)10.1016/j.carbpol.2017.06.073 (DOI)000407696800032 ()28821071 (PubMedID)
    Funder
    Swedish Research Council Formas
    Available from: 2017-10-24 Created: 2017-10-24 Last updated: 2018-10-12Bibliographically approved
    2. Hemocompatibility of Ca2+-Crosslinked Nanocellulose Hydrogels: Toward Efficient Management of Hemostasis
    Open this publication in new window or tab >>Hemocompatibility of Ca2+-Crosslinked Nanocellulose Hydrogels: Toward Efficient Management of Hemostasis
    2017 (English)In: Macromolecular Bioscience, ISSN 1616-5187, E-ISSN 1616-5195, Vol. 17, no 11, article id 1700236Article in journal (Refereed) Published
    Abstract [en]

    The present work investigates Ca2+-crosslinked nanofibrillated cellulose hydrogels as potential hemostatic wound dressings by studying core interactions between the materials and a central component of wounds and wound healing—the blood. Hydrogels of wood-derived anionic nanofibrillated cellulose (NFC) and NFC hydrogels that incorporate kaolin or collagen are studied in an in vitro whole blood model and with platelet-free plasma assays. The evaluation of thrombin and factor XIIa formation, platelet reduction, and the release of activated complement system proteins, shows that the NFC hydrogel efficiently triggered blood coagulation, with a rapid onset of clot formation, while displaying basal complement system activation. By using the NFC hydrogel as a carrier of kaolin, the onset of hemostasis is further boosted, while the NFC hydrogel containing collagen exhibits blood activating properties comparable to the anionic NFC hydrogel. The herein studied NFC hydrogels demonstrate great potential for being part of advanced wound healing dressings that can be tuned to target certain wounds (e.g., strongly hemorrhaging ones) or specific phases of the wound healing process for optimal wound management.

    Keywords
    biocompatibility, blood coagulation, complement system, nanofibrillated cellulose, wound dressing
    National Category
    Nano Technology
    Research subject
    Engineering Science with specialization in Nanotechnology and Functional Materials
    Identifiers
    urn:nbn:se:uu:diva-332127 (URN)10.1002/mabi.201700236 (DOI)000415130800015 ()28941135 (PubMedID)
    Funder
    Swedish Research Council Formas
    Available from: 2017-10-24 Created: 2017-10-24 Last updated: 2018-10-12Bibliographically approved
    3. Ion-crosslinked wood-derived nanocellulose hydrogels with tunable antibacterial properties: Candidate materials for advanced wound care applications
    Open this publication in new window or tab >>Ion-crosslinked wood-derived nanocellulose hydrogels with tunable antibacterial properties: Candidate materials for advanced wound care applications
    Show others...
    2018 (English)In: Carbohydrate Polymers, ISSN 0144-8617, E-ISSN 1879-1344, Vol. 181, p. 345-350Article in journal (Refereed) Published
    Abstract [en]

    Development of advanced dressings with antimicrobial properties for the treatment of infected wounds is an important approach in the fight against evolution of antibiotic resistant bacterial strains. Herein, the effects of ion-crosslinked nanocellulose hydrogels on bacteria commonly found in infected wounds were investigated in vitro. By using divalent calcium or copper ions as crosslinking agents, different antibacterial properties against the bacterial strains Staphylococcus epidermidis and Pseudomonas aeruginosa were obtained. Calcium crosslinked hydrogels were found to retard S. epidermidis growth (up to 266% increase in lag time, 36% increase in doubling time) and inhibited P. aeruginosa biofilm formation, while copper crosslinked hydrogels prevented S. epidermidis growth and were bacteriostatic towards P. aeruginosa (49% increase in lag time, 78% increase in doubling time). The wound dressing candidates furthermore displayed barrier properties towards both S. epidermidis and P. aeruginosa, hence making them interesting for further development of advanced wound dressings with tunable antibacterial properties.

    Keywords
    Nanofibrillated cellulose, Biofilm, Wound dressing, Infected wound
    National Category
    Nano Technology
    Research subject
    Engineering Science with specialization in Nanotechnology and Functional Materials
    Identifiers
    urn:nbn:se:uu:diva-333382 (URN)10.1016/j.carbpol.2017.10.085 (DOI)000418661000041 ()29253982 (PubMedID)
    Funder
    Swedish Research Council Formas
    Available from: 2017-11-13 Created: 2017-11-13 Last updated: 2018-10-12Bibliographically approved
    4. In vitro and in vivo evaluation of the wound healing properties of nanofibrillated cellulose hydrogels
    Open this publication in new window or tab >>In vitro and in vivo evaluation of the wound healing properties of nanofibrillated cellulose hydrogels
    (English)In: Article in journal (Refereed) Submitted
    National Category
    Nano Technology
    Research subject
    Engineering Science with specialization in Nanotechnology and Functional Materials
    Identifiers
    urn:nbn:se:uu:diva-362724 (URN)
    Available from: 2018-10-09 Created: 2018-10-09 Last updated: 2018-10-12
    5. Towards Tunable Protein-Carrier Wound Dressings Based on Nanocellulose Hydrogels Crosslinked with Calcium Ions
    Open this publication in new window or tab >>Towards Tunable Protein-Carrier Wound Dressings Based on Nanocellulose Hydrogels Crosslinked with Calcium Ions
    2018 (English)In: Nanomaterials, E-ISSN 2079-4991, Vol. 8, no 7, article id 550Article in journal (Refereed) Published
    Abstract [en]

    A Ca2+-crosslinked wood-based nanofibrillated cellulose (NFC) hydrogel was investigated to build knowledge toward the use of nanocellulose for topical drug delivery applications in a chronic wound healing context. Proteins of varying size and isoelectric point were loaded into the hydrogel in a simple soaking procedure. The release of the proteins from the hydrogel was monitored and kinetics determining parameters of the release processes were assessed. The integrity of the hydrogel and proteins were also studied. The results showed that electrostatic interactions between the proteins and the negatively-charged NFC hydrogel structure played a central role in the loading process. The release of the proteins were governed by Fickian diffusion. An increased protein size, as well as a positive protein charge facilitated a slower and more sustained release process from the hydrogel matrix. At the same time, the positively-charged protein was shown to increase the post-loading hydrogel strength. Released proteins maintained structural stability and activity, thus indicating that the Ca2+-crosslinked NFC hydrogel could function as a carrier of therapeutic proteins without compromising protein function. It is foreseen that, by utilizing tunable charge properties of the NFC hydrogel, release profiles can be tailored to meet very specific treatment needs.

    Place, publisher, year, edition, pages
    MDPI, 2018
    Keywords
    nanofibrillated cellulose, ion-crosslinked, drug delivery, wound healing, chronic wounds
    National Category
    Nano Technology
    Research subject
    Engineering Science with specialization in Nanotechnology and Functional Materials
    Identifiers
    urn:nbn:se:uu:diva-362722 (URN)10.3390/nano8070550 (DOI)000442523100101 ()30036970 (PubMedID)
    Funder
    Swedish Research Council Formas, 942-2015-475
    Available from: 2018-10-09 Created: 2018-10-09 Last updated: 2018-10-30Bibliographically approved
  • 33.
    Basu, Alex
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Celma, Gunta
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Strömme, Maria
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Ferraz, Natalia
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    In vitro and in vivo evaluation of the wound healing properties of nanofibrillated cellulose hydrogelsIn: Article in journal (Refereed)
  • 34.
    Basu, Alex
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Ferraz, Natalia
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Ion-crosslinked nanocellulose hydrogels for biomedical applications2015Conference paper (Refereed)
  • 35.
    Basu, Alex
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Ferraz, Natalia
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Nanocellulose hydrogels as candidates for advanced wound healing solutions2018Conference paper (Refereed)
  • 36.
    Basu, Alex
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Ferraz, Natalia
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Nanocellulose hydrogels for topical wound care applications2016Conference paper (Other academic)
  • 37.
    Basu, Alex
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Ferraz, Natalia
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Nanocellulose hydrogels for wound-healing applications2016Conference paper (Refereed)
  • 38.
    Basu, Alex
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Ferraz, Natalia
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Nanocellulose hydrogels: preparation, characterization and cytotoxicity studies toward biomedical applications2016Conference paper (Refereed)
  • 39.
    Basu, Alex
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Ferraz, Natalia
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Nanofibrillated cellulose hydrogels for wound healing solutions: the status quo and future prospects2015In: Uppsala Biomaterials Conference 2015, 2015Conference paper (Refereed)
  • 40.
    Basu, Alex
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Heitz, Karen
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Strömme, Maria
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Welch, Ken
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Ferraz, Natalia
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Ion-crosslinked wood-derived nanocellulose hydrogels with tunable antibacterial properties: Candidate materials for advanced wound care applications2018In: Carbohydrate Polymers, ISSN 0144-8617, E-ISSN 1879-1344, Vol. 181, p. 345-350Article in journal (Refereed)
    Abstract [en]

    Development of advanced dressings with antimicrobial properties for the treatment of infected wounds is an important approach in the fight against evolution of antibiotic resistant bacterial strains. Herein, the effects of ion-crosslinked nanocellulose hydrogels on bacteria commonly found in infected wounds were investigated in vitro. By using divalent calcium or copper ions as crosslinking agents, different antibacterial properties against the bacterial strains Staphylococcus epidermidis and Pseudomonas aeruginosa were obtained. Calcium crosslinked hydrogels were found to retard S. epidermidis growth (up to 266% increase in lag time, 36% increase in doubling time) and inhibited P. aeruginosa biofilm formation, while copper crosslinked hydrogels prevented S. epidermidis growth and were bacteriostatic towards P. aeruginosa (49% increase in lag time, 78% increase in doubling time). The wound dressing candidates furthermore displayed barrier properties towards both S. epidermidis and P. aeruginosa, hence making them interesting for further development of advanced wound dressings with tunable antibacterial properties.

  • 41.
    Basu, Alex
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Hong, Jaan
    Uppsala University, Disciplinary Domain of Medicine and Pharmacy, Faculty of Medicine, Department of Immunology, Genetics and Pathology, Clinical Immunology.
    Ferraz, Natalia
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Hemocompatibility of Ca2+-Crosslinked Nanocellulose Hydrogels: Toward Efficient Management of Hemostasis2017In: Macromolecular Bioscience, ISSN 1616-5187, E-ISSN 1616-5195, Vol. 17, no 11, article id 1700236Article in journal (Refereed)
    Abstract [en]

    The present work investigates Ca2+-crosslinked nanofibrillated cellulose hydrogels as potential hemostatic wound dressings by studying core interactions between the materials and a central component of wounds and wound healing—the blood. Hydrogels of wood-derived anionic nanofibrillated cellulose (NFC) and NFC hydrogels that incorporate kaolin or collagen are studied in an in vitro whole blood model and with platelet-free plasma assays. The evaluation of thrombin and factor XIIa formation, platelet reduction, and the release of activated complement system proteins, shows that the NFC hydrogel efficiently triggered blood coagulation, with a rapid onset of clot formation, while displaying basal complement system activation. By using the NFC hydrogel as a carrier of kaolin, the onset of hemostasis is further boosted, while the NFC hydrogel containing collagen exhibits blood activating properties comparable to the anionic NFC hydrogel. The herein studied NFC hydrogels demonstrate great potential for being part of advanced wound healing dressings that can be tuned to target certain wounds (e.g., strongly hemorrhaging ones) or specific phases of the wound healing process for optimal wound management.

  • 42.
    Basu, Alex
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Lindh, Jonas
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Ålander, Eva
    Rise Bioeconomy.
    Strömme, Maria
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Ferraz, Natalia
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    On the use of ion-crosslinked nanocellulose hydrogels for wound healing solutions: Physicochemical properties and application-oriented biocompatibility studies2017In: Carbohydrate Polymers, ISSN 0144-8617, E-ISSN 1879-1344, Vol. 174, p. 299-308Article in journal (Refereed)
    Abstract [en]

    Calcium ion-crosslinked nanofibrillated cellulose (NFC) hydrogels were investigated as potential materials for wound healing dressings. The physicochemical properties of the hydrogels were examined by rheology and water retention tests. Skin cells and monocytes were selected for application-oriented bio-compatibility studies. The NFC hydrogels presented entangled fibrous networks and solid-like behavior. Water retention tests showed the material's potential to maintain a suitable moist environment for different type of wounds. The hydrogels did not affect dermal fibroblasts monolayer cultures upon directcontact, as cell monolayers remained intact after application, incubation and removal of the materials. Inflammatory response studies with blood-derived mononuclear cells revealed the inert nature of the hydrogels in terms of cytokine secretion and reactive oxygen species production. Results highlight the great potential of ion-crosslinked NFC hydrogels for the development of advanced wound dressings, where further functionalization of the material could lead to improved properties towards the healing of specific wound types.

  • 43.
    Basu, Alex
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Strömme, Maria
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Ferraz, Natalia
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Towards Tunable Protein-Carrier Wound Dressings Based on Nanocellulose Hydrogels Crosslinked with Calcium Ions2018In: Nanomaterials, E-ISSN 2079-4991, Vol. 8, no 7, article id 550Article in journal (Refereed)
    Abstract [en]

    A Ca2+-crosslinked wood-based nanofibrillated cellulose (NFC) hydrogel was investigated to build knowledge toward the use of nanocellulose for topical drug delivery applications in a chronic wound healing context. Proteins of varying size and isoelectric point were loaded into the hydrogel in a simple soaking procedure. The release of the proteins from the hydrogel was monitored and kinetics determining parameters of the release processes were assessed. The integrity of the hydrogel and proteins were also studied. The results showed that electrostatic interactions between the proteins and the negatively-charged NFC hydrogel structure played a central role in the loading process. The release of the proteins were governed by Fickian diffusion. An increased protein size, as well as a positive protein charge facilitated a slower and more sustained release process from the hydrogel matrix. At the same time, the positively-charged protein was shown to increase the post-loading hydrogel strength. Released proteins maintained structural stability and activity, thus indicating that the Ca2+-crosslinked NFC hydrogel could function as a carrier of therapeutic proteins without compromising protein function. It is foreseen that, by utilizing tunable charge properties of the NFC hydrogel, release profiles can be tailored to meet very specific treatment needs.

  • 44.
    Basu, Alex
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Tummala, Gopi
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Heitz, Karen
    Gustafsson, Simon
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Strietzel, Christian
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Yang, Jiaojiao
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Notfors, Celina
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Wang, Huan
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Strömme, Maria
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Miljövänliga nanomaterial från växtriket tillåter gröna alternative för framtiden2017In: SciFest 2017 / [ed] Uppsala Universitet, 2017Conference paper (Other academic)
  • 45. Bayat, N
    et al.
    Lopes, Viviana
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Lakshmanan, R
    Rajarao, GK
    Cristobal, S
    Assessment of functionalized iron oxide nanoparticles in vitro: Introduction to integrated nanoimpact index2015In: Environmental Science: Nano, Vol. 2, p. 380-394Article in journal (Refereed)
    Abstract [en]

    Functionalization of super paramagnetic iron oxide NPs (SPIONs) with different coatings renders them with unique physicochemical properties that allow them to be used in a broad range of applications such as drug targeting and water purification. However, it is required to fill the gap between the promises of any new functionalized SPIONs and the effects of these coatings on the NPs safety. Nanotoxicology is offering diverse strategies to assess the effect of exposure to SPIONs in a case-by-case manner but an integrated nanoimpact scale has not been developed yet. We have implemented the classical integrated biological response (IBR) into an integrated nanoimpact index (INI) as an early warning scale of nano-impact based on a combination of toxicological end points such as cell proliferation, oxidative stress, apoptosis and genotoxicity. Here, the effect of SPIONs functionalized with tri-sodium citrate (TSC), polyethylenimine (PEI), aminopropyl-triethoxysilane (APTES) and Chitosan (chitosan) were assessed on human keratinocytes and endothelial cells. Our results show that endothelial cells were more sensitive to exposure than keratinocytes and the initial cell culture density modulated the toxicity. PEI-SPIONs had the strongest effects in both cell types while TSC-SPIONS were the most biocompatible. This study emphasizes not only the importance of surface coatings but also the cell type and the initial cell density on the selection of toxicity assays. The INI developed here could offer an initial rationale to choose either modifying SPIONs properties to reduce its nanoimpact or performing a complete risk assessment to define the risk boundaries.

  • 46. Bayat, N
    et al.
    Lopes, Viviana
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Jensen, LD
    Cristobal, S
    Vascular toxicity of ultra-small TiO2 nanoparticles and single walled carbon nanotubes in vitro and in vivo2015In: Biomaterials, ISSN 0142-9612, E-ISSN 1878-5905, Vol. 63, p. 1-13Article in journal (Refereed)
    Abstract [en]

    Ultra-small nanoparticles (USNPs) at 1-3 nm are a subset of nanoparticles (NPs) that exhibit intermediate physicochemical properties between molecular dispersions and larger NPs. Despite interest in their utilization in applications such as theranostics, limited data about their toxicity exist. Here the effect of TiO2-USNPs on endothelial cells in vitro, and zebrafish embryos in vivo, was studied and compared to larger TiO2-NPs (30 nm) and to single walled carbon nanotubes (SWCNTs). In vitro exposure showed that TiO2-USNPs were neither cytotoxic, nor had oxidative ability, nevertheless were genotoxic. In vivo experiment in early developing zebrafish embryos in water at high concentrations of TiO2-USNPs caused mortality possibly by acidifying the water and caused malformations in the form of pericardial edema when injected. Myo1C involved in glomerular development of zebrafish embryos was upregulated in embryos exposed to TiO2-USNPs. They also exhibited anti-angiogenic effects both in vitro and in vivo plus decreased nitric oxide concentration. The larger TiO2-NPs were genotoxic but not cytotoxic. SWCNTs were cytotoxic in vitro and had the highest oxidative ability. Neither of these NPs had significant effects in vivo. To our knowledge this is the first study evaluating the effects of TiO2-USNPs on vascular toxicity in vitro and in vivo and this strategy could unravel USNPs potential applications.

  • 47.
    Bejhed, Rebecca
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Physics.
    Svedlindh, Peter
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Physics.
    Gunnarsson, Klas
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Physics.
    Strömme, Maria
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Planar coils for immobilization of magnetic nanobeads2009In: 9, Karlsruhe, 2009, p. 12-19Conference paper (Refereed)
  • 48.
    Bejhed Stjernberg, Rebecca
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Physics.
    Gunnarsson, Klas
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Physics.
    Strömme, Maria
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Svedlindh, Peter
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Physics.
    A planar coil for immobilization of magnetic nanobeads, fabricationand verification2009Conference paper (Refereed)
  • 49.
    Bejhed Stjernberg, Rebecca
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Physics.
    Strömme, Maria
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Svedlindh, Peter
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Physics.
    Ahlford, Annika
    Stockholm Univ, Dept Biochem & Biophys, Sci Life Lab, Solna, Sweden..
    Strömberg, Mattias
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Solid State Physics.
    Magnetic nanobeads present during enzymatic amplification and labeling for a simplified DNA detection protocol based on AC susceptometry2015In: AIP Advances, ISSN 2158-3226, E-ISSN 2158-3226, Vol. 5, no 12, article id 127139Article in journal (Refereed)
    Abstract [en]

    Magnetic biosensors are promising candidates for low-cost point-of-care biodiagnostic devices. For optimal efficiency it is crucial to minimize the time and complexity of the assay protocol including target recognition, amplification, labeling and read-out. In this work, possibilities for protocol simplifications for a DNA biodetection principle relying on hybridization of magnetic nanobeads to rolling circle amplification (RCA) products are investigated. The target DNA is recognized through a padlock ligation assay resulting in DNA circles serving as templates for the RCA process. It is found that beads can be present during amplification without noticeably interfering with the enzyme used for RCA (phi29 polymerase). As a result, the bead-coil hybridization can be performed immediately after amplification in a one-step manner at elevated temperature within a few minutes prior to read-out in an AC susceptometer setup, i.e. a combined protocol approach. Moreover, by recording the phase angle xi = arctan(chi ''/chi'), where chi and chi '' are the in-phase and out-of-phase components of the AC susceptibility, respectively, at one single frequency the total assay time for the optimized combined protocol would be no more than 1.5 hours, often a relevant time frame for diagnosis of cancer and infectious disease. Also, applying the phase angle method normalization of AC susceptibility data is not needed. These findings are useful for the development of point-of-care biodiagnostic devices relying on bead-coil binding and magnetic AC susceptometry.

  • 50.
    Bjärnhall Prytz, Nicklas
    Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
    Interactions of cellulose and aromatic organic molecules modelled with density functional theory: A computational study2015Independent thesis Basic level (degree of Bachelor), 10 credits / 15 HE creditsStudent thesis
    Abstract [en]

    In this study, the interaction energies between aromatic organic molecules (AOMs) and cellulose are explored using density functional theory (DFT) through the software SIESTA and the exchange-correlational functional VDW-DRSLL. Three AOMs will be modelled: benzene, benzamide and benzoic acid. Firstly, the interaction energies of the dimers of the AOMs are determined. Then, the obtained interaction energies of the cellulose-AOM complexes are compared to the former in order to decide which interaction is stronger. It is found that the studied AOMs are more likely to interact with cellulose than with another identical monomer; benzamide has the highest propensity to interact, followed by benzoic acid and benzene. Furthermore, for all interaction energy calculations a counterpoise correction term will be introduced as an addition to the SIESTA optimisation and it will be shown that without this correction the acquired energy minima will deviate significantly from accepted values from previous studies.

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