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Harnessing Mesoporous Spheres - transport studies and biotechnological applications
Stockholm University, Faculty of Science, Department of Physical, Inorganic and Structural Chemistry. (Materials Chemistry Research Group)
2009 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Applications in controlled release and delivery calls for a good understanding of molecular transport within the carrier material and the dominating release mechanisms. It is clear that a better understanding of hindered transport and diffusion of guest molecules is important when developing new porous materials, e.g., surfactant templated silica spheres, for biotechnological applications. Confocal laser scanning microscopy was used to quantify the bulk release and intraparticle transport of small charged fluorescent dyes, and fluorescently-tagged neutral dextran, from mesoporous silica spheres. The time dependent release and the concentration profiles within the spheres have been used to analyze the release mechanisms using appropriate models. While the small, non-adsorbing anionic dye is released following a simple diffusion driven process, the concentration of the cationic dye varies radially within the spheres after loading. The release of the cationic dye is controlled by diffusion after an initial period of rapid release, which could be due to a significant fraction of the cationic dye that remains permanently attached to the negatively charged walls of the mesoporous silica spheres. The diffusion of dextran and the resulting flat concentration profiles could be related to the complex structural feature of the cylindrical pores close to the surface, and a possible conformational change of the dextran with the concentration. The stability and leaching of a catalytic enzyme, lipase, immobilized in hydrophobilized mesoporous support has also been quantified. Colloidal monodisperse mesoporous silica spheres were synthesized and transmission electron microscopy showed that the inner pore structure display a radially extending pores. The mesoporous spheres were used as solid supports for a lipid membrane incorporated with a multi-subunit redox-driven proton pump, which was shown to remain functional.

Place, publisher, year, edition, pages
Stockholm: Department of Physical, Inorganic and Structural Chemistry, Stockholm University , 2009. , 69 p.
Keyword [en]
Mesoporous, spheres, particles, CLSM, TEM, controlled-release, molecular transport, lipid membrane, enzyme, intraparticle, lipase, solid support
National Category
Inorganic Chemistry
Research subject
Materials Science
Identifiers
URN: urn:nbn:se:su:diva-27797ISBN: 978-91-7155-898-5 (print)OAI: oai:DiVA.org:su-27797DiVA: diva2:218328
Public defence
2009-09-02, Nordenskiöldsalen, Geovetenskapens hus, Svante Arrhenius väg 8 C, Stockholm, 10:00 (English)
Opponent
Supervisors
Projects
Synthesis, functionalisation and controlled release of mesoporous materials
Available from: 2009-05-27 Created: 2009-05-19 Last updated: 2009-05-20Bibliographically approved
List of papers
1. Release and molecular transport of cationic and anionic fluorescent molecules in mesoporous silica spheres
Open this publication in new window or tab >>Release and molecular transport of cationic and anionic fluorescent molecules in mesoporous silica spheres
2008 (English)In: Langmuir, ISSN 0743-7463, E-ISSN 1520-5827, Vol. 24, no 19, 11096-11102 p.Article in journal (Refereed) Published
Abstract [en]

We describe here a method for study of bulk release and local molecular transport within mesoporous silica spheres. We have analyzed the loading and release of charged fluorescent dyes from monodisperse mesoporous silica (MMS) spheres with an average pore size of 2.7 nm. Two different fluorescent dyes, one cationic and one anionic, have been loaded into the negatively charged porous material and both the bulk release and the local molecular transport within the MMS spheres have been quantified by confocal laser scanning microscopy. Analysis of the time-dependent release and the concentration profiles of the anionic dye within the spheres show that the spheres are homogeneous and that the release of this nonadsorbing dye follows a simple diffusion-driven process. The concentration of the cationic dye varies radially within the MMS spheres after loading; there is a significantly higher concentration of the dye close to the surface of the spheres (forming a “skin”) compared to that at the core. The release of the cationic dye is controlled by diffusion after an initial period of rapid release. The transport of the cationic dye within the MMS spheres of the dye from the core to near the surface is significantly faster compared to the transport within the surface “skin”. A significant fraction of the cationic dye remains permanently attached to the negatively charged walls of the MMS spheres, preferentially near the surface of the spheres. Relating bulk release to the local molecular transport within the porous materials provides an important step toward the design of new concepts in controlled drug delivery and chromatography.

Identifiers
urn:nbn:se:su:diva-15440 (URN)10.1021/la801179v (DOI)000259673500084 ()
Available from: 2008-12-02 Created: 2008-12-02 Last updated: 2017-12-13Bibliographically approved
2. Intraparticle Transport and Release of Dextran in Silica Spheres with Cylindrical Mesopores
Open this publication in new window or tab >>Intraparticle Transport and Release of Dextran in Silica Spheres with Cylindrical Mesopores
Show others...
2010 (English)In: Langmuir, ISSN 0743-7463, E-ISSN 1520-5827, Vol. 6, no 1, 466-470 p.Article in journal (Refereed) Published
Abstract [en]

The transport of oligomeric molecules in silica spheres with cylindrical mesopores has been quantified and related to the features of the internal structures in the spherical particles and the interactions at the polymer-pore interface. An emulsion-solvent-evaporation method was used to produce silica spheres having cylindrical mesopores with an average pore diameter of 6.5 nm. The transport of dextran molecules (fluorescently tagged) with molecular weights of 3000 and 10000 g/mol were quantified using confocal laser scanning microscopy (CLSM). The intraparticle concentrations profiles in the dextran-containing spheres were flat at all times, suggesting that the underpinning diffusion is not fully isotropic and the release is controlled by the pores close to the external surface of the spheres. The release of dextran into the solution is characterized by an initial burst, followed by a long-term sustained release. This behaviour cannot be described by a spherical model with a single diffusion constant (or a surface-induced mass transfer resistance). The release follows a logarithmic time-dependency that can be described by a Temkin model.

Keyword
Mesoporous particles, controlled release, dextran, CLSM, molecular transport
National Category
Inorganic Chemistry
Research subject
Materials Science
Identifiers
urn:nbn:se:su:diva-27800 (URN)10.1021/la902092e (DOI)
Projects
Synthesis, functionalisation and controlled release of mesoporous materials
Available from: 2009-05-19 Created: 2009-05-19 Last updated: 2017-12-13Bibliographically approved
3. Improved enzymatic activity of Thermomyces lanuginosus lipase immobilized in a hydrophobic particulate
Open this publication in new window or tab >>Improved enzymatic activity of Thermomyces lanuginosus lipase immobilized in a hydrophobic particulate
2010 (English)In: Journal of Colloid and Interface Science, ISSN 0021-9797, E-ISSN 1095-7103, Vol. 343, no 1, 359-365 p.Article in journal (Refereed) Published
Abstract [en]

Lipase from Thermomyces lanuginosus has been immobilized within particulate mesoporous silica carriers, with either hydrophilic or hydrophobic supporting surfaces, produced by the newly developed emulsion and solvent evaporation (ESE) method.  The Michaelis-Menten model was used to calculate the parameters related to the enzymatic activity of lipase i.e. the turnover number, kcat, and the specific activity. The specific activity was improved by immobilization of lipase onto the hydrophobic support, compared to lipase immobilized onto the hydrophilic support and lipase free in solution. The enhanced enzymatic activity of lipase onto a hydrophobic support was attributed to interfacial activation of the Thermomyces lanuginosus lipase when it is attached to a hydrophobic surface and a reduced denaturation. Confocal scanning laser microscopy (CLSM) studies, of fluorescently tagged lipase, showed that leakage of the lipase from the mesoporous particles was limited to an initial period of only a few hours. Both the rate and the amount of lipase leached were reduced when the lipase was immobilized onto the hydrophobic support.

Place, publisher, year, edition, pages
Elsevier Inc., 2010
Keyword
Enzyme, lipase, mesoporous, silica, immobilization, hydrophobic, spheres, particles
National Category
Inorganic Chemistry Industrial Biotechnology Chemical Process Engineering Other Materials Engineering
Research subject
Inorganic Chemistry
Identifiers
urn:nbn:se:su:diva-27826 (URN)10.1016/j.jcis.2009.11.014 (DOI)
Projects
Synthesis, functionalisation and controlled release of mesoporous materials
Available from: 2009-05-20 Created: 2009-05-20 Last updated: 2017-12-13Bibliographically approved
4. The radial dependence of the spatial mesostructure of monodisperse mesoporous silica spheres
Open this publication in new window or tab >>The radial dependence of the spatial mesostructure of monodisperse mesoporous silica spheres
2008 (English)In: Microporous and Mesoporous Materials, ISSN 1387-1811, E-ISSN 1873-3093, Vol. 112, 589-596 p.Article in journal (Refereed) Published
Abstract [en]

The pore structure of monodisperse mesostructured silica spheres has been investigated by a combination of X-ray diffraction, nitrogen sorption isotherms and transmission electron microscopy (TEM). The radial dependence of the mesostructure has been obtained by TEM analysis of thin microtomed slices taken at different distance from the particle core. A structural model is proposed based on the TEM observations where bundles of the hexagonally ordered cylindrical channels bend and twist, without any preferred direction, close to the particle core and attain a radially extended structure closer to the particle surface. Thermal calcination results in a pore shrinkage of about 16% and some loss of the long-range mesostructure while radiative disintegration and partial removal of the organic template by an UV/Ozone treatment had a negligible effect on the inorganic framework in terms of pore size or spatial pore arrangement.

Keyword
Mesoporous particles, Monodisperse, TEM, Stoeber method, Colloid
Identifiers
urn:nbn:se:su:diva-15273 (URN)10.1016/j.micromeso.2007.10.041 (DOI)000256713300066 ()
Available from: 2008-11-26 Created: 2008-11-26 Last updated: 2017-12-13Bibliographically approved
5. A Membrane-reconstituted Multisubunit Functional Proton Pump on Mesoporous Silica Particles
Open this publication in new window or tab >>A Membrane-reconstituted Multisubunit Functional Proton Pump on Mesoporous Silica Particles
2009 (English)In: ACS Nano, ISSN 1936-0851, E-ISSN 1936-086X, Vol. 3, no 9, 2639-2646 p.Article in journal (Refereed) Published
Abstract [en]

We have investigated formation of a proteolipid membrane surrounding mesoporous silica particles with a diameter of 550 nm and pore sizes of 3.0 nm. A multisubunit redox-driven proton pump, cytochrome c oxidase, was incorporated into the membrane and we show that the enzyme is fully functional, both with respect to catalysis of O2 reduction to water, and charge separation across the membrane. The orientation of cytochrome c oxidase in the membrane was found to be the same (~70/30 %) in the lipid vesicles and in the silica-particle supported lipid membrane, which provides information on the mechanism by which the vesicles adsorb to the surface. Furthermore, cytochrome c oxidase could maintain a proton electrochemical gradient across the supported proteomembrane, i.e. the membrane system was proton tight, defining an interior particle compartment that is separated from the surrounding aqueous media. Such a biofunctional cellular interface, supported onto a colloid that has a connected interior cytoskeleton-like pore structure, provides a basis for functional studies of membrane-bound transport proteins, and also for applications within pharmaceutical drug delivery.

Keyword
Supported lipid bilayer, mesoporous spheres, nanoparticles, membrane protein, drug delivery, cytochrome c oxidase
National Category
Inorganic Chemistry Industrial Biotechnology Physical Chemistry
Research subject
Biochemistry; Materials Science
Identifiers
urn:nbn:se:su:diva-27829 (URN)10.1021/nn9005413 (DOI)000269988600027 ()
Projects
Synthesis, functionalisation and controlled release of mesoporous materials
Available from: 2009-05-20 Created: 2009-05-20 Last updated: 2017-12-13Bibliographically approved

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