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Multilayer Structures for Biomaterial Applications: Biomacromolecule-based Coatings
KTH, School of Chemical Science and Engineering (CHE), Chemistry, Surface Chemistry.
2005 (English)Doctoral thesis, comprehensive summary (Other scientific)
Abstract [en]

The cellular response to a biomaterial, such as a dental implant, is mainly governed by the surface properties, and can thus be altered by the introduction of a surface coating. In this thesis the buildup of a biomacromolecule-based coating formed by layerby-layer (LbL) deposition of the charged polypeptides poly(L-lysine) (PLL) and poly(L-glutamic acid) (PGA) has been studied. In an attempt to make these coatings bioactive and useful for bone-anchored implants, an amelogenin protein mixture (EMD), has been immobilized in these thin polyelectrolyte multilayer (PEM) films. Multilayers were also built by LbL deposition of the natural biomacromolecules collagen (Col) and hyaluronic acid (HA). Multilayer films of these two extra-cellular biomacromolecules should be of interest for use as a scaffold for tissue engineering.

The buildup of the multilayer films has been followed in situ, using ellipsometry, quartz crystal microbalance with dissipation (QCM-D), and dual polarization interferometry (DPI). The studied PLL/PGA multilayers were found to be highly hydrated, and to exhibit a two-regime buildup behavior, with an initial “slow-growing” regime, and a second “fast-growing” regime with a linear growth in film thickness and more than linear growth in mass. A net diffusion of polypeptides into the film during the buildup led to an increase in density of the films for each layer adsorbed. A change in density was also observed in the Col/HA film, where HA penetrated and diffused into the porous fibrous Col network.

The formed PLL/PGA films were further found to be rather stable during drying, and post-buildup changes in temperature and pH, not losing any mass as long as the temperature was not raised too rapidly. The film thickness responded to changes in the ambient media and collapsed reversibly when dried. A swelling/de-swelling behavior of the film was also observed for changes in the temperature and pH.

The EMD protein adsorbed to silica surfaces as nanospheres, and could by itself form multilayers. The adsorption of EMD onto PLL/PGA multilayer films increased at lower pH (5.0), and EMD could be immobilized in several layers by alternate deposition of EMD and PGA.

Place, publisher, year, edition, pages
Stockholm: KTH , 2005. , xvii, 67 p.
Series
Trita-YTK, ISSN 1650-0490 ; 0505
Keyword [en]
multilayer, layer-by-layer deposition, physical chemistry, surface chemistry, adsorption, ellipsometry, QCM-D, DPI, protein adsorption, polypeptides, biomaterials, biosurfaces, amelogenin, solid/liquid interface
National Category
Physical Chemistry
Identifiers
URN: urn:nbn:se:kth:diva-551ISBN: 91-7178-216-8 (print)OAI: oai:DiVA.org:kth-551DiVA: diva2:14411
Public defence
2005-12-16, F3, KTH, Lindstedtsvägen 26, Stockholm, 13:00
Opponent
Supervisors
Note
QC 20101019Available from: 2005-12-08 Created: 2005-12-08 Last updated: 2010-10-19Bibliographically approved
List of papers
1. Self-assembly/aggregation behavior and adsorption of enamel matrix derivate protein to silica surfaces
Open this publication in new window or tab >>Self-assembly/aggregation behavior and adsorption of enamel matrix derivate protein to silica surfaces
2006 (English)In: Langmuir, ISSN 0743-7463, E-ISSN 1520-5827, Vol. 22, no 5, 2227-2234 p.Article in journal (Refereed) Published
Abstract [en]

Adsorption of the amelogein protein mixture enamel matrix derivate (EMD) to silica surfaces has been studied by in situ ellipsometry and quartz crystal microbalance with dissipation (QCM-D). The protein was found to adsorb as nanospheres in mono- or multilayers, depending on the concentration of "free" nanospheres available in solution. The concentration of free nanospheres is determined by the competitive processes of adsorption and rapid aggregation into microscopic particles, measured by dynamic light scattering (DLS). Multilayers could also be formed by sequential injections of fresh EMD solution. At higher temperature, an up to 6 times thicker gel-like film was formed on the substrate surface, and decreasing the pH lead to disruption of the multi layer/aggregate formation and a decreased amount adsorbed.

Keyword
Adsorption, Crystals, Light scattering, Proteins, Quartz, Silica, Dynamic light scattering (DLS), Enamel matrix derivate (EMD), Gel-like films, Multilayer/aggregate formation
National Category
Physical Chemistry
Identifiers
urn:nbn:se:kth:diva-8919 (URN)10.1021/la0525123 (DOI)000235744500043 ()2-s2.0-33644905268 (Scopus ID)
Note

QC 20101019. Uppdaterad från submitted till published (20101019). Tidigare titel: Self-assembly/Aggregation Behavior, and Adsorption of Enamel Matrix Derivate Protein Nanospheres to Silica Surfaces

Available from: 2005-12-08 Created: 2005-12-08 Last updated: 2017-06-15Bibliographically approved
2. Multilayers of Charged Polypeptides As Studied by in Situ Ellipsometry and Quartz Crystal Microbalance with Dissipation
Open this publication in new window or tab >>Multilayers of Charged Polypeptides As Studied by in Situ Ellipsometry and Quartz Crystal Microbalance with Dissipation
2004 (English)In: Langmuir, ISSN 0743-7463, E-ISSN 1520-5827, Vol. 20, no 5, 1739-1745 p.Article in journal (Refereed) Published
Abstract [en]

The buildup of poly(L-glutamic acid) (PGA) and poly(L-lysine) (PLL) multilayers on silica and titanium surfaces, with and without an initial layer of polyethyleneimine (PEI), was investigated and characterized by means of in situ ellipsometry and quartz crystal microbalance with dissipation. A two-regime buildup was found in all systems, where the length of the first slow-growing regime is dependent on the structure of the initial layers. In the second fast-growing regime, the film thickness grows linearly while the mass increases more than linearly (close to exponentially) with the number of deposited layers. The film refractive indices as well as the water contents indicate that the film density changes as the multilayer film builds up. The change in film density was proposed to be due to polypeptides diffusing into the multilayer film as they attach. Furthermore, the use of PEI as the initial layer was found to induce a difference in the thickness increments for PGA and PLL.

Keyword
Biocompatibility, Biopolymers, Composition, Density (specific gravity), Ellipsometry, Multilayers, Polyelectrolytes, Refractive index, Silica, Surfaces, Titanium, Water, Film thickness, Poly l glutamic acid, Poly l lysine, Quartz crystal microbalance, Thickness increment
National Category
Physical Chemistry
Identifiers
urn:nbn:se:kth:diva-8920 (URN)10.1021/la035475t (DOI)000189241500030 ()2-s2.0-1542315206 (Scopus ID)
Note
QC 20101019Available from: 2005-12-08 Created: 2005-12-08 Last updated: 2017-12-14Bibliographically approved
3. Stability of Polypeptide Multilayers As Studied by in Situ Ellipsometry: Effects of Drying and Post-Buildup Changes in Temperature and pH
Open this publication in new window or tab >>Stability of Polypeptide Multilayers As Studied by in Situ Ellipsometry: Effects of Drying and Post-Buildup Changes in Temperature and pH
2004 (English)In: Journal of the American Chemical Society, ISSN 0002-7863, E-ISSN 1520-5126, Vol. 126, no 51, 17009-17015 p.Article in journal (Refereed) Published
Abstract [en]

Polyelectrolyte multilayers (PEM) of poly(L-glutamic acid) (PGA) and poly(L-lysine) (PLL) with an initial layer of polyethyleneimine (PEI) were built on silica and titanium surfaces using the layer-by-layer (LbL) technique. The stability of the film during drying/rewetting, temperature cycles, and pH shifts was studied in situ by means of ellipsometry. The film thickness was found to decrease significantly (approximately 70%) upon drying, but the original film thickness was regained upon rewetting, and the buildup could be continued. The thickness in the dry state was found to be extremely sensitive to ambient humidity, needing several hours to equilibrate. Changes in temperature and pH were also found to influence the multilayer thickness, leading to swelling and deswelling of as much as 8% and 10-20% respectively. The film does not necessarily regain its original thickness as the pH is shifted back, but instead shows clear signs of hysteresis.

Keyword
Drying, Ellipsometry, Hysteresis, Multilayers, Organic acids, pH effects, Polyelectrolytes, Silica, Swelling, Thermal effects, Wetting
National Category
Physical Chemistry
Identifiers
urn:nbn:se:kth:diva-8921 (URN)10.1021/ja0464645 (DOI)000225910400058 ()2-s2.0-11344269733 (Scopus ID)
Note
QC 20100930Available from: 2005-12-08 Created: 2005-12-08 Last updated: 2017-12-14Bibliographically approved
4. Immobilization of Enamel Matrix Derivate Protein onto Polypeptide Multilayers: Comparative in Situ Measurements using Ellipsometry, Quartz Crystal Microbalance with Dissipation, and Dual Polarization Interferometry
Open this publication in new window or tab >>Immobilization of Enamel Matrix Derivate Protein onto Polypeptide Multilayers: Comparative in Situ Measurements using Ellipsometry, Quartz Crystal Microbalance with Dissipation, and Dual Polarization Interferometry
2006 (English)In: Langmuir, ISSN 0743-7463, E-ISSN 1520-5827, Vol. 22, no 26, 11065-11071 p.Article in journal (Refereed) Published
Abstract [en]

The buildup of biodegradable poly(L-glutamic acid) (PGA) and poly(L-lysine) (PLL) multilayers on silica and titanium surfaces and the immobilization of enamel matrix derivate (EMD) protein was followed by utilizing in situ ellipsometry, quartz crystal microbalance with dissipation, and dual-polarization interferometry (DPI). The use of the relatively new DPI technique validated earlier published ellipsometry measurements of the PLL-PGA polypeptide films. The hydrophobic aggregating EMD protein was successfully immobilized both on top of and within the multilayer structures at pH 5.0. DPI measurements further indicated that the immobilization of EMD is influenced by the flow pattern during adsorption. The formed polypeptide-EMD multilayer films are of interest since it is known that EMD is able to trigger cell response and induce biomineralization. The multilayer films thus have potential to be useful as bioactive and biodegradable coatings for future dental implants.

Keyword
Dual-polarization interferometry, Enamel matrix derivate proteins, Polypeptide multilayers, Quartz crystal microbalance
National Category
Physical Chemistry
Identifiers
urn:nbn:se:kth:diva-8922 (URN)10.1021/la0607712 (DOI)000242771200035 ()2-s2.0-33846380249 (Scopus ID)
Note
QC 20100917. Uppdaterad från Manuskript till Artikel (20100917)Available from: 2005-12-08 Created: 2005-12-08 Last updated: 2017-12-14Bibliographically approved
5. Build-up of Collagen and Hyaluronic Acid Polyelectrolyte
Open this publication in new window or tab >>Build-up of Collagen and Hyaluronic Acid Polyelectrolyte
Show others...
2005 (English)In: Biomacromolecules, ISSN 1525-7797, E-ISSN 1526-4602, Vol. 6, no 3, 1353-1359 p.Article in journal (Refereed) Published
Abstract [en]

We have used a novel polyelectrolyte multilayer (PEM) coating consisting of the polyelectrolytes collagen and hyaluronic acid. The build-up by the layer-by-layer deposition technique is outlined by ex situ and in situ ellipsometric measurements. When collagen was added, the thickness of the PEM was increased, and the refractive index was decreased. Corresponding but opposite effects were noted when hyaluronic acid was added. These changes are considered to be explained by a diffusion mechanism. It was also found that the PEM layers were unstable at physiological pH. However, by cross-linking using N-(3-di-methylaminopropyl)-N-ethylcarbodiimide together with N-hydroxysuccinimide, a stable PEM layer resulted. These tissue friendly PEM layers are expected to have a great impact in the design of artificial extracellular matrixes. Also, the insertion of fluorescence labels demonstrates the potential for incorporation of other functionalities.

Keyword
Carboxylic acids, Collagen, Coloring, Crosslinking, Deposition, Diffusion, Ellipsometry, Fluorescence, Multilayers, pH effects, Physiology, Polyelectrolytes, Refractive index, Hyaluronic acid, Layer-by-layer deposition mechanism, Polyelectrolyte multilayers (PEM)
National Category
Physical Chemistry
Identifiers
urn:nbn:se:kth:diva-8924 (URN)000229138900025 ()
Note
QC 20101019Available from: 2005-12-08 Created: 2005-12-08 Last updated: 2017-12-14Bibliographically approved

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