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Dobryden, I., Ruiz, M. C., Zhang, X., Dédinaité, A., Wieland, D. C., Winnik, F. M. & Claesson, P. M. (2019). Thermoresponsive Pentablock Copolymer on Silica: Temperature Effects on Adsorption, Surface Forces, and Friction. Paper presented at AESSON PM, 1987, JOURNAL OF COLLOID AND INTERFACE SCIENCE, V117, P366 jas OJ, 2002, LANGMUIR, V18, P1604 ltermo A, 1996, JOURNAL OF COLLOID AND INTERFACE SCIENCE, V183, P506 trov P, 1997, LANGMUIR, V13, P3331 ein J, 2000, JOURNAL OF PHYSICS-CONDENSED MATTER4th Liquid Matter Conference, JUL 03-07, 1999, GRANADA, SPAIN, V12, PA19 unkett MA, 2003, LANGMUIR, V19, P4673 nquy Xavier, 2014, JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, V136, P6199 ttersson Torbjorn, 2008, JOURNAL OF COLLOID AND INTERFACE SCIENCE, V324, P246 ndin Maria, 2008, LANGMUIR, V24, P3814. Langmuir, 35(3), 653-661
Open this publication in new window or tab >>Thermoresponsive Pentablock Copolymer on Silica: Temperature Effects on Adsorption, Surface Forces, and Friction
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2019 (English)In: Langmuir, ISSN 0743-7463, E-ISSN 1520-5827, Vol. 35, no 3, p. 653-661Article in journal (Refereed) Published
Abstract [en]

The adsorption of hydrophilic or amphiphilic multiblock copolymers provides a powerful means to produce well-defined "smart" surfaces, especially if one or several blocks are sensitive to external stimuli. We focus here on an A-B-A-B-A copolymer, where A is a cationic poly((3acrylamido-propyl)-trimethylammonium chloride) (PAMPTMA) block containing 15 (end blocks) or 30 (middle block) repeat units and B is a neutral thermosensitive water-soluble poly(2-isopropyl-2-oxazoline) (PIPOZ) block with 50 repeat units. X-ray reflectivity and quartz crystal microbalance with dissipation monitoring were employed to study the adsorption of PAMPTMA(15)-PAMPTMA(30)-PIPOZ(50)-PAMPTMA(15) on silica surfaces. The latter technique was employed at different temperatures up to 50 degrees C. Surface forces and friction between the two silica surfaces across aqueous pentablock copolymer solutions at different temperatures were determined with the atomic force microscopy colloidal probe force and friction measurements. The cationic pentablock copolymer was found to have a high affinity to the negatively charged silica surface, leading to a thin (2 nm) and rigid adsorbed layer. A steric force was encountered at a separation of around 3 nm from hard wall contact. A capillary condensation of a polymer-rich phase was observed at the cloud point of the solution. The friction forces were evaluated using Amontons' rule modified with an adhesion term.

Place, publisher, year, edition, pages
AMER CHEMICAL SOC, 2019
National Category
Chemical Sciences
Identifiers
urn:nbn:se:kth:diva-244115 (URN)10.1021/acs.langmuir.8b03729 (DOI)000456749400007 ()30605339 (PubMedID)
Conference
AESSON PM, 1987, JOURNAL OF COLLOID AND INTERFACE SCIENCE, V117, P366 jas OJ, 2002, LANGMUIR, V18, P1604 ltermo A, 1996, JOURNAL OF COLLOID AND INTERFACE SCIENCE, V183, P506 trov P, 1997, LANGMUIR, V13, P3331 ein J, 2000, JOURNAL OF PHYSICS-CONDENSED MATTER4th Liquid Matter Conference, JUL 03-07, 1999, GRANADA, SPAIN, V12, PA19 unkett MA, 2003, LANGMUIR, V19, P4673 nquy Xavier, 2014, JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, V136, P6199 ttersson Torbjorn, 2008, JOURNAL OF COLLOID AND INTERFACE SCIENCE, V324, P246 ndin Maria, 2008, LANGMUIR, V24, P3814
Funder
Swedish Research Council, 2015-05080
Note

QC 20190219

Available from: 2019-02-19 Created: 2019-02-19 Last updated: 2019-02-19Bibliographically approved
Bełdowski, P., Weber, P., Dédinaité, A., Claesson, P. M. & Gadomski, A. (2018). Correction: Physical crosslinking of hyaluronic acid in the presence of phospholipids in an aqueous nano-environment (Soft Matter (2018) DOI: 10.1039/c8sm01388h). Soft Matter, 14(47)
Open this publication in new window or tab >>Correction: Physical crosslinking of hyaluronic acid in the presence of phospholipids in an aqueous nano-environment (Soft Matter (2018) DOI: 10.1039/c8sm01388h)
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2018 (English)In: Soft Matter, Vol. 14, no 47Article in journal (Refereed) Published
Abstract [en]

Correction for 'Physical crosslinking of hyaluronic acid in the presence of phospholipids in an aqueous nano-environment' by Piotr Bełdowski et al., Soft Matter, 2018, DOI: 10.1039/c8sm01388h. 

Place, publisher, year, edition, pages
Royal Society of Chemistry, 2018
National Category
Corrosion Engineering
Identifiers
urn:nbn:se:kth:diva-246563 (URN)10.1039/c8sm90222d (DOI)000452321400018 ()2-s2.0-85058156639 (Scopus ID)
Note

Erratum

QC 20190527

Available from: 2019-05-27 Created: 2019-05-27 Last updated: 2019-05-27Bibliographically approved
Beldowski, P., Weber, P., Dédinaité, A., Claesson, P. M. & Gadomski, A. (2018). Physical crosslinking of hyaluronic acid in the presence of phospholipids in an aqueous nano-environment. Soft Matter, 14(44), 8997-9004
Open this publication in new window or tab >>Physical crosslinking of hyaluronic acid in the presence of phospholipids in an aqueous nano-environment
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2018 (English)In: Soft Matter, ISSN 1744-683X, E-ISSN 1744-6848, Vol. 14, no 44, p. 8997-9004Article in journal (Refereed) Published
Abstract [en]

Hyaluronic acid and phospholipids are two components in the synovial joint cavity that contribute to joint lubrication synergistically. Molecular dynamics simulations were performed and hydrogen bonds in hyaluronic acid were analyzed to identify specific sites that are responsible for its physical cross-linking. Two molecular masses of hyaluronic acid, 10 kDa and 160 kDa, were considered. We use molecular dynamics simulations and the small world network approach to investigate dynamic couplings using a distance map applied to oxygen atoms in a chain of hyaluronic acid in the presence of phospholipids and water. The distance characterizing the coupling can be defined in various ways to bring out the most evident differences between various scenarios of the polymer chain conformation We show herein a physical distance understood as H-bond length and classes of these distances which are defined in a coarse-grained picture of the molecule. Simulation results indicate that addition of phospholipids has little influence on hyaluronic acid crosslinking. However, longer chains and addition of lipids promote appreciably long lasting (resilient) networks that may be of importance in biological systems. Specific sites for hydrogen bonding of phospholipids to hyaluronic acid have also been identified.

Place, publisher, year, edition, pages
ROYAL SOC CHEMISTRY, 2018
National Category
Corrosion Engineering
Identifiers
urn:nbn:se:kth:diva-239758 (URN)10.1039/c8sm01388h (DOI)000450442300013 ()30394485 (PubMedID)2-s2.0-85056530941 (Scopus ID)
Note

QC 20190109

Available from: 2019-01-09 Created: 2019-01-09 Last updated: 2019-01-09Bibliographically approved
Poulsen, N. N., Ostergaard, J., Petersen, N. J., Daasbjerg, K., Iruthayaraj, J., Dédinaité, A., . . . Jensen, H. (2017). Automated coating procedures to produce poly(ethylene glycol) brushes in fused-silica capillaries. Journal of Separation Science, 40(3), 779-788
Open this publication in new window or tab >>Automated coating procedures to produce poly(ethylene glycol) brushes in fused-silica capillaries
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2017 (English)In: Journal of Separation Science, ISSN 1615-9306, E-ISSN 1615-9314, Vol. 40, no 3, p. 779-788Article in journal (Refereed) Published
Abstract [en]

Many bioanalytical methods rely on electrophoretic separation of structurally labile and surface active biomolecules such as proteins and peptides. Often poor separation efficiency is due to surface adsorption processes leading to protein denaturation and surface fouling in the separation channel. Flexible and reliable approaches for preventing unwanted protein adsorption in separation science are thus in high demand. We therefore present new coating approaches based on an automated in-capillary surface-initiated atom transfer radical polymerization process (covalent coating) aswell as by electrostatically adsorbing a presynthesized polymer leading to functionalized molecular brushes. The electroosmotic flow was measured following each step of the covalent coating procedure providing a detailed characterization and quality control. Both approaches resulted in good fouling resistance against the four model proteins cytochrome c, myoglobin, ovalbumin, and human serum albumin in the pH range 3.4-8.4. Further, even samples containing 10% v/v plasma derived from human blood did not show signs of adsorbing to the coated capillaries. The covalent as well as the electrostatically adsorbed coating were both found to be stable and provided almost complete suppression of the electroosmotic flow in the pH range 3.4-8.4. The coating procedures may easily be integrated in fully automated capillary electrophoresis methodologies.

Place, publisher, year, edition, pages
WILEY-V C H VERLAG GMBH, 2017
Keywords
adsorption, automation, capillary electrophoresis, molecular brushes
National Category
Biological Sciences
Identifiers
urn:nbn:se:kth:diva-205144 (URN)10.1002/jssc.201600878 (DOI)000397029500018 ()27868374 (PubMedID)2-s2.0-85007473706 (Scopus ID)
Note

QC 20170412

Available from: 2017-04-12 Created: 2017-04-12 Last updated: 2017-06-29Bibliographically approved
Wieland, D. C., Zander, T., Garamus, V. M., Krywka, C., Dédinaité, A., Claesson, P. M. & Willumeit-Roemer, R. (2017). Complex solutions under shear and pressure: a rheometer setup for X-ray scattering experiments. Journal of Synchrotron Radiation, 24, 646-652
Open this publication in new window or tab >>Complex solutions under shear and pressure: a rheometer setup for X-ray scattering experiments
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2017 (English)In: Journal of Synchrotron Radiation, ISSN 0909-0495, E-ISSN 1600-5775, Vol. 24, p. 646-652Article in journal (Refereed) Published
Abstract [en]

A newly developed high-pressure rheometer for in situ X-ray scattering experiments is described. A commercial rheometer was modified in such a way that X-ray scattering experiments can be performed under different pressures and shear. First experiments were carried out on hyaluronan, a ubiquitous biopolymer that is important for different functions in the body such as articular joint lubrication. The data hint at a decreased electrostatic interaction at higher pressure, presumably due to the increase of the dielectric constant of water by 3% and the decrease of the free volume at 300bar.

Place, publisher, year, edition, pages
INT UNION CRYSTALLOGRAPHY, 2017
Keywords
rheology, pressure, small-angle X-ray scattering, complex solutions, hyaluronan
National Category
Chemical Sciences
Identifiers
urn:nbn:se:kth:diva-207663 (URN)10.1107/S1600577517002648 (DOI)000400385400012 ()28452756 (PubMedID)2-s2.0-85018331890 (Scopus ID)
Note

QC 20170602

Available from: 2017-06-02 Created: 2017-06-02 Last updated: 2017-11-10Bibliographically approved
Wieland, D. C., Degen, P., Zander, T., Gayer, S., Raj, A., An, J., . . . Willumeit-Roemer, R. (2016). Structure of DPPC-hyaluronan interfacial layers - effects of molecular weight and ion composition. Soft Matter, 12(3), 729-740
Open this publication in new window or tab >>Structure of DPPC-hyaluronan interfacial layers - effects of molecular weight and ion composition
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2016 (English)In: Soft Matter, ISSN 1744-683X, E-ISSN 1744-6848, Vol. 12, no 3, p. 729-740Article in journal (Refereed) Published
Abstract [en]

Hyaluronan and phospholipids play an important role in lubrication in articular joints and provide in combination with glycoproteins exceptionally low friction coefficients. We have investigated the structural organization of 1,2-dipalmitoyl-sn-glycero-3-phosphocholine (DPPC) Langmuir layers at the solution-air interface at different length scales with respect to the adsorption of hyaluronan (HA). This allows us to assemble a comprehensive picture of the adsorption and the resulting structures, and how they are affected by the molecular weight of HA and the presence of calcium ions. Brewster angle microscopy and grazing incident diffraction were used to determine the lateral structure at the micro- and macro scale. The data reveals an influence of HA on both the macro and micro structure of the DPPC Langmuir layer, and that the strength of this effect increases with decreasing molecular weight of HA and in presence of calcium ions. Furthermore, from X-ray reflectivity measurements we conclude that HA adsorbs to the hydrophilic part of DPPC, but data also suggest that two types of interfacial structures are formed at the interface. We argue that hydrophobic forces and electrostatic interactions play important rules for the association between DPPC and HA. Surface pressure area isotherms were used to determine the influence of HA on the phase behavior of DPPC while electrophoretic mobility measurements were used to gain insight into the binding of calcium ions to DPPC vesicles and hyaluronan.

Place, publisher, year, edition, pages
Royal Society of Chemistry, 2016
National Category
Materials Engineering Chemical Sciences Physical Sciences
Identifiers
urn:nbn:se:kth:diva-183346 (URN)10.1039/c5sm01708d (DOI)000369746800010 ()26508354 (PubMedID)2-s2.0-84954134754 (Scopus ID)
Note

QC 20160307

Available from: 2016-03-07 Created: 2016-03-07 Last updated: 2017-11-30Bibliographically approved
Wieland, D. C., Garamus, V. M., Zander, T., Krywka, C., Wang, M., Dedinaite, A., . . . Willumeit-Roemer, R. (2016). Studying solutions at high shear rates: a dedicated microfluidics setup. Journal of Synchrotron Radiation, 23, 480-486
Open this publication in new window or tab >>Studying solutions at high shear rates: a dedicated microfluidics setup
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2016 (English)In: Journal of Synchrotron Radiation, ISSN 0909-0495, E-ISSN 1600-5775, Vol. 23, p. 480-486Article in journal (Refereed) Published
Abstract [en]

The development of a dedicated small-angle X-ray scattering setup for the investigation of complex fluids at different controlled shear conditions is reported. The setup utilizes a microfluidics chip with a narrowing channel. As a consequence, a shear gradient is generated within the channel and the effect of shear rate on structure and interactions is mapped spatially. In a first experiment small-angle X-ray scattering is utilized to investigate highly concentrated protein solutions up to a shear rate of 300000 s(-1). These data demonstrate that equilibrium clusters of lysozyme are destabilized at high shear rates.

Place, publisher, year, edition, pages
INT UNION CRYSTALLOGRAPHY, 2016
Keywords
shear, complex solutions, small-angle X-ray scattering (SAXS), microfluidics, lysozyme, aggregation, rheology, protein interaction, beamline setup
National Category
Materials Chemistry
Identifiers
urn:nbn:se:kth:diva-184963 (URN)10.1107/S1600577515024856 (DOI)000371387900014 ()26917136 (PubMedID)2-s2.0-84959274343 (Scopus ID)
Note

QC 20160407

Available from: 2016-04-07 Created: 2016-04-07 Last updated: 2017-11-30Bibliographically approved
Zander, T., Wieland, D. C., Raj, A., Wang, M., Nowak, B., Krywka, C., . . . Willumeit-Romer, R. (2016). The influence of hyaluronan on the structure of a DPPC-bilayer under high pressures. Colloids and Surfaces B: Biointerfaces, 142, 230-238
Open this publication in new window or tab >>The influence of hyaluronan on the structure of a DPPC-bilayer under high pressures
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2016 (English)In: Colloids and Surfaces B: Biointerfaces, ISSN 0927-7765, E-ISSN 1873-4367, Vol. 142, p. 230-238Article in journal (Refereed) Published
Abstract [en]

The superior lubrication properties of synovial joints have inspired many studies aiming at uncovering the molecular mechanisms which give rise to low friction and wear. However, the mechanisms are not fully understood yet, and, in particular, it has not been elucidated how the biolubricants present at the interface of cartilage respond to high pressures, which arise during high loads of joints. In this study we utilize a simple model system composed of two biomolecules that have been implied as being important for joint lubrication. It consists of a solid supported dipalmitoylphosphatidylcholin (DPPC) bilayer, which was formed via vesicles fusion on a flat Si wafer, and the anionic polysaccharide hyaluronan (HA). We first characterized the structure of the HA layer that adsorbed to the DPPC bilayers at ambient pressure and different temperatures using X-ray reflectivity (XRR) measurements. Next, XRR was utilized to evaluate the response of the system to high hydrostatic pressures, up to 2 kbar (200 MPa), at three different temperatures. By means of fluorescence microscopy images the distribution of DPPC and HA on the surface was visualized. Our data suggest that HA adsorbs to the headgroup region that is oriented towards the water side of the supported bilayer. Phase transitions of the bilayer in response to temperature and pressure changes were also observed in presence and absence of HA. Our results reveal a higher stability against high hydrostatic pressures for DPPC/HA composite layers compared to that of the DPPC bilayer in absence of HA.

Keywords
Lubrication, Synovial joint, Vesicle fusion, Supported DPPC bilayer, Hyaluronan, High pressure, X-ray reflectivity
National Category
Physical Chemistry
Identifiers
urn:nbn:se:kth:diva-187770 (URN)10.1016/j.colsurfb.2016.02.040 (DOI)000375169600028 ()26954090 (PubMedID)
Funder
EU, FP7, Seventh Framework Programme, 312284
Note

QC 20160530

Available from: 2016-05-30 Created: 2016-05-30 Last updated: 2017-11-30Bibliographically approved
Liu, X., Dédinaité, A., Nylander, T., Dabkowska, A. P., Skoda, M., Makuska, R. & Claesson, P. M. (2015). Association of anionic surfactant and physisorbed branched brush layers probed by neutron and optical reflectometry. Journal of Colloid and Interface Science, 440, 245-252
Open this publication in new window or tab >>Association of anionic surfactant and physisorbed branched brush layers probed by neutron and optical reflectometry
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2015 (English)In: Journal of Colloid and Interface Science, ISSN 0021-9797, E-ISSN 1095-7103, Vol. 440, p. 245-252Article in journal (Refereed) Published
Abstract [en]

Pre-adsorbed branched brush layers were formed on silica surfaces by adsorption of a diblock copolymer consisting of a linear cationic block and an uncharged bottle-brush block. The charge of the silica surface was found to affect the adsorption, with lower amounts of the cationic polyelectrolyte depositing on less charged silica. Cleaning under basic conditions rendered surfaces more negatively charged (more negative zeta-potential) than acid cleaning and was therefore used to increase polyelectrolyte adsorption. The structure of adsorbed layers of the diblock copolymer was as determined by neutron reflectometry found to be about 70 nm thick and very water rich (97%). Interactions between the anionic surfactant sodium dodecylsulfate (SDS) and such pre-adsorbed diblock polymer layers were studied by neutron reflectometry and by optical reflectometry. Optical reflectometry was also used for deducing interactions between the individual blocks of the diblock copolymer and SDS at the silica/aqueous interface. We find that SDS is readily incorporated in the diblock copolymer layer at low SDS concentrations, and preferentially co-localized with the cationic block of the polymer next to the silica surface. At higher SDS concentrations some desorption of polyelectrolyte/surfactant complexes takes place.

Keywords
Polymer brush layer, Diblock copolymer, SDS, Adsorption, Polyelectrolyte-surfactant complex, Optical reflectometry, Neutron reflectivity
National Category
Chemical Sciences
Identifiers
urn:nbn:se:kth:diva-157337 (URN)10.1016/j.jcis.2014.11.002 (DOI)000346461100031 ()2-s2.0-84911423822 (Scopus ID)
Funder
Swedish Research CouncilVINNOVAEU, FP7, Seventh Framework Programme, 290251
Note

QC 20150220. Updated from manuscript to published article.

Available from: 2014-12-09 Created: 2014-12-09 Last updated: 2017-12-05Bibliographically approved
An, J., Liu, X., Linse, P., Dedinaite, A., Winnik, F. M. & Claesson, P. M. (2015). Tethered Poly(2-isopropyl-2-oxazoline) Chains: Temperature Effects on Layer Structure and Interactions Probed by AFM Experiments and Modeling. Langmuir, 31(10), 3039-3048
Open this publication in new window or tab >>Tethered Poly(2-isopropyl-2-oxazoline) Chains: Temperature Effects on Layer Structure and Interactions Probed by AFM Experiments and Modeling
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2015 (English)In: Langmuir, ISSN 0743-7463, E-ISSN 1520-5827, Vol. 31, no 10, p. 3039-3048Article in journal (Refereed) Published
Abstract [en]

Thermoresponsive polymer layers on silica surfaces have been obtained by utilizing electrostatically driven adsorption of a cationic-nonionic diblock copolymer. The cationic block provides strong anchoring to the surface for the nonionic block of poly(2-isopropyl-2-oxazoline), referred to as PIPOZ. The PIPOZ chain interacts favorably with water at low temperatures, but above 46 degrees C aqueous solutions of PIPOZ phase separate as water becomes a poor solvent for the polymer. We explore how a change in solvent condition affects interactions between such adsorbed layers and report temperature effects on both normal forces and friction forces. To gain further insight, we utilize self-consistent lattice mean-field theory to follow how changes in temperature affect the polymer segment density distributions and to calculate surface force curves. We find that with worsening of the solvent condition an attraction develops between the adsorbed PIPOZ layers, and this observation is in good agreement with predictions of the mean-field theory. The modeling also demonstrates that the segment density profile and the degree of chain interpenetration under a given load between two PIPOZ-coated surfaces rise significantly with increasing temperature.

National Category
Chemical Sciences Physical Sciences
Identifiers
urn:nbn:se:kth:diva-165219 (URN)10.1021/la504653w (DOI)000351327300013 ()25686020 (PubMedID)2-s2.0-84925004133 (Scopus ID)
Note

QC 20150506

Available from: 2015-05-06 Created: 2015-04-24 Last updated: 2017-12-04Bibliographically approved
Organisations
Identifiers
ORCID iD: ORCID iD iconorcid.org/0000-0002-2288-819X

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