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  • 1.
    Bastardo Zambrano, Luis Alejandro
    KTH, Skolan för kemivetenskap (CHE), Kemi.
    Chitosan-SDS association probed by Small-Angle Neutron ScatteringManuskript (Annet (populærvitenskap, debatt, mm))
  • 2.
    Bastardo Zambrano, Luis Alejandro
    KTH, Skolan för kemivetenskap (CHE), Kemi, Ytkemi.
    Self assembly of surfactants and polyelectrolytes in solution and at interfaces2005Doktoravhandling, med artikler (Annet vitenskapelig)
    Abstract [en]

    This thesis focuses on the study of the interactions between polyelectrolytes and surfactants in aqueous solutions and at interfaces, as well as on the structural changes these molecules undergo due to that interaction. Small–angle neutron scattering, dynamic, and static light scattering were the main techniques used to investigate the interactions in bulk. The first type of polymer studied was a negatively charge glycoprotein (mucin); its interactions with ionic sodium alkyl sulfate surfactants and nonionic surfactants were determined. This system is of great relevance for several applications such as oral care and pharmaceutical products, since mucin is the main component of the mucus layer that protects the epithelial surfaces (e.g. oral tissues). Sodium dodecyl sulfate (SDS) on the other hand, has been used as foaming agent in tooth pastes for a very long time. In this work it is seen how SDS is very effective in dissolving the large aggregates mucin forms in solution, as well as in removing preadsorbed mucin layers from different surfaces. On the other hand, the nonionic surfactant n-dodecyl β-D-maltopyranoside (C12-mal), does not affect significantly the mucin aggregates in solution, neither does it remove mucin effectively from a negatively charge hydrophilic surface (silica). It can be suggested that nonionic surfactants (like the sugar–based C12-mal) could be used to obtain milder oral care products. The second type of systems consisted of positively charged polyelectrolytes and a negatively charged surfactant (SDS). These systems are relevant to a wide variety of applications ranging from mining and cleaning to gene delivery therapy. It was found that the interactions of these polyelectrolytes with SDS depend strongly on the polyelectrolyte structure, charge density and the solvent composition (pH, ionic strength, and so on). Large solvent isotopic effects were found in the interaction of polyethylene imine (PEI) and SDS, as well as on the interactions of this anionic surfactant and the sugar–based n-decyl β-D-glucopyranoside (C10G1). These surfactants mixtures formed similar structures in solutions to the ones formed by some of the polyelectrolytes studied, i.e. ellipsoidal micelles at low electrolyte concentration and stiff rods, at high electrolyte and SDS concentrations.

  • 3.
    Bastardo Zambrano, Luis Alejandro
    et al.
    KTH, Tidigare Institutioner                               , Kemi.
    Claesson, Per Martin
    KTH, Tidigare Institutioner                               , Kemi.
    Brown, W.
    Department of Physical Chemistry, University of Uppsala,.
    Interactions between mucin and alkyl sodium sulfates in solution: a light scattering study2002Inngår i: Langmuir, ISSN 0743-7463, E-ISSN 1520-5827, Vol. 18, nr 10, s. 3848-3853Artikkel i tidsskrift (Fagfellevurdert)
    Abstract [en]

    The properties of negatively charged mucin in aqueous solutions and its interaction with anionic sodium alkyl sulfates with different hydrocarbon chain lengths were studied by means of dynamic light scattering. It was observed that mucin forms aggregates in aqueous solutions with a hydrodynamic radius above 500 nm. These aggregates dissolve when sodium dodecyl sulfate or sodium decyl sulfate is present at sufficiently high concentration, above about 0.2 cmc (critical micellar concentration). On the other hand, sodium octyl sulfate is not very effective in dissolving the mucin aggregates. The hydrodynamic radius of the dissolved mucin, decorated with some associated surfactant, is found to be in the range of 40-90 nm. The observation that the dissolving power of the sodium alkyl sulfates decreases with decreasing surfactant chain length suggests that the association between the surfactant and mucin is hydrophobically driven. The kinetics of the dissolution process depends on the surfactant concentration, a higher surfactant concentration giving rise to a more rapid dissolution of the aggregates. It was also observed that when the ionic strength is increased, the surfactant concentration needed to dissolve the mucin aggregates decreases. This can be explained by reduction of repulsive electrostatic forces by the salt.

  • 4.
    Bastardo Zambrano, Luis Alejandro
    et al.
    KTH, Tidigare Institutioner                               , Kemi.
    Dedinaite, A.
    Unilever Res. Dvmt. Port Sunlight, Quarry Road East, Bebington, Wirral.
    Interactions between Mucin and Surfactants at Solid-Liquid Interfaces2002Inngår i: Langmuir, ISSN 0743-7463, E-ISSN 1520-5827, Vol. 18, nr 24, s. 9383-9392Artikkel i tidsskrift (Fagfellevurdert)
    Abstract [en]

    The association between mucin and surfactants at the solid-liquid interface has been investigated employing reflectometry. The study is particularly aimed at understanding the removal of preadsorbed mucin layers by surfactant addition. To this end we investigated the effect of three different surfactants, one anionic surfactant, sodium dodecylsulfate (SDS), and two nonionic ones, penta(oxy ethylene) dodecyl ether (C12E5) and n-dodecyl beta-D-maltopyranoside (C-12-mal), All three surfactants were found to be potent in removing mucin from hydrophobic surfaces. On the otherhand, C-12-mal was found to have a very limited effect on mucin adsorbed to hydrophilic negatively charged surfaces, whereas the mucin layer was removed by SDS and C12E5. The association between mucin and the three different surfactants was also investigated by means of dynamic light scattering and surface tension measurements. It was concluded that SDS associates readily with mucin above a critical surfactant concentration, about 0.2 cmc, whereas the nonionic surfactants associate with mucin to a very limited degree. The results obtained with the different techniques allow us to propose that C12E5 removes mucin from silica surfaces by competitive adsorption, whereas the removal of mucin by SDS is due to formation of mucin/SDS complexes that have reduced surface affinity and increased water solubility compared to mucin alone.

  • 5.
    Bastardo Zambrano, Luis Alejandro
    et al.
    KTH, Skolan för kemivetenskap (CHE), Kemi, Ytkemi.
    Garamus, V. M.
    GKSS Research Centre, Geesthacht.
    Bergström, Lars Magnus
    KTH, Skolan för kemivetenskap (CHE), Kemi, Ytkemi.
    Claesson, Per M.
    KTH, Skolan för kemivetenskap (CHE), Kemi, Ytkemi.
    The structures of complexes between polyethylene imine and sodium dodecyl sulfate in D2O: a scattering study2005Inngår i: Journal of Physical Chemistry B, ISSN 1520-6106, E-ISSN 1520-5207, Vol. 109, nr 1, s. 167-174Artikkel i tidsskrift (Fagfellevurdert)
    Abstract [en]

    The association between a highly branched polyelectrolyte with ionizable groups, polyethylene imine (PEI), and an anionic surfactant, sodium dodecyl sulfate (SDS), has been investigated at two pH values, using small-angle neutron and light scattering. The scattering data allow us to obtain a detailed picture of the association structures formed. Small-angle neutron scattering (SANS) measurements in solutions containing highly charged PEI at low pH and low SDS concentrations indicate the presence of disklike aggregates. The aggregates change to a more complex three-dimensional structure with increasing surfactant concentration. One pronounced feature in the scattering curves is the presence of a Bragg-like peak at high q-values observed at a surfactant concentration of 4.2 mM and above. This scattering feature is attributed to the formation of a common well-ordered PEI/SDS structure, in analogue to what has been reported for other polyelectrolyte-surfactant systems. Precipitation occurred at the charge neutralization point, and X-ray diffraction measurements on the precipitate confirmed the existence of an ordered structure within the PEI/SDS aggregates, which was identified as a lamellar internal organization. Polyethylene imine has a low charge density in alkaline solutions. At pH 10.1 and under conditions where the surfactant was contrast matched, the SANS scattering curves showed only small changes with increasing surfactant concentration. This suggests that the polymer acts as a template onto which the surfactant molecules aggregate. Data from both static light scattering and SANS recorded under conditions where SDS and to a lower degree PEI contribute to the scattering were found to be consistent with a structure of stacked elliptic bilayers. These structures increased in size and became more compact as the surfactant concentration was increased up to the charge neutralization point.

  • 6.
    Bastardo Zambrano, Luis Alejandro
    et al.
    KTH, Skolan för kemivetenskap (CHE), Kemi, Ytkemi.
    Iruthayaraj, Joseph
    KTH, Skolan för kemivetenskap (CHE), Kemi, Ytkemi.
    Lundin, Maria
    KTH, Skolan för kemivetenskap (CHE), Kemi, Ytkemi.
    Dédinaité, Andra
    KTH, Skolan för kemivetenskap (CHE), Kemi, Ytkemi.
    Vareikis, Aušvydas
    Department of Polymer Chemistry, Vilnius University.
    Makuška, Ričardas
    Department of Polymer Chemistry, Vilnius University.
    van der Wal, Albert
    Lever Faberage Europe Global Technology Centre, Unilever R and D.
    Furó, István
    KTH, Skolan för kemivetenskap (CHE), Kemi, Fysikalisk kemi.
    Garamus, Vasil M.
    GKSS Research Centre.
    Claesson, Per M.
    KTH, Skolan för kemivetenskap (CHE), Kemi, Ytkemi.
    Soluble complexes in aqueous mixtures of low charge density comb polyelectrolyte and oppositely charged surfactant probed by scattering and NMR2007Inngår i: Journal of Colloid and Interface Science, ISSN 0021-9797, E-ISSN 1095-7103, Vol. 312, nr 1, s. 21-33Artikkel i tidsskrift (Fagfellevurdert)
    Abstract [en]

    A low charge density polyelectrolyte with a high graft density of 45 units long poly(ethylene oxide) side-chains has been synthesized. In this comb polymer, denoted PEO(45)MEMA:METAC-2, 2 mol% of the repeating methacrylate units in the polymer backbone carry a permanent positive charge and the remaining 98 mol% a 45 unit long PEO side-chain. Here we describe the solution conformation of this polymer and its association with an anionic surfactant, sodium dodecylsulfate, SDS. It will be shown that the polymer can be viewed as a stiff rod with a cross-section radius of gyration of 29 A. The cross section of the rod contracts with increasing temperature due to decreased solvency of the PEO side-chains. The anionic surfactant associates to a significant degree with PE045MEMA:METAC-2 to form soluble complexes at all stoichiometries. A cooperative association is observed as the free SDS concentration approaches 7 mM. At saturation the number of SDS molecules associated with the polymer amounts to 10 for each PEO side-chain. Two distinct populations of associated surfactants are observed, one is suggested to be molecularly distributed over the comb polymer and the other constitutes small micellar-like structures at the periphery of the aggregate. These conclusions are reached based on results from small-angle neutron scattering, static light scattering, NMR, and surface tension measurements.

  • 7.
    Bastardo Zambrano, Luis Alejandro
    et al.
    KTH, Skolan för kemivetenskap (CHE), Kemi, Ytkemi.
    Mészaros, R.
    Department of Colloid Chemistry, Eötvös Loránd University, Budapest.
    Varga, I.
    Department of Colloid Chemistry, Eötvös Loránd University, Budapest.
    Gilanyi, T.
    Department of Colloid Chemistry, Eötvös Loránd University, Budapest.
    Claesson, Per Martin
    KTH, Skolan för kemivetenskap (CHE), Kemi, Ytkemi.
    Deuterium isotope effects on the interaction between hyperbranched polyethylene imine and an anionic surfactant2005Inngår i: Journal of Physical Chemistry B, ISSN 1520-6106, E-ISSN 1520-5207, Vol. 109, nr 33, s. 16196-16202Artikkel i tidsskrift (Fagfellevurdert)
    Abstract [en]

    Solvent isotope effects on the interaction between the hyperbranched cationic polyelectrolyte, polyethylene imine (PEI), and the anionic surfactant sodium dodecyl sulfate (SDS) were investigated using potentiometric titration and eletrophoretic mobility measurements. In the basic pH range, a significantly higher fraction of the amine groups was found to be protonated when the PEI was dissolved in D2O compared to H2O at the same pH/pD. The difference in polymer charge in the two solvents decreases gradually with decreasing pH, and it completely diminishes at around pH = 4. Electrophoretic mobility measurements of PEI/SDS complexes at different pH values correlated very well with these observations. At pH/pD approximate to 9 a much higher mobility of the PEI/SDS complexes was found in D2O than in H2O at low surfactant concentrations, and the charge neutralization point shifted to a considerably larger surfactant concentration in heavy water. These results can be explained by the significantly higher charge density of the PEI in D2O compared to H2O. However, at the natural pH/pD as well as at pH = 4 and pD = 4 conditions the PEI molecules have roughly equal charge densities, which result in very similar charged characteristics (mobilities) of the PEI/SDS complexes as well as the same charge neutralization SDS concentration. It can be concluded that extreme care must be taken in the general analysis of those experiments in which weak polyelectrolyte/surfactant aggregates are investigated in heavy water, and then these observations are correlated with structures of the same system in water.

  • 8.
    Bergström, L. M.
    et al.
    Department of Pharmacy, Pharmaceutical Physical Chemistry, Uppsala University.
    Bastardo Zambrano, Luis Alejandro
    KTH, Skolan för kemivetenskap (CHE), Kemi, Ytkemi.
    Garamus, V. M.
    GKSS Research Centre, Geesthacht.
    A small-angle neutron and static light scattering study of micelles formed in aqueous mixtures of a nonionic alkylglucoside and an anionic surfactant2005Inngår i: Journal of Physical Chemistry B, ISSN 1520-6106, E-ISSN 1520-5207, Vol. 109, nr 25, s. 12387-12393Artikkel i tidsskrift (Fagfellevurdert)
    Abstract [en]

    The size and shape of micelles formed in aqueous mixtures of the anionic surfactant sodium dodecyl sulfate (SDS) and the nonionic sugar-based surfactant n-decyl beta-D-glucopyranoside (C(10)G) at different concentrations of added salt have been investigated with small-angle neutron and static light scattering. Rather small prolate ellipsoidal micelles form in the absence of added salt and at [NaCl] = 10 mM in D2O. The micelles grow considerably in length to large rods as the electrolyte concentration is raised to [NaCl] = 0.1 M. In excess of nonionic surfactant ([SDS]/[C(10)G] = 1:3) at [NaCl] = 0.1 M in D2O, several thousands of Angstroms long wormlike micelles are observed. Most interestingly, a conspicuously large isotope solvent effect was observed from static light scattering data according to which micelles formed at [SDS]/[C(10)G] = 1:3 and [NaCl] = 0.1 M in H2O are at least five times smaller than micelles formed in the corresponding samples in D2O.

  • 9.
    Dedinaite, Andra
    et al.
    KTH, Skolan för kemivetenskap (CHE), Kemi, Ytkemi.
    Bastardo Zambrano, Luis Alejandro
    Oliveira, C. P.
    Pedersen, J. S.
    Claesson, Per M
    KTH, Skolan för kemivetenskap (CHE), Kemi, Ytkemi.
    Vareikis, A.
    Makuska, R.
    Solution properties of bottle-brush polyelectrolytes2007Inngår i: PROCEEDINGS OF BALTIC POLYMER SYMPOSIUM 2007    , 2007, s. 112-116Konferansepaper (Fagfellevurdert)
    Abstract [en]

    Aqueous solution properties of bottle brush polyelectrolytes, where side-chains are attached to a polymer backbone, have been studied. The side chains consist of 45 units long poly(ethylene oxide) groups and the backbone is of the methacrylate type. Small-angle X-ray scattering (SAXS) was used to elucidate the solution conformation of this class of polymer and how it is affected by the side chain density and charge density. The effect of temperature on the solution conformation, and in particular the side chain extension, has also been quantified. At higher concentrations the interactions between the polymer chains in solution affects the scattering, and it is shown that this interaction is well described by a model originally developed for wormlike micelles.

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