Structural elucidation of soluble polyelectrolyte-micelle complexes: intra- vs interpolymer association

Xia, Jiliang; Zhang, Huiwen; Rigsbee, Daniel R.; Dubin, Paul L.; Shaikh, Tehseen

doi:10.1021/ma00063a019

Cited by 102 publications

(130 citation statements)

References 5 publications

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“…8 (4) At σ > σ φ , bulk phase separation (either coacervation or precipitation) occurs. (5) The magnitude of σ φ -σ c depends, in a complicated way, on inter alia stoichiometry and micelle structure, 9 but within this range, soluble macromolecular complexes are formed reversibly and may be characterized by numerous scattering, hydrodynamic, and spectroscopic methods. Many of these conclusions have been shown to apply to protein-polyelectrolyte complexes as well.…”

Section: Introductionmentioning

confidence: 99%

Complex Formation between Bovine Serum Albumin and Strong Polyelectrolytes: Effect of Polymer Charge Density

1998

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Light scattering and pH titration were used to examine the binding of bovine serum albumin (BSA) to poly-(diallyldimethylammonium chloride) (PDADMAC), poly(acrylamidomethylpropyl sulfonate) (PAMPS), poly-(methacrylamidopropyltrimethylammonium chloride) (PMAPTAC), and an AMPS-acrylamide random copolymer (PAMPS 80 AAm 20 ). The critical protein charge required to induce protein-polyelectrolyte complexation, (Zpr) c , was found to vary linearly with the square root of the ionic strength (I 1/2 ), i.e., with the Debye-Hu ¨ckel parameter (κ), the proportionality constant being a function of polyelectrolyte chain parameters such as intrinsic stiffness and charge density. This linearity was remarkably continuous through Zpr ) 0, with (Zpr) c occurring predominantly "on the wrong side" of the isoionic point; i.e., the onset of binding was typically observed when the global protein charge was of the same sign as the polyelectrolyte. Binding of BSA to the lower charge density polyanion (PAMPS 80 AAm 20 ) unexpectedly occurred under conditions where binding to the more highly charged homopolyanion (PAMPS) did not. The theoretical treatment of Muthukumar was used to interpret the linearity of (Zpr) c vs I 1/2 and the observed influence of polyelectrolyte structural parameters. The apparent applicability of this model to the heterogeneous amphoteric protein surface suggests that binding of polyelectrolytes takes place at "charge patches" whose effective charge densities are different from, but nevertheless linearly dependent on, the global charge density.

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Section: Introductionmentioning

confidence: 99%

Complex Formation between Bovine Serum Albumin and Strong Polyelectrolytes: Effect of Polymer Charge Density

1998

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“…Static [28,30,49] and quasielastic [25,[27][28][29]49] light scattering especially have provided important information on the size and structure of polymermicelle complexes but soluble complexes can only be detected by QELS if their lifetime (residence time) is sufficiently long and the scattering intensity of the complexes is sufficiently large compared with those of the micelles and polymers from which they form.…”

Section: Introductionmentioning

confidence: 99%

Interactions of micelles with fluorescence-labeled polyelectrolytes

Morishima

Mizusaki

Yoshida

et al. 1999

Colloids and Surfaces A: Physicochemical and Engineering Aspect

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Pyrene-labeled polyelectrolytes can be used to study the interaction between the polyelectrolyte and an oppositely charged micelle, if the micelle incorporates a fluorescence quencher. If the charge on the micelle is varied systematically, polymer-micelle complex formation can be observed at some well-defined micelle surface charge density. Applying a kinetic model to steady-state and time-dependent fluorescence quenching data, one can estimate the binding constant (K), association rate constant, and lifetime (residence time). K increases strongly with increase in micelle surface charge density (|) or decrease in ionic strength (v). These effects arise from the dependence of association rate constant and residence time on | and v. While these observations reflect the fundamental electrostatic nature of the interaction, it is also found that micelles preferentially bind to pyrene sites, so that complex formation results from the conjoint action of electrostatic and hydrophobic forces.

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“…Indeed, polyelectrolyte-micelle complexation is more appropriately considered as a subset of polyelectrolyte-colloid interaction, and distinct from interactions of polymers with surfactants below the CMC. Included in the list of polyelectrolytes studied in combination with oppositely charged micelles are poly(acrylamidomethylpropanesulfonate) (PAMPS) and AMPS-acrylamide copolymers (10), poly(vinylsulfonate) (PVS) (12), poly(styrenesulfonate) (PSS) (13), poly(methacrylamidopropyltrimethylammonium chloride) (PMAPTAC) (14), sulfonated poly(vinylalcohol) (PVAS) (15), MAPTACacrylamide copolymers (16), and poly(dimethyldiallylammonium chloride) (PDADMAC) (17). All of these are strong polyelectrolytes, inasmuch as all ionic residues are fully dissociated, regardless of pH.…”

Section: Introductionmentioning

confidence: 99%

Binding of Polycarboxylic Acids to Cationic Mixed Micelles: Effects of Polymer Counterion Binding and Polyion Charge Distribution

Yoshida

Sokhakian

Dubin

1998

Journal of Colloid and Interface Science

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Mixed micelles of cetyltrimethylammonium chloride (CTAC) and n-dodecyl hexaoxyethylene glycol monoether (C 12 E 8 ) bind to polyanions when the mole fraction of the cationic surfactant exceeds a critical value (Y c ). Y c corresponds to a critical micelle surface charge density at which polyelectrolyte will bind to this colloidal particle. Turbidimetric titrations were used to determine Y c for such cationic-nonionic micelles in the presence of acrylic acid and acrylamido-2-methylpropane sulfonate homopolymers (PAA and PAMPS, respectively) and their copolymers with acrylamide, as function of pH, ionic strength, and polyelectrolyte counterion. In 0.20 M NaCl, Y c for PAA is found to be remarkably insensitive to pH, i.e., virtually independent of the apparent polymer charge density app . On the other hand, the expected inverse relationship between Y c and app is observed either for PAA when NaCl is replaced by TMACl (tetramethylammonium chloride), or when app is manipulated using acrylic acid/acrylamide copolymers at high pH. The effective charge density of PAA is thus seen to be suppressed by specific sodium ion binding, indicating that the influence of salts on the interaction of polycarboxylic acids with colloidal particles may differ qualitatively from their effect on the analogous behavior of strong polyanions. Comparisons between homo-and copolymers of acrylic acid were carried out also to test the hypothesis that the "mobility" of charges on PAA at moderate pH (degree of ionization less than unity) could make this "annealed" polymer exhibit the behavior of a more highly charged one. The results, while consistent with this expectation, were obscured by the likely effect of copolymer sequence distributions.

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Structural elucidation of soluble polyelectrolyte-micelle complexes: intra- vs interpolymer association

Cited by 102 publications

References 5 publications

Complex Formation between Bovine Serum Albumin and Strong Polyelectrolytes: Effect of Polymer Charge Density

Complex Formation between Bovine Serum Albumin and Strong Polyelectrolytes: Effect of Polymer Charge Density

Interactions of micelles with fluorescence-labeled polyelectrolytes

Binding of Polycarboxylic Acids to Cationic Mixed Micelles: Effects of Polymer Counterion Binding and Polyion Charge Distribution

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