Complex Formation by Electrostatic Interaction between Carboxyl-Terminated Dendrimers and Oppositely Charged Polyelectrolytes

Miura, Norihiko; Dubin, Paul L.; Moorefield, and C. N.; Newkome, George R.

doi:10.1021/la990125l

Cited by 69 publications

(83 citation statements)

References 26 publications

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“…These experiments confirm that complexation occurs only when the surface charge density exceeds a critical value. This value typically grows with the reciprocal Debye screening length as j c j b with b 1 ÿ 1:4 [15,[25][26][27]. Our results agree with the experimental findings when we take the above dependence of l into account.…”

Section: -2supporting

confidence: 90%

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Critical Adsorption of Polyelectrolytes onto Charged Spherical Colloids

Winkler

Cherstvy

2006

Phys. Rev. Lett.

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The adsorption of a flexible polyelectrolyte in a salt solution onto an oppositely charged spherical surface is investigated. An analytical solution is derived, which is valid for any sphere radius and consistently recovers the result of a planar surface in the limit of large sphere radii, by substituting the Debye-Hückel potential via the Hulthén potential. Expressions for critical quantities such as the critical radius and the critical surface charge density are provide. A comparison of our theoretical results with experiments and computer simulations yields remarkable good agreement. DOI: 10.1103/PhysRevLett.96.066103 PACS numbers: 68.43.De, 82.35.Rs The complexation of charged macroions by oppositely charged polyelectrolytes is a fundamental process in biological systems and many technical applications. Particular examples are the complexation of histone proteins by DNA in nucleosomal core particles [1,2] as well as complexes of polyelectrolytes with charged colloids and micelles [3]. Industrial applications are as diverse as stabilization of colloidal suspensions, water treatment, and paper making [4].The understanding of the complexation between a polyion and a macroion surface accompanied by screening effects due to counterions and salt posses a major theoretical challenge [5]. Despite significant efforts and progresses [5][6][7][8][9][10][11], the understanding of charged complexes is still unsatisfactory and lacks behind that of neutral complexes. Certain insight into the complexation process is typically obtained by approximation schemes, e.g., variational calculations [6 -9], which, however, may lead to controversial results [12] and often apply only in limiting situations such as pointlike particles [9] or large colloidal radii [6].The theoretical studies of the adsorption behavior of polyelectrolytes onto spherical surfaces [7,10,11,13,14] lead to the observation of a phase-transition-like behavior; i.e., a bound polymer state appears at certain critical conditions which depend on, e.g., the sphere radius and screening of the Coulomb interaction. The variational calculations of Muthukumar and his co-workers [6,8] have provided useful insight into this transition in the limit of large sphere radii. Experiments on polyelectrolyte-protein and -micelle complexes [15] and computer simulations [14], however, typically yield dependencies of the critical quantities on the Debye screening length which deviate from the theoretical predictions. To understand and interpret the experimental results correctly, an analytical solution of the adsorption problem valid for any sphere radius is mandatory.In this Letter, we will present an exact solution for the critical adsorption of a flexible polyelectrolyte onto an oppositely charged spherical macroion. Expressions for critical quantities are provided, which are valid for any sphere radius. In particular, in the limit of zero macroion curvature, the results for a planar surface are obtained. In general, we find a significantly different dependence of the critica...

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Section: -2supporting

confidence: 90%

“…[15,23,[25][26][27]. These experiments confirm that complexation occurs only when the surface charge density exceeds a critical value.…”

Section: -2supporting

confidence: 63%

Critical Adsorption of Polyelectrolytes onto Charged Spherical Colloids

Winkler

Cherstvy

2006

Phys. Rev. Lett.

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“…In this case host and guest molecules and macromolecules possess charges of the opposite sign. Several experimental studies [5,6,7] clarify general structure of dendrimerlinear polyelectrolyte (PE) complexes. In particular, atomic-force-microscopy data [8] and titration combined with spectroscopy [9] indicate that DNA macromolecules wrap around charged dendrimer-like polymers.…”

Section: Introductionmentioning

confidence: 99%

Dynamics of Complexation of a Charged Dendrimer by Linear Polyelectrolyte: Computer Modelling

Lyulin

Darinskii

2007

E-Polymers

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Brownian-dynamics simulations have been performed for complexes formed by a charged dendrimer and a long oppositely charged linear polyelectrolyte when overcharging phenomenon is always observed. After complex formation the orientational mobility of the individual dendrimer bonds, the fluctuations of the dendrimer size, and the dendrimer rotational diffusion have been simulated. Corresponding relaxation times do not depend on the linear-chain length in a complex and are close to those for a single neutral dendrimer. At the same time fluctuations of the size of a complex are completely defined by the corresponding fluctuations of a linear polyelectrolyte size. Adsorbed polyelectrolyte practically does not feel the rotation of a dendrimer; simulated complexes may be considered as nuts with light core (dendrimer) and heavy shell (adsorbed linear polymer); the electrostatic contacts between dendrimer and oppositely charged linear polymer are easily broken due to the very fast dendrimer-size fluctuations.

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“…[3,4] Experimental efforts have also been focused on the complexation of charged dendrimers with oppositely charged polyelectrolytes. [5][6][7][8] All these investigations focus on spherical dendrimers carrying ionogenic terminal groups, e.g., polyamidoamine and polypropyleneimine.…”

Section: Introductionmentioning

confidence: 99%

Conformations of Highly Charged Dendronized Polymers in Aqueous Solutions of Varying Ionic Strength

Girbasova

Aseyev

Saratovsky

et al. 2003

Macro Chemistry & Physics

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Conformations of two linear, charged dendronized polymers in aqueous solutions of different ionic strengths have been studied by light scattering. Both polymers have a polyacrylic core. The repeating unit of the first of the polymers studied contains a residue of aspartic acid bound to a carboxylic group of the core by an amide group as a first‐generation dendron, whereas the second polymer contains second‐generation dendrons constructed of three molecules of aspartic acid. The dendritic polymers adopt different conformations depending on the generation. Polymers with first‐generation dendrons are flexible and their conformation is sensitive to salt. The polymers with dendrons of the second generation adopt a semi‐flexible rod conformation. Their conformation is not sensitive to salt but is determined by the bulkiness of the dendrons.Polyacrylic polymers having a residue of aspartic acid as a first‐generation dendron (P1), and having a second‐generation dendron on the basis of aspartic acid (P2).magnified imagePolyacrylic polymers having a residue of aspartic acid as a first‐generation dendron (P1), and having a second‐generation dendron on the basis of aspartic acid (P2).

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Complex Formation by Electrostatic Interaction between Carboxyl-Terminated Dendrimers and Oppositely Charged Polyelectrolytes

Cited by 69 publications

References 26 publications

Critical Adsorption of Polyelectrolytes onto Charged Spherical Colloids

Critical Adsorption of Polyelectrolytes onto Charged Spherical Colloids

Dynamics of Complexation of a Charged Dendrimer by Linear Polyelectrolyte: Computer Modelling

Conformations of Highly Charged Dendronized Polymers in Aqueous Solutions of Varying Ionic Strength

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