Polyelectrolyte Brushes

Rühe, Jürgen; Ballauff, Matthias; Biesalski, Markus; Dziezok, Peter; Gröhn, Franziska; Johannsmann, Diethelm; Houbenov, Nikolay; Hugenberg, Norbert; Konradi, Rupert; Minko, Sergiy; Motornov, Michail; Netz, Roland R.; Schmidt, Manfred; Seidel, Christian; Stamm, Manfred; Stephan, Thomas; Usov, Denys; Zhang, Haining

doi:10.1007/b11268

Cited by 393 publications

(272 citation statements)

References 107 publications

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“…Neglecting also correlation effects at the surface, which are similar to the Onsager-Samarras effect [71], the pressure acting on the surface equals the sum of the surface osmotic pressure, P os = ρ + (0) + ρ − (0), proportional to the surface ion densities, and the electrostatic double layer attraction attraction P el = −2πℓ B σ 2 s , compare our discussion after Eq. (15). Equating surface and bulk pressures, P bulk = P os + P el , we obtain 2c s = ρ…”

Section: Charged Plate In the Presence Of Saltmentioning

confidence: 97%

“…If the polymers are under good-solvent conditions, they will swell and inhibit close contacts between two colloids. For this task, charged polymers are ideal, since they swell a lot in water [15]. Many structures obtained with charged colloids bear resemblance with atomic structures, but occur on length and time scales that are much easier to observe experimentally.…”

Section: Introductionmentioning

confidence: 99%

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Statics and dynamics of strongly charged soft matter

Boroudjerdi¹,

Kim²,

Naji³

et al. 2005

Physics Reports

346

523

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Soft matter materials, such as polymers, membranes, proteins, are often electrically charged. This makes them water soluble, which is of great importance in technological application and a prerequisite for biological function. We discuss a few static and dynamic systems that are dominated by charge effects. One class comprises complexation between oppositely charged objects, for example the adsorption of charged ions or charged polymers on oppositely charged substrates of different geometry. Here the main questions are whether adsorption occurs and what the effective charge of the resulting complex is. We explicitly discuss the adsorption behavior of polyelectrolytes on substrates of planar, cylindrical and spherical geometry with specific reference to DNA adsorption on supported charged lipid layers, DNA adsorption on oppositely charged cylindrical dendro-polymers, and DNA binding on globular histone proteins, respectively. In all these systems salt plays an important role, and some of the important features can already be obtained on the linear Debye-Hückel level. The second class comprises effective interactions between similarly charged objects. Here the main theme is to understand the experimental finding that similarly and highly charged bodies attract each other in the presence of multi-valent counterions. This is demonstrated using field-theoretic arguments as well as Monte-Carlo simulations for the case of two homogeneously charged bodies. Realistic surfaces, on the other hand, are corrugated and also exhibit modulated charge distributions, which is important for static properties such as the counterion-density distribution, but has even more pronounced consequences for dynamic properties such as the counterion mobility. More pronounced dynamic effects are obtained with highly condensed charged systems in strong electric fields. Likewise, an electrostatically collapsed highly charged polymer is unfolded and oriented in strong electric fields. All charged systems occur in water, and water by itself is not a very well understood material. At the end of this review, we give a very brief and incomplete account of the behavior of water at planar surfaces. The coupling between water structure and charge effects is largely unexplored, and a few directions for future research are sketched. On an even more nanoscopic level, we demonstrate using ab-initio methods that specific interactions between oppositely charged groups (which occur when their electron orbitals start to overlap) are important and cause ion-specific effects that have recently moved into the focus of interest.

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Section: Charged Plate In the Presence Of Saltmentioning

confidence: 97%

Section: Introductionmentioning

confidence: 99%

Statics and dynamics of strongly charged soft matter

Boroudjerdi¹,

Kim²,

Naji³

et al. 2005

Physics Reports

346

523

View full text Add to dashboard Cite

show abstract

“…9 Specifically, we describe the ARM region as an osmotic brush. 10 In other words, the equilibrium size of the layer is determined by the osmotic pressure of the counterions and the entropic elasticity of the ARMs.…”

Section: Entropic Elasticity Of Armsmentioning

confidence: 99%

Multishell Structures of Virus Coat Proteins

et al. 2010

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Under conditions of low ionic strength and a pH ranging between about 3.7 and 5.0, solutions of purified coat proteins of cowpea chlorotic mottle virus (CCMV) form spherical multishell structures in the absence of viral RNA. The outer surfaces of the shells in these structures are negatively charged, whereas the inner surfaces are positively charged due to a disordered cationic N-terminal domain of the capsid protein, the arginine-rich RNA-binding motif that protrudes into the interior. We show that the main forces stabilizing these multishells are counterion release combined with a lower charge density in the RNA-binding motif region of the outer shells due to their larger radii of curvature, arguing that these compensate for the outer shells not being able to adopt the smaller, optimal, radius of curvature of the inner shell. This explains why the structures are only stable at low ionic strengths at pHs for which the outer surface is negatively charged and why the larger outer shells are not observed separately in solution. We show how to calculate the free energy of shells of nonoptimal radius of curvature from the elastic properties of the native shell. The spacing between shells is determined mainly by the entropic elasticity of the RNA-binding motifs. Although we focus on CCMV multishells, we also predict the solution conditions under which multishells formed by CCMV coat protein mutants with a lower RNA-binding motif charge are stable, and we examine other viruses as well. We conclude that at a given surface charge density, the boundaries separating regions of stable multishells with different numbers of shells shift to lower ionic strengths upon either increasing the length of the RNAbinding motif, increasing the stiffness of the shells, or decreasing the charge per RNA-binding motif.

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“…P olymer brushes form when macromolecular chains are end-tethered to surfaces at high grafting densities 1,2 . The swelling and mutual steric repulsion of the polymers cause the chains to stretch and extend into the solvent, producing a molecular coating that can reduce non-specific interactions of the underlying surface with cells and biological macromolecules 3 .…”

mentioning

confidence: 99%

Stimuli-sensitive intrinsically disordered protein brushes

et al. 2014

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Grafting polymers onto surfaces at high density to yield polymer brush coatings is a widely employed strategy to reduce biofouling and interfacial friction. These brushes almost universally feature synthetic polymers, which are often heterogeneous and do not readily allow incorporation of chemical functionalities at precise sites along the constituent chains. To complement these synthetic systems, we introduce a biomimetic, recombinant intrinsically disordered protein that can assemble into an environment-sensitive brush. This macromolecule adopts an extended conformation and can be grafted to solid supports to form oriented protein brushes that swell and collapse dramatically with changes in solution pH and ionic strength. We illustrate the value of sequence specificity by using proteases with mutually orthogonal recognition sites to modulate brush height in situ to predictable values. This study demonstrates that stimuli-responsive brushes can be fabricated from proteins and introduces them as a new class of smart biomaterial building blocks.

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Polyelectrolyte Brushes

Cited by 393 publications

References 107 publications

Statics and dynamics of strongly charged soft matter

Statics and dynamics of strongly charged soft matter

Multishell Structures of Virus Coat Proteins

Stimuli-sensitive intrinsically disordered protein brushes

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