Complexation of oppositely charged polyelectrolytes: Effect of discrete charge distribution along the chain

Palyulin, Vladimir V.

doi:10.1103/physreve.81.041802

Cited by 29 publications

(30 citation statements)

References 18 publications

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“…The phenomenon of a collapse of a polymer network was first explicitly described by Tanaka in 1978 [199]. Since then much theoretical and experimental research has been devoted to this problem [188, 189,191,[200][201][202][203][204][205][206][207][208][209]212]. A c c e p t e d M a n u s c r i p t 54 the formation of a denser structure occurs.…”

Section: Effects Of Cohesive Interaction Strength Chain Length Charmentioning

confidence: 99%

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Pressure sensitive adhesives based on interpolymer complexes

Feldstein

Dormidontova

Khokhlov

2015

Progress in Polymer Science

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Section: Effects Of Cohesive Interaction Strength Chain Length Charmentioning

confidence: 99%

“…Page 53 of 227 A c c e p t e d M a n u s c r i p t 55 The effects of charge distributions along the chains of interactive polyelectrolytes are described in [191] and [212]. concentration [222].…”

Section: Figure 26mentioning

confidence: 99%

Pressure sensitive adhesives based on interpolymer complexes

Feldstein

Dormidontova

Khokhlov

2015

Progress in Polymer Science

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“…This approximation for the structure factor of charged monomers is generally used in the RPA consideration of PE complexation. [17][18][19][20]22,23 It is a reliable approximation for chains with the regular equidistant charge spacing when the adjacent ionic units are separated by f −1 − 1 uncharged monomers 21 (see Supporting Information). In what follows, we compute over the entire range of λ values, −1 ≤ λ ≤ 1, because λ = −1 corresponds to the important theoretical limit of homogeneously charged PEs.…”

Section: Acs Macro Lettersmentioning

confidence: 99%

Controlling Complex Coacervation via Random Polyelectrolyte Sequences

Rumyantsev

Jackson

et al. 2019

ACS Macro Lett.

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The utilization of chemical sequence control in polymeric materials is key to enabling material design on par with biomacromolecular systems. One important avenue for scalable sequence-controlled polymers leverages the random copolymerization of distinct monomers, with the statistical distribution of the monomeric sequence arising from reaction kinetics following a first-order Markov process. Here we utilize the framework of the random phase approximation (RPA) to develop a theory for the phase behavior of symmetric polyelectrolyte coacervates whose chemical sequences are dictated by simple statistical distributions. We find that a high charge “blockiness” within the random sequences favors the formation of denser and more salt-resistant coacervates while simultaneously increasing the width of the two-phase region. We trace these physical effects to the increased cooperativity of Coulomb interactions that results from increased charge blockiness in oppositely charged polyelectrolytes.

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“…33,34,36,37 In our group, fluctuations of polymer and charge densities were examined independently (discrete charge distribution), which allowed getting a general expression for the free energy unifying different limiting cases. 38 The RPA theory for rod-like polymer chains capable of liquid-crystalline ordering was developed in ref. [39][40][41][42].…”

Section: Introductionmentioning

confidence: 99%

Explicit description of complexation between oppositely charged polyelectrolytes as an advantage of the random phase approximation over the scaling approach

Rumyantsev

2017

Phys. Chem. Chem. Phys.

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A polyelectrolyte complex (PEC) of oppositely charged linear chains is considered within the Random Phase Approximation (RPA). We study the salt-free case and use the continuous model assuming a homogeneous distribution of the charges throughout the polyions. The RPA correction to the PEC free energy is renormalized via subtraction of polyion self-energy in order to find the correlation free energy of the complex. An analogous procedure is usually carried out in the case of the Debye-Hückel (DH) plasma (a gas of point-like ions), where the infinite self-energy of point-like charges is subtracted from the diverging RPA correction. The only distinction is that in the PEC both the RPA correction and chain self-energy of connected like charges are convergent. This renormalization allows us to demonstrate that the correlation free energy of the PEC is negative, as could be expected, while the scaling approach postulates rather than proving the negative sign of the energy of interactions between the blobs. We also demonstrate that the increasing concentration of oppositely charged polyions in the solution first results in the formation of neutral globules of the PEC consisting of two polyions as soon as the concentration reaches a certain threshold value, c, whereas solution macroscopic phase separation (precipitation of globules) occurs at a much higher concentration, c, c ≫ c. Partitioning of polyions between different states is calculated and analytical dependencies of c and c on the polyion length, degree of ionization and solvent polarity are found.

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Complexation of oppositely charged polyelectrolytes: Effect of discrete charge distribution along the chain

Cited by 29 publications

References 18 publications

Pressure sensitive adhesives based on interpolymer complexes

Pressure sensitive adhesives based on interpolymer complexes

Controlling Complex Coacervation via Random Polyelectrolyte Sequences

Explicit description of complexation between oppositely charged polyelectrolytes as an advantage of the random phase approximation over the scaling approach

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