Explicit Ion Effects on the Charge and Conformation of Weak Polyelectrolytes

Rathee, Vikramjit S.; Sidky, Hythem; Sikora, Benjamin J.; Whitmer, Jonathan K.

doi:10.3390/polym11010183

Cited by 32 publications

(43 citation statements)

References 101 publications

(145 reference statements)

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“…Moreover, they were not concerned with multi-component reaction equilibria at which some of the reacting species have very low concentrations or with situations where some reactive species might not be exchanged. Recent simulations of weak polyelectrolytes by Rathee et al 60,61 also closely resemble our method. However, their coupling to the multi-component reservoir was incomplete, which may lead to artifacts under specic conditions.…”

Section: Introductionsupporting

confidence: 71%

“…However, this method becomes highly inecient when the number of particles of one or more reacting species is low. This limitation concerns especially H + and OH ions when simulating acid-base equilibria close to pH = 7, because their concentration is very low 58,60,61 . Thus, combining these methods for simulating reactive systems coupled to a reservoir is a complicated task.…”

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Grand-reaction method for simulations of ionization equilibria coupled to ion partitioning

Landsgesell¹,

Rud²,

Hebbeker³

et al. 2020

Preprint

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We developed a new method for coarse-grained simulations of acid-base equilibria in a system coupled to a reservoir at a given pH and concentration of added salt, that we term the Grand-reaction method. More generally, it can be used for simulations of any reactive system coupled to a reservoir of a known composition. Conceptually, it can be regarded as an extension of the reaction ensemble, combining explicit simulations of reactions within the system and Grand-canonical exchange of particles with the reservoir. To demonstrate its strength, we applied our method to a solution of weak polyelectrolytes in equilibrium with a reservoir. Our results show that the ionization and swelling of a weak polyelectrolyte are affected by the Donnan effect due to the partitioning of ions and by the polyelectrolyte effect due to electrostatic repulsion along the chain. Both effects lead to a similar shift in ionization and swelling as a function of pH; albeit for different physical reasons. By comparison with published results, we showed that neglecting one or the other effect may lead to erroneous predictions or misinterpretations of results. In contrast, the Grand-reaction method accounts for both effects on the results and allows us to quantify them. Finally, we outline possible extensions and generalizations of the method and provide a set of guidelines for its safe application by a broad community of users.<br><div><br></div>

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Section: Introductionsupporting

confidence: 71%

Section: Introductionmentioning

confidence: 99%

Grand-reaction method for simulations of ionization equilibria coupled to ion partitioning

Landsgesell¹,

Rud²,

Hebbeker³

et al. 2020

Preprint

View full text Add to dashboard Cite

show abstract

“…In spite of the fact that weak PE systems can also offer many such advantages, only a few works have been reported. For instance, the responsiveness to instantaneous environmental changes (e.g., pH, ionic strength and temperature) come from the physical proximity of weakly charged groups to each other [21]. The effect of PE density can be particularly promi-nent when there are many charged groups present in the system.…”

Section: Review Introductionmentioning

confidence: 99%

Multilayer capsules made of weak polyelectrolytes: a review on the preparation, functionalization and applications in drug delivery

Sharma¹,

Sundaramurthy²

2020

Beilstein J. Nanotechnol.

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Multilayer capsules have been of great interest for scientists and medical communities in multidisciplinary fields of research, such as drug delivery, sensing, biomedicine, theranostics and gene therapy. The most essential attributes of a drug delivery system are considered to be multi-functionality and stimuli responsiveness against a range of external and internal stimuli. Apart from the highly explored strong polyelectrolytes, weak polyelectrolytes offer great versatility with a highly controllable architecture, unique stimuli responsiveness and easy tuning of the properties for intracellular delivery of cargo. This review describes the progress in the preparation, functionalization and applications of capsules made of weak polyelectrolytes or their combination with biopolymers. The selection of a sacrificial template for capsule formation, the driving forces involved, the encapsulation of a variety of cargo and release based on different internal and external stimuli have also been addressed. We describe recent perspectives and obstacles of weak polyelectrolyte/biopolymer systems in applications such as therapeutics, biosensing, bioimaging, bioreactors, vaccination, tissue engineering and gene delivery. This review gives an emerging outlook on the advantages and unique responsiveness of weak polyelectrolyte based systems that can enable their widespread use in potential applications.

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“…et al60,61 published two articles where they investigated weak polyelectrolytes in equilibrium with two independent reservoirs; one consisting of a salt solution (NaCl or MgSO 4 at various concentrations) and the other consisting of KOH at c = 10 −2.7 M, to ensure a constant value of pH = 11.3. They varied the polymer ionization by varying the reaction constant of the ionization reaction.…”

mentioning

confidence: 99%

Grand-reaction method for simulations of ionization equilibria coupled to ion partitioning

Landsgesell¹,

Rud²,

Hebbeker³

et al. 2020

Preprint

View full text Add to dashboard Cite

We developed a new method for coarse-grained simulations of acid-base equilibria in a system coupled to a reservoir at a given pH and concentration of added salt, that we term the Grand-reaction method. More generally, it can be used for simulations of any reactive system coupled to a reservoir of a known composition. Conceptually, it can be regarded as an extension of the reaction ensemble, combining explicit simulations of reactions within the system and Grand-canonical exchange of particles with the reservoir. To demonstrate its strength, we applied our method to a solution of weak polyelectrolytes in equilibrium with a reservoir. Our results show that the ionization and swelling of a weak polyelectrolyte are aected by the Donnan eect due to the partitioning of ions and by the polyelectrolyte eect due to electrostatic repulsion along the chain. Both eects lead to a similar shift in ionization and swelling as a function of pH; albeit for dierent physical reasons. By comparison with published results, 1 we showed that neglecting one or the other eect may lead to erroneous predictions or misinterpretations of results. In contrast, the Grand-reaction method accounts for both eects on the results and allows us to quantify them. Finally, we outline possible extensions and generalizations of the method and provide a set of guidelines for its safe application by a broad community of users.

show abstract

Explicit Ion Effects on the Charge and Conformation of Weak Polyelectrolytes

Cited by 32 publications

References 101 publications

Grand-reaction method for simulations of ionization equilibria coupled to ion partitioning

Grand-reaction method for simulations of ionization equilibria coupled to ion partitioning

Multilayer capsules made of weak polyelectrolytes: a review on the preparation, functionalization and applications in drug delivery

Grand-reaction method for simulations of ionization equilibria coupled to ion partitioning

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