Influence of anions on behavior of cationic polyelectrolyte poly(diallyldimethylammonium chloride) and its copolymer in aqueous solutions

Лезов, А. А.; Рогожин, В. Б.; Donets, Alexey V.; Лезова, А. А.; Gubarev, A. S.; Vlasov, Petr S.; Samokhvalova, S. A.; Polushina, G. E.; Polushin, S. G.; Цветков, Н. В.

doi:10.1016/j.molliq.2021.118369

Cited by 2 publications

(4 citation statements)

References 42 publications

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“…For the 3,3-I ionenes the inter-chain aggregation is indeed pronounced, 3,3-I ionene shows a significantly lower D NMR than all the other systems (roughly a factor of 2 lower) throughout the entire concentration range. This scenario is consistent with the evolution of viscosity (¥) of aqueous solutions of a neighbouring cationic PE, poly(diallyldimethylammonium), along the halide series [68]. Indeed, ¥ decreases between Cland Brsolutions of this PE (chains change from a rod-like to a more globular conformation), and the system becomes insoluble with I -(no Fdata are available in ref [68]).…”

Section: Resultssupporting

confidence: 77%

“…This scenario is consistent with the evolution of viscosity (¥) of aqueous solutions of a neighbouring cationic PE, poly(diallyldimethylammonium), along the halide series [68]. Indeed, ¥ decreases between Cland Brsolutions of this PE (chains change from a rod-like to a more globular conformation), and the system becomes insoluble with I -(no Fdata are available in ref [68]). We attach importance to the fact that 3,3-F ionenes show somewhat lower D NMR than Br-and Cl-ionenes, in the moderate to high c p range.…”

Section: Resultssupporting

confidence: 77%

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Ion-specific effects in polyelectrolyte solutions: chain-chain interactions, chain rigidity and dynamics

Hotton,

Sakhawoth,

Rollet

et al. 2024

Preprint

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Ion-specific effects in aqueous solutions of polyelectrolytes are addressed here. We focus on ionene cationic chains, featuring simple structure, absence of side-groups and very regular chain charge density. Ion-specific effects in ionene solutions are demonstrated using a series of monovalent (halide) counterions. The study combines both static and dynamic measurements by small angle neutron scattering, neutron spin echo and PFG-NMR. Ion-specific effects are a phenomenon at high polyelectrolyte concentration and the nature of the counterion is seen to influence drastically the ionene chain-chain interactions. The origin lies in the closer approach of large, highly polarisable counterions to the chain backbone, leading to more constricted counterion clouds. Equally affected is the local chain rigidity, as well as collective and self-diffusion coefficients at larger scales. Small, nonpolarizable, strongly hydrating counterions, here F− ions, lead to locally rigid chains. For such chains, the nm-scale collective dynamics as seen by neutron spin echo, is the fastest, while the self-diffusion seen at μm scale by PFG-NMR is the slowest. In other words, the loss of charge on the chain due to ion-specific counterion ”condensation” has the opposite effect on collective diffusion and self-diffusion of the chains.

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Section: Resultssupporting

confidence: 77%

Section: Resultssupporting

confidence: 77%

Ion-specific effects in polyelectrolyte solutions: chain-chain interactions, chain rigidity and dynamics

Hotton,

Sakhawoth,

Rollet

et al. 2024

Preprint

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“…Specifically, PDADMA–PSS PECs prepared with NaCl, NaBr, and NaNO 3 exhibited similar PDADMA concentrations of 53–54 mol %, but PECs prepared with NaI contained slightly more PDADMA at 57.6 mol %, as listed in Table S1. Elsewhere, we reported excess PDADMA for PECs prepared from NaCl solutions, which was ascribed to differences in the linear charge density and hydrophilicity between PSS and PDADMA, as well as the resulting counterion condensation …”

Section: Resultsmentioning

confidence: 99%

“…Elsewhere, we reported excess PDADMA for PECs prepared from NaCl solutions, 9 which was ascribed to differences in the linear charge density and hydrophilicity between PSS and PDADMA, as well as the resulting counterion condensation. 61 The doping level, which is related to the fraction of extrinsic ion pairs within the PEC, was estimated using elemental analysis via NAA and the preceding compositional analysis via NMR spectroscopy. Because of the asymmetric stoichiometry within the PECs, the doping levels for the polycation and polyanion will be dissimilar.…”

Section: Pec Composition and Doping Levelmentioning

confidence: 99%

Counter Anion Type Influences the Glass Transition Temperature of Polyelectrolyte Complexes

Lalwani,

Hellikson,

Batys

et al. 2024

Macromolecules

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Salt acts as a plasticizer in polyelectrolyte complexes (PECs), which impacts the physical, thermal, and mechanical properties, thus having implications in applications, such as drug delivery, energy storage, and smart coatings. Added salt disrupts polycation–polyanion intrinsic ion pairs, lowering a hydrated PEC’s glass transition temperature (T g). However, the relative influence of counterion type on the PEC’s T g is not well understood. Here, the effect of anion type (NaCl, NaBr, NaNO3, and NaI) on the T g of solid-like, hydrated PECs composed of poly(diallydimethylammonium) (PDADMA)–poly(styrenesulfonate) (PSS) is investigated. With increasing the chaotropic nature of the salt anion, the T g decreases. The relative differences are attributed to the doping level, the amount of bound water, the mobility of water molecules within the PECs, and the strength of interactions between the PEs. For all studied salt concentrations and salt types, the T g followed the scaling of −1/T g ≈ ln([IP]/[H2O]), in which [IP]/[H2O] is the ratio of intrinsic pairs to water. The scaling estimates that about 7 to 17% of the intrinsic ion pairs should be weakened for the PEC to partake in a glass transition. Put together, this study highlights that the T g in PECs is impacted by the salt anion, but the mechanism of the glass transition remains unchanged.

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Influence of anions on behavior of cationic polyelectrolyte poly(diallyldimethylammonium chloride) and its copolymer in aqueous solutions

Cited by 2 publications

References 42 publications

Ion-specific effects in polyelectrolyte solutions: chain-chain interactions, chain rigidity and dynamics

Ion-specific effects in polyelectrolyte solutions: chain-chain interactions, chain rigidity and dynamics

Counter Anion Type Influences the Glass Transition Temperature of Polyelectrolyte Complexes

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