Molecular theory of the electrostatic collapse of dipolar polymer gels

Budkov, Yu. A.; Kalikin, Nikolai N.; Kolesnikov, A. L.

doi:10.1039/d0cc08296a

Cited by 7 publications

(12 citation statements)

References 49 publications

(38 reference statements)

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“…Dumbbellshaped molecules functionalized with ionic liquids were proposed, e.g., as "hybrid" electrolyte for lithium-metal batteries 208 . Soft dumbbell particles with opposite charges [209][210][211][212] and their applications to dipolar liquids and gels can also be mentioned.…”

Section: B Physical Rationales and Further Discussionmentioning

confidence: 99%

Non-Gaussian, transiently anomalous, and ergodic self-diffusion of flexible dumbbells in crowded two-dimensional environments: Coupled translational and rotational motions

et al. 2021

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We employ Langevin-dynamics simulations to unveil non-Brownian and non-Gaussian center-ofmass self-diffusion of massive flexible dumbbell-shaped particles in crowded two-dimensional solutions. We also study the intra-dumbbell dynamics due to the relative motion of the two constituent elastically-coupled disks. Our main focus is on effects of the crowding fraction φ and the particle structure on the diffusion characteristics. We evaluate the time-averaged mean-squared displacement (TAMSD), the displacement probability-density function (PDF) and the displacement autocorrelation function (ACF) of the dimers. For the TAMSD at highly crowded conditions of dumbbells, e.g., we observe a transition from the short-time ballistic behavior, via an intermediate subdiffusive regime, to long-time Brownian-like spreading dynamics. The crowded system of dimers exhibits two distinct diffusion regimes distinguished by the scaling exponent of the TAMSD, the dependence of the diffusivity on φ, and the features of the displacement-ACF. We attribute these regimes to a crowding-induced transition from a viscous to a viscoelastic diffusion medium upon growing φ. We also analyze the relative motion in the dimers, finding that larger φ suppress their vibrations and yield strongly non-Gaussian PDFs of rotational displacements. For the diffusion coefficients D(φ) of translational and rotational motion of the dumbbells an exponential decay with φ for weak and a power-law D(φ) ∝ (φ − φ ) 2.4 for strong crowding is found. A comparison of simulation results with theoretical predictions for D(φ) is discussed and some relevant experimental systems are overviewed.

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Section: B Physical Rationales and Further Discussionmentioning

confidence: 99%

Non-Gaussian, transiently anomalous, and ergodic self-diffusion of flexible dumbbells in crowded two-dimensional environments: Coupled translational and rotational motions

et al. 2021

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Section: B Physical Rationales and Further Discussionmentioning

confidence: 99%

Non-Gaussian, transiently anomalous and ergodic self-diffusion of flexible dumbbells in crowded two-dimensional environments: coupled translational and rotational motions

Klett

Cherstvy

Shin

et al. 2021

Preprint

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We employ Langevin-dynamics simulations to unveil non-Brownian and non-Gaussian center-of-mass self-diffusion of massive flexible dumbbell-shaped particles in crowded two-dimensional solutions. We also study the intra-dumbbell dynamics due to the relative motion of the two constituent elastically-coupled disks. Our main focus is on effects of the crowding fraction φ and the particle structure on the diffusion characteristics. We evaluate the time-averaged mean-squared displacement (TAMSD), the displacement probability-density function (PDF) and the displacement autocorrelation function (ACF) of the dimers. For the TAMSD at highly crowded conditions of dumbbells, e.g., we observe a transition from the short-time ballistic behavior, via an intermediate subdiffusive regime, to long-time Brownian-like spreading dynamics. The crowded system of dimers exhibits two distinct diffusion regimes distinguished by the scaling exponent of the TAMSD, the dependence of the diffusivity on φ, and the features of the displacement-ACF. We attribute these regimes to a crowding-induced transition from a viscous to a viscoelastic diffusion medium upon growing φ. We also analyze the relative motion in the dimers, finding that larger φ suppress their vibrations and yield strongly non-Gaussian PDFs of rotational displacements. For the diffusion coefficients D(φ) of translational and rotational motion of the dumbbells an exponential decay with φ for weak and a power-law D(φ) ∝ (φ - φ*)2.4 for strong crowding is found. A comparison of simulation results with theoretical predictions for D(φ) is discussed and some relevant experimental systems are overviewed.

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“…For instance, as shown in Figure 2B, the gel column began to shrink near the anode only 1 h after applying 5 V, and approximately half of the gel column was distorted after 12 h. The gel distortion prevented long-time observations even under applied lower voltages. Thus, the Frontiers in Physics frontiersin.org observation time in the current experiments, including experiments with cyclic alternating voltages, was limited up to 60 h. It should be noted that gel distortion or shrinkage under electric fields has been observed in various systems [22][23][24], and related theoretical approaches are being developed [25]; however, the details of the observed distortion are still unclear.…”

Section: Precipitation Patterns Under Constant Voltagesmentioning

confidence: 94%

Periodic band formation of Fe(OH)3 precipitate through reaction–diffusion–reaction processes

Hayashi

2023

Front. Phys.

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This paper reports a new class of periodic banding of Fe(OH)3 precipitate through reaction–diffusion–reaction (RDR) processes in agarose gel sandwiched between two metal rods (Ti and Fe) with cyclic alternating voltages. In the RDR processes, electrochemical reactions at metal rods to generate reactant ions, diffusion of the ions influenced by the electric field in the gel, and reactions of the ions to form precipitates were coupled to generate periodic bands of Fe(OH)3 precipitates at the cathode side. The banding morphologies, spatial Fe distribution, and microscopic morphologies of the precipitates were investigated by visual inspection, Fe Kα intensity distribution measurements, and scanning electron microscopy observations. The periodic banding strongly depended on the applied voltages, the periods for voltage alternation, the cycle number (NC), and the length of the gel column. Periodic bands resembling Liesegang bands were most clearly observed with high reproducibility for 50 mm gel columns under the applied cyclic alternating voltages of 3 and 1 V for 1 and 4 h, respectively. The number of the periodic bands formed in this system was generally given by NC—NC1 + 1, where NC1 is the cycle number where the first band emerges. These periodic bands contained significant amounts of Fe atoms that were almost uniformly distributed in the agarose gel, strongly supporting the formation of gelatinous Fe(OH)3 precipitates in the bands.

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Molecular theory of the electrostatic collapse of dipolar polymer gels

Abstract: We develop a new quantitative molecular theory of liquid-phase dipolar polymer gels. We model monomer units of the polymer network as a couple of charged sites separated by a fluctuating...

Cited by 7 publications

References 49 publications

Non-Gaussian, transiently anomalous, and ergodic self-diffusion of flexible dumbbells in crowded two-dimensional environments: Coupled translational and rotational motions

Non-Gaussian, transiently anomalous, and ergodic self-diffusion of flexible dumbbells in crowded two-dimensional environments: Coupled translational and rotational motions

Non-Gaussian, transiently anomalous and ergodic self-diffusion of flexible dumbbells in crowded two-dimensional environments: coupled translational and rotational motions

Periodic band formation of Fe(OH)3 precipitate through reaction–diffusion–reaction processes

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