Stimuli-responsive adsorption of poly(acrylic acid) onto silver nanoparticles: Role of polymer chain length and degree of ionization

Kyrychenko, Alexander; Blazhynska, Margaret M.; Slavgorodska, Maria V.; Kalugin, Oleg N.

doi:10.1016/j.molliq.2018.11.130

Cited by 25 publications

(47 citation statements)

References 85 publications

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“…Simulations at different pH are performed by varying the degree of deprotonation ( f ) of PAA20 defined as the ratio of COO − units to total number of COO − and COOH units, which is determined using the Henderson–Hasselbalch equation

f = 1 / (1 + 10^{pKa - pH})

with

pKa = 6.27

f=0.05 and

f = 0.6

cases simulated in this study correspond to

pH = 5

(representative of gastric fluid) and

pH = 6.5

(representative of intestinal fluid), respectively .…”

Section: Methodsmentioning

confidence: 99%

Mimicking the Dissolution Mechanisms of pH‐Responsive Drug Release Formulations in Atomistic MD Simulations

Katiyar

Jha

2019

Advcd Theory and Sims

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Atomistic molecular dynamics (MD) simulations of poly(acrylic acid) (PAA)-doxorubicin (DOX) formulations dissolved in water are performed to mimic three common drug release mechanisms of pH-responsive polymer-drug formulations. The effect of formulation matrix swelling in a reverse manner is mimicked by performing sequential water removal during the MD simulations followed by re-equilibration, until an amorphous state devoid of water is achieved. Then, MD simulations for different PAA and DOX compositions are performed that mimic the different dissolution stages of an eroding and non-swellable matrix, respectively. An Arrhenius law dependence of diffusion coefficient is established on the changes in PAA-DOX interaction energy, which in turn shows power law dependence on concentration. Together, the three sets of simulations demonstrate how the molecular-level interactions (e.g., hydrogen bonding, ionic complexation) drive macroscopic changes in the drug release behavior described in terms of drug/water diffusion coefficients, and also highlight the potential of atomistic simulations in the prediction of drug release behavior of novel polymer-drug formulations using the diffusion coefficients obtained in atomistic simulations.

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f = 1 / (1 + 10^{pKa - pH})

with

pKa = 6.27

f=0.05 and

f = 0.6

cases simulated in this study correspond to

pH = 5

(representative of gastric fluid) and

pH = 6.5

(representative of intestinal fluid), respectively .…”

Section: Methodsmentioning

confidence: 99%

Mimicking the Dissolution Mechanisms of pH‐Responsive Drug Release Formulations in Atomistic MD Simulations

Katiyar

Jha

2019

Advcd Theory and Sims

View full text Add to dashboard Cite

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“…In both models, the repulsion and dispersion terms of nonbonded interactions between silver atoms were computed by using the Lennard-Jones 12−6 potential energy function (5), which describes the dependence of the potential interaction energy V LJ (r ij ) of two silver atoms as a function of the interatomic distance. The nonbonded interaction parameters Ag-Ag were based on non-polarizable INTERFACE-FF [31,36,49] and were validated in our recent works [8,19,24,37]. For MD simulations in vacuum, no of any rigid bonds and restraints were applied between silver atoms, so that the silver core crystalline structure was maintained by the Ag-Ag nonbonded LJ interactions.…”

Section: Molecular Dynamics Simulation Setupmentioning

confidence: 99%

“…The initial values of q and l 0 were taken from the original study [44]. The nonbonded interaction parameters Ag-Ag σ=0.2964 nm and ε=19.05865 kJ/mol were taken from our recent works [9,24]. However, both parameters σ and ε were assigned to zero for the virtual site.…”

Section: Molecular Dynamics Simulation Setupmentioning

confidence: 99%

“…Atomic-scale theoretical methods can provide important insight to the solution-phase synthesis of silver nanostructures that involves the seeded growth [6][7] and the morphological stability [8][9], as well as adsorption of stabilizing agents and solvent molecules onto inorganic metal nanocrystals [10][11][12]. Numerous MD simulation studies of silver and gold nanoparticles protected by organic ligand monolayers [13][14][15][16][17][18], synthetic polymers [19][20][21][22][23][24][25][26], and peptides [27][28][29][30] have been conducted in the last decade.…”

Section: Introductionmentioning

confidence: 99%

“…https://doi.org/10.26565/2220-637X-2019- The main goal of our study is the implementation of the polarizable Ag model to the existing nonpolarizable FF, which were recently used for MD simulations of silver nanoparticles and interfaces [8,19,24,[37][38]. Besides, the influence of polarization effects on the adsorption of water molecules and ions at the silver/water interface is considered.…”

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Polarizable force field for molecular dynamics simulations of silver nanoparticles

2019

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Contact of silver metal surfaces with water, ions and organic ligands experiences induced charges, leading to attractive polarization. These forces play an important role at inorganic/organic interfaces and complement other non-bonded surface interactions. Despite the importance of these interactions, it, however, remains difficult to implement polarization effects to classical molecular dynamics (MD) simulations. In this contribution, we first present an overview of two popular polarizable models, such as Drude oscillator and the rigid rod model, which are utilized to mimic the polarizability of bulk metals. Second, we implemented the rigid rod model to the polarizable force field (FF) for a silver atom, which was further adapted for atomistic MD simulations of silver nanoparticles (AgNPs) composed of 1397 atoms. In our model, induced charge polarization is represented by the displacement of a charge-carrying virtual site attached rigidly to an original Ag atom. To explore the role of polarization, we compared the performance of the classical nonpolarizable FF and the new polarizable model in the MD simulations of adsorption of water and ions onto quasi-spherical AgNP and the flat crystalline silver surface. The analysis of the radial distribution function of Ag-Ag atoms demonstrated that the introduction of the polarization effect had minor effects on face-centered cubic (fcc) packing of silver atoms of bare and water-solvated AgNPs. We found that the polarizable FF causes some increase in attractive interactions between the silver surface and water molecules and Na+ ions. As a crucial test of the developed polarizable model, the structure of adsorbed interfacial water molecules was analyzed. Our data suggest that the environment-induced polarization of the silver surface contributes significantly to the structure of adsorbed interfacial water layers and it also plays an important role in the adsorption of positive ions. However, it was also found out that the polarization effect has a rather short-range effect, so that a minor contribution of silver polarization was seen for adsorption of water molecules and ions from distant solvation shells.

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Understanding the pore structure evolution of polyethylene separator with dissipative particle dynamics simulation

Wang,

Wu,

et al. 2023

Polymer Engineering & Sci

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The commercialized lithium‐ion battery separators are mass‐produced by mixing ultra‐high molecular weight polyethylene (UHMWPE) and paraffin oil (PO). The dissipative particle dynamics method is utilized to investigate the extrinsic factors (shear rate and cooling rate) and the intrinsic factors (the molecular chain length) on the microstructure of the UHMWPE‐PO mixture. For the mixture with UHMWPE possessing the same chain length, the high shear rate promoted a lower porosity (~28%) and smaller pores. In contrast, the slow shearing led to a high porosity (~40%) and larger pores. For the mixture with UHMWPE possessing short and long chains, the shear rate hardly affects the porosity and the pore size: the porosity was kept at ~30%, and the pore size was reduced by ~35% compared to the model with the same‐chain‐length UHMWPE. The cooling rate after shearing is the dominant factor in determining the porosity and pore size: the fast cooling raised the porosity by ~33% but hardly increased the pore size, while the slow cooling raised the porosity by ~74%, and the pore size by ~105%. The current study provided a deep understanding of the pore structure evolution in separator processing.Highlights The effects of processing parameters on the pore structures are numerically illustrated. MD simulation and rheometer measurement assist DPD interaction parameters calibration for UHMWPE and PO. The low shear rate leads to a higher porosity and pore size. At the high shear rate, short UHMWPE chains reduce porosity but do not increase pore size. The fast‐cooling process slightly increases the porosity while keeping the pore size.

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Stimuli-responsive adsorption of poly(acrylic acid) onto silver nanoparticles: Role of polymer chain length and degree of ionization

Cited by 25 publications

References 85 publications

Mimicking the Dissolution Mechanisms of pH‐Responsive Drug Release Formulations in Atomistic MD Simulations

Mimicking the Dissolution Mechanisms of pH‐Responsive Drug Release Formulations in Atomistic MD Simulations

Polarizable force field for molecular dynamics simulations of silver nanoparticles

Understanding the pore structure evolution of polyethylene separator with dissipative particle dynamics simulation

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