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Article ; Online: Coarse-Grained Model Incorporating Short- and Long-Range Effective Potentials for the Fast Simulation of Micelle Formation in Solutions of Ionic Surfactants.

Peroukidis, Stavros D / Stott, Ian P / Mavrantzas, Vlasis G

The journal of physical chemistry. B

2022 Volume 126, Issue 29, Page(s) 5555–5569

Abstract: A coarse-grained model comprising short- and long-range effective potentials, parametrized with the iterative Boltzmann inversion (IBI) method, is presented for capturing micelle formation in aqueous solutions of ionic surfactants using as a model system ...

Abstract	A coarse-grained model comprising short- and long-range effective potentials, parametrized with the iterative Boltzmann inversion (IBI) method, is presented for capturing micelle formation in aqueous solutions of ionic surfactants using as a model system sodium dodecyl sulfate (SDS). In the coarse-grained (CG) model, each SDS molecule is represented as a sequence of four beads while each water molecule is modeled as a single bead. The proposed CG scheme involves ten potential energy functions: four of them describe bonded interactions and control the distribution functions of intramolecular degrees of freedom (bond lengths, valence angles, and dihedrals) along an SDS molecule while the other six account for intermolecular interactions between pairs of SDS and water beads and control the radial distribution functions. The nonbonded effective potentials between coarse-grained SDS molecules extend up to about 12 nm and capture structural and morphological features of the micellar solution both at short and long distances. The long-range component of these potentials, in particular, captures correlations between surfactant molecules belonging to different micelles and is essential to describe ordering associated with micelle formation. A new strategy is introduced for determining the effective potentials through IBI by using information (target distribution functions) extracted from independent atomistic simulations of a micellar reference system (a salt-free SDS solution at total surfactant concentration
MeSH term(s)	Micelles ; Molecular Dynamics Simulation ; Surface-Active Agents ; Temperature ; Water/chemistry
Chemical Substances	Micelles ; Surface-Active Agents ; Water (059QF0KO0R)
Language	English
Publishing date	2022-07-15
Publishing country	United States
Document type	Journal Article ; Research Support, Non-U.S. Gov't
ISSN	1520-5207
ISSN (online)	1520-5207
DOI	10.1021/acs.jpcb.2c02751
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: Local density dependent potentials for an underlying van der Waals equation of state: A simulation and density functional theory analysis.

O'Connor, James P D / Cook, Joanne L / Stott, Ian P / Masters, Andrew J / Avendaño, Carlos

The Journal of chemical physics

2023 Volume 159, Issue 19

Abstract: There is an ever increasing use of local density dependent potentials in the mesoscale modeling of complex fluids. Questions remain, though, about the dependence of the thermodynamic and structural properties of such systems on the cutoff distance used ... ...

Abstract	There is an ever increasing use of local density dependent potentials in the mesoscale modeling of complex fluids. Questions remain, though, about the dependence of the thermodynamic and structural properties of such systems on the cutoff distance used to calculate these local densities. These questions are particularly acute when it comes to the stability and structure of the vapor/liquid interface. In this article, we consider local density dependent potentials derived from an underlying van der Waals equation of state. We use simulation and density functional theory to examine how the bulk thermodynamic and interfacial properties vary with the cutoff distance, rc, used to calculate the local densities. We show quantitatively how the simulation results for bulk thermodynamic properties and vapor-liquid equilibrium approach the van der Waals limit as rc increases and demonstrate a scaling law for the radial distribution function in the large rc limit. We show that the vapor-liquid interface is stable with a well-defined surface tension and that the interfacial density profile is oscillatory, except for temperatures close to critical. Finally, we show that in the large rc limit, the interfacial tension is proportional to rc and, therefore, unlike the bulk thermodynamic properties, does not approach a constant value as rc increases. We believe that these results give new insights into the properties of local density dependent potentials, in particular their unusual interfacial behavior, which is relevant for modeling complex fluids in soft matter.
Language	English
Publishing date	2023-10-02
Publishing country	United States
Document type	Journal Article
ZDB-ID	3113-6
ISSN	1089-7690 ; 0021-9606
ISSN (online)	1089-7690
ISSN	0021-9606
DOI	10.1063/5.0171331
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Article: Coarse-Grained Model Incorporating Short- and Long-Range Effective Potentials for the Fast Simulation of Micelle Formation in Solutions of Ionic Surfactants

Peroukidis, Stavros D. / Stott, Ian P. / Mavrantzas, Vlasis G.

Journal of physical chemistry. 2022 July 15, v. 126, no. 29

2022

Abstract	A coarse-grained model comprising short- and long-range effective potentials, parametrized with the iterative Boltzmann inversion (IBI) method, is presented for capturing micelle formation in aqueous solutions of ionic surfactants using as a model system sodium dodecyl sulfate (SDS). In the coarse-grained (CG) model, each SDS molecule is represented as a sequence of four beads while each water molecule is modeled as a single bead. The proposed CG scheme involves ten potential energy functions: four of them describe bonded interactions and control the distribution functions of intramolecular degrees of freedom (bond lengths, valence angles, and dihedrals) along an SDS molecule while the other six account for intermolecular interactions between pairs of SDS and water beads and control the radial distribution functions. The nonbonded effective potentials between coarse-grained SDS molecules extend up to about 12 nm and capture structural and morphological features of the micellar solution both at short and long distances. The long-range component of these potentials, in particular, captures correlations between surfactant molecules belonging to different micelles and is essential to describe ordering associated with micelle formation. A new strategy is introduced for determining the effective potentials through IBI by using information (target distribution functions) extracted from independent atomistic simulations of a micellar reference system (a salt-free SDS solution at total surfactant concentration cT equal to 103 mM, temperature T equal to 300 K, and pressure P equal to 1 atm) obtained through a multiscale approach described in an earlier study. It employs several optimization steps for bonded and nonbonded interactions and a gradual parametrization of the short- and long-range components of the latter, followed by reparametrization of the bonded ones. The proposed CG model can reproduce remarkably accurately the microstructure and morphology of the reference system within only a few hours of computational time. It is therefore very promising for future studies of structural and morphological behavior of various liquid surfactant formulations.
Keywords	liquids ; micelles ; microstructure ; models ; potential energy ; sodium dodecyl sulfate ; temperature
Language	English
Dates of publication	2022-0715
Size	p. 5555-5569.
Publishing place	American Chemical Society
Document type	Article
ISSN	1520-5207
DOI	10.1021/acs.jpcb.2c02751
Database	NAL-Catalogue (AGRICOLA)

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Article: Analytical modeling of micelle growth. 4. Molecular thermodynamics of wormlike micelles from ionic surfactants: Theory vs. experiment

Danov, Krassimir D / Kralchevsky, Peter A / Stanimirova, Rumyana D / Stoyanov, Simeon D / Cook, Joanne L / Stott, Ian P

Journal of colloid and interface science. 2021 Feb. 15, v. 584

2021

Abstract: The aggregation number and length of spherocylindrical (rodlike, wormlike) micelles in solutions of an ionic surfactant and salt can be predicted knowing the molecular parameters and the input concentrations of the species. This can be achieved by ... ...

Abstract	The aggregation number and length of spherocylindrical (rodlike, wormlike) micelles in solutions of an ionic surfactant and salt can be predicted knowing the molecular parameters and the input concentrations of the species. This can be achieved by upgrading the quantitative molecular thermodynamic model from the previous parts of this series with an expression for the electrostatic component of micelle scission energy that is the excess free energy of the spherical endcaps with respect to the cylindrical part of the micelle.The thermodynamics of micellization is extended to the case of multicomponent system, which may contain several surfactants (both ionic and nonionic) and salts, taking into account the effect of counterion binding in the Stern layer on the micellar surface. Furthermore, the considerations are focused on a system that consists of single ionic surfactant plus salt.Excellent agreement was achieved between the theoretical model and experimental data for wormlike micelles from anionic and cationic surfactants at various concentrations of salt and temperatures. In accord with the experimental observations, at high salt concentrations, the model predicts loss of chemical equilibrium between the endcaps and cylindrical part of the wormlike micelles, which implies transition to self-assemblies of other, e.g. branched, morphology or the onset of crystallization and phase separation.
Keywords	Gibbs free energy ; chemical equilibrium ; cleavage (chemistry) ; crystallization ; energy ; micelles ; separation ; theoretical models ; thermodynamic models
Language	English
Dates of publication	2021-0215
Size	p. 561-581.
Publishing place	Elsevier Inc.
Document type	Article
Note	NAL-AP-2-clean
ZDB-ID	241597-5
ISSN	1095-7103 ; 0021-9797
ISSN (online)	1095-7103
ISSN	0021-9797
DOI	10.1016/j.jcis.2020.10.004
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Article: Analytical modeling of micelle growth. 3. Electrostatic free energy of ionic wormlike micelles – Effects of activity coefficients and spatially confined electric double layers

Danov, Krassimir D / Kralchevsky, Peter A / Stoyanov, Simeon D / Cook, Joanne L / Stott, Ian P

Journal of colloid and interface science. 2021 Jan. 01, v. 581

2021

Abstract: Hypotheses: To correctly predict the aggregation number and size of wormlike micelles from ionic surfactants, the molecular-thermodynamic theory has to calculate the free energy per molecule in the micelle with accuracy better than 0.01 kT, which is a ... ...

Abstract	Hypotheses: To correctly predict the aggregation number and size of wormlike micelles from ionic surfactants, the molecular-thermodynamic theory has to calculate the free energy per molecule in the micelle with accuracy better than 0.01 kT, which is a serious challenge. The problem could be solved if the effects of mutual confinement of micelle counterion atmospheres, as well as the effects of counterion binding, surface curvature and ionic interactions in the electric double layer (EDL), are accurately described.Theory: The electric field is calculated using an appropriate cell model, which takes into account the aforementioned effects. Expressions for the activity coefficients have been used, which vary across the EDL and describe the electrostatic, hard sphere, and specific interactions between the ions. New approach for fast numerical calculation of the electrostatic free energy is developed.Findings: The numerical results demonstrate the variation of quantities characterizing the EDL of cylindrical and spherical micelles with the rise of electrolyte concentration. The effect of activity coefficients leads to higher values of the free energy per surfactant molecule in the micelle as compared with the case of neglected ionic interactions. The results are essential for the correct prediction of the size of wormlike micelles from ionic surfactants. This study can be extended to mixed micelles of ionic and nonionic surfactants for interpretation of the observed synergistic effects.
Keywords	Gibbs free energy ; electric field ; electrostatic interactions ; ionic surfactants ; ions ; micelles ; models ; nonionic surfactants ; prediction ; synergism
Language	English
Dates of publication	2021-0101
Size	p. 262-275.
Publishing place	Elsevier Inc.
Document type	Article
ZDB-ID	241597-5
ISSN	1095-7103 ; 0021-9797
ISSN (online)	1095-7103
ISSN	0021-9797
DOI	10.1016/j.jcis.2020.07.059
Database	NAL-Catalogue (AGRICOLA)

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Article ; Online: Quantitative Prediction of the Structure and Viscosity of Aqueous Micellar Solutions of Ionic Surfactants: A Combined Approach Based on Coarse-Grained MARTINI Simulations Followed by Reverse-Mapped All-Atom Molecular Dynamics Simulations.

Peroukidis, Stavros D / Tsalikis, Dimitrios G / Noro, Massimo G / Stott, Ian P / Mavrantzas, Vlasis G

Journal of chemical theory and computation

2020 Volume 16, Issue 5, Page(s) 3363–3372

Abstract: We address the problem of the quantitative prediction of micelle formation in dilute aqueous solutions of ionic surfactants using sodium dodecyl sulfate (SDS) as a model system through a computational approach that involves three steps: (a) execution of ... ...

Abstract	We address the problem of the quantitative prediction of micelle formation in dilute aqueous solutions of ionic surfactants using sodium dodecyl sulfate (SDS) as a model system through a computational approach that involves three steps: (a) execution of coarse-grained simulations based on the MARTINI force field (with slightly modified parameters to afford the formation of large micelles); (b) reverse mapping of the final self-assembled coarse-grained configuration into an all-atom configuration; and (c) final relaxation of this all-atom configuration through short-time (on the order of a few tens of nanoseconds), detailed isothermal-isobaric molecular dynamics simulations using the CHARMM36 force field. For a given concentration of the solution in SDS molecules, the modified MARTINI-based coarse-grained simulations lead to the formation of large micelles characterized by mean aggregation numbers above the experimentally observed ones. However, by reintroducing the detailed chemical structure through a strategy that solves a well-defined geometric problem and re-equilibrating, these large micellar aggregates quickly dissolve to smaller ones and equilibrate to sizes that perfectly match the average micelle size measured experimentally at the given surfactant concentration. From the all-atom molecular dynamics simulations, we also deduce the surfactant diffusivity
Language	English
Publishing date	2020-04-23
Publishing country	United States
Document type	Journal Article
ISSN	1549-9626
ISSN (online)	1549-9626
DOI	10.1021/acs.jctc.0c00229
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: Analytical modeling of micelle growth. 3. Electrostatic free energy of ionic wormlike micelles - Effects of activity coefficients and spatially confined electric double layers.

Danov, Krassimir D / Kralchevsky, Peter A / Stoyanov, Simeon D / Cook, Joanne L / Stott, Ian P

Journal of colloid and interface science

2020 Volume 581, Issue Pt A, Page(s) 262–275

Abstract	Hypotheses: To correctly predict the aggregation number and size of wormlike micelles from ionic surfactants, the molecular-thermodynamic theory has to calculate the free energy per molecule in the micelle with accuracy better than 0.01 kT, which is a serious challenge. The problem could be solved if the effects of mutual confinement of micelle counterion atmospheres, as well as the effects of counterion binding, surface curvature and ionic interactions in the electric double layer (EDL), are accurately described. Theory: The electric field is calculated using an appropriate cell model, which takes into account the aforementioned effects. Expressions for the activity coefficients have been used, which vary across the EDL and describe the electrostatic, hard sphere, and specific interactions between the ions. New approach for fast numerical calculation of the electrostatic free energy is developed. Findings: The numerical results demonstrate the variation of quantities characterizing the EDL of cylindrical and spherical micelles with the rise of electrolyte concentration. The effect of activity coefficients leads to higher values of the free energy per surfactant molecule in the micelle as compared with the case of neglected ionic interactions. The results are essential for the correct prediction of the size of wormlike micelles from ionic surfactants. This study can be extended to mixed micelles of ionic and nonionic surfactants for interpretation of the observed synergistic effects.
Language	English
Publishing date	2020-07-25
Publishing country	United States
Document type	Journal Article
ZDB-ID	241597-5
ISSN	1095-7103 ; 0021-9797
ISSN (online)	1095-7103
ISSN	0021-9797
DOI	10.1016/j.jcis.2020.07.059
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: Microstructural and thermodynamic characterization of wormlike micelles formed by polydisperse ionic surfactant solutions.

Flores, Stephen L / Mu, Junju / Cabry, Christopher P / Peterson, Joseph / De Hert, Sergio Carrillo / Morrison, Lisa / Stott, Ian P / Cook, Joanne L / Masters, Andrew J / Hardacre, Christopher / Avendaño, Carlos

The Journal of chemical physics

2023 Volume 159, Issue 5

Abstract: For industrial applications of self-assembled wormlike micelles, measurement and characterization of a micellar material's microstructure and rheology are paramount for the development and deployment of new high-performing and cost-effective formulations. ...

Abstract	For industrial applications of self-assembled wormlike micelles, measurement and characterization of a micellar material's microstructure and rheology are paramount for the development and deployment of new high-performing and cost-effective formulations. Within this workflow, there are significant bottlenecks associated with experimental delays and a lack of transferability of results from one chemistry to another. In this work, we outline a process to predict microscopic and thermodynamic characteristics of wormlike micelles directly from rheological data by combining a more robust and efficient fitting algorithm with a recently published constitutive model called the Toy Shuffling model [J. D. Peterson and M. E. Cates, J. Rheol. 64, 1465-1496 (2020) and J. D. Peterson and M. E. Cates, J. Rheol. 65, 633-662 (2021)]. To support this work, linear rheology measurements were taken for 143 samples comprising a common base formulation of commercial sodium lauryl ether sulfate, cocamidopropyl betaine, and salt (NaCl). The steady state zero shear viscosity evident in linear rheology was measured in duplicate via direct steady and oscillatory shear experiments. Fitting the collected data to the model, we found trends in the microstructural and thermodynamic characteristics that agree with molecular dynamics simulations. These trends validate our new perspective on the parameters that inform the study of the relationship between chemical formulation and rheology. This work, when implemented at scale, can potentially be used to inform and test strategies for predicting self-assembled micellar structures based on chemical formulation.
Language	English
Publishing date	2023-08-01
Publishing country	United States
Document type	Journal Article
ZDB-ID	3113-6
ISSN	1089-7690 ; 0021-9606
ISSN (online)	1089-7690
ISSN	0021-9606
DOI	10.1063/5.0153746
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Article ; Online: Analytical modeling of micelle growth. 3. Electrostatic free energy of ionic wormlike micelles – Effects of activity coefficients and spatially confined electric double layers

Danov, Krassimir D. / Kralchevsky, Peter A. / Stoyanov, Simeon D. / Cook, Joanne L. / Stott, Ian P.

Journal of Colloid and Interface Science

2021 Volume 581, Issue Part A

Abstract	Hypotheses: To correctly predict the aggregation number and size of wormlike micelles from ionic surfactants, the molecular-thermodynamic theory has to calculate the free energy per molecule in the micelle with accuracy better than 0.01 kT, which is a serious challenge. The problem could be solved if the effects of mutual confinement of micelle counterion atmospheres, as well as the effects of counterion binding, surface curvature and ionic interactions in the electric double layer (EDL), are accurately described. Theory: The electric field is calculated using an appropriate cell model, which takes into account the aforementioned effects. Expressions for the activity coefficients have been used, which vary across the EDL and describe the electrostatic, hard sphere, and specific interactions between the ions. New approach for fast numerical calculation of the electrostatic free energy is developed. Findings: The numerical results demonstrate the variation of quantities characterizing the EDL of cylindrical and spherical micelles with the rise of electrolyte concentration. The effect of activity coefficients leads to higher values of the free energy per surfactant molecule in the micelle as compared with the case of neglected ionic interactions. The results are essential for the correct prediction of the size of wormlike micelles from ionic surfactants. This study can be extended to mixed micelles of ionic and nonionic surfactants for interpretation of the observed synergistic effects.
Keywords	Electrostatic free energy ; Finite ionic size effects ; Ionic activity coefficients ; Ionic surfactants ; Ionic wormlike micelles
Subject code	660
Language	English
Publishing country	nl
Document type	Article ; Online
ZDB-ID	241597-5
ISSN	1095-7103 ; 0021-9797
ISSN (online)	1095-7103
ISSN	0021-9797
Database	BASE - Bielefeld Academic Search Engine (life sciences selection)

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Article ; Online: Analytical modeling of micelle growth. 1. Chain-conformation free energy of binary mixed spherical, wormlike and lamellar micelles.

Danov, Krassimir D / Kralchevsky, Peter A / Stoyanov, Simeon D / Cook, Joanne L / Stott, Ian P

Journal of colloid and interface science

2019 Volume 547, Page(s) 245–255

Abstract: Hypotheses: A quantitative molecular-thermodynamic theory of the growth of giant wormlike micelles of nonionic surfactants can be developed on the basis of a generalized model, which includes the classical "phase separation" and "mass action" models as ... ...

Abstract	Hypotheses: A quantitative molecular-thermodynamic theory of the growth of giant wormlike micelles of nonionic surfactants can be developed on the basis of a generalized model, which includes the classical "phase separation" and "mass action" models as special cases. The generalized model describes spherocylindrical micelles, which are simultaneously multicomponent and polydisperse in size. Theory: By analytical minimization of the free-energy functional we derived explicit expressions for the chain-extension and chain-end distribution functions in the hydrocarbon core of mixed micelles from two surfactants of different chainlengths. Findings: The hydrocarbon core of a two-component micelle is divided in two regions, outer and inner, where the ends of the shorter and longer chains are located. The derived analytical expression for the chain-conformation free energy implies that the mixing of surfactants with different chainlengths is always nonideal and synergistic, i.e. it leads to decrease of the micellar free energy and to enhancement of micellization and micelle growth. The derived expressions are applicable to surfactants with different headgroups (nonionic, ionic, zwitterionic) and to micelles of different shapes (spherical, wormlike, lamellar). The results can be incorporated in a quantitative theory of the growth of giant mixed micelles in formulations with practical applications in detergency.
Language	English
Publishing date	2019-04-01
Publishing country	United States
Document type	Journal Article
ZDB-ID	241597-5
ISSN	1095-7103 ; 0021-9797
ISSN (online)	1095-7103
ISSN	0021-9797
DOI	10.1016/j.jcis.2019.03.105
Database	MEDical Literature Analysis and Retrieval System OnLINE

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