Serge Durand-Vidal

Centre National de la Recherche Scientifique

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Pierre Turq

Sorbonne Université

Emmanuelle Dubois

PHENIX laboratory

Marie Jardat

Centre National de la Recherche Scientifique

Ivan T. Lucas

Sorbonne Université

Olivier Bernard

École Polytechnique Fédérale de Lausanne

Natalie Malikova

PHENIX laboratory

Jean‐François Dufrêche

Laboratoire de Chimie Théorique

Virginie Marry

Sorbonne Université

Guillaume Mériguet

Sorbonne Université

Didier Devilliers

Sorbonne Université

Cooperative Institutions

Centre National de la Recherche Scientifique

Sorbonne Université

PHENIX laboratory

Université Paris Cité

Commissariat à l'Énergie Atomique et aux Énergies Alternatives

Délégation Paris 6

Réseau sur le Stockage Electrochimique de l'énergie

ESPCI Paris

Université Paris-Saclay

CEA Paris-Saclay

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An Analytical Model for Probing Ion Dynamics in Clays with Broadband Dielectric Spectroscopy

The Journal of Physical Chemistry B (2005)

Benjamin Rotenberg Agathe Cadène Jean‐François Dufrêche Serge Durand-Vidal Jean‐Claude Badot

A simple two-state model is proposed to explicitly derive the ionic contribution to the frequency-dependent dielectric permittivity of clay. This model is based on a separation of time scales and accounts for two possible solvation modes (inner/outer-sphere complexes) for ions in the interlayer spacing and a possible chemical exchange between both forms. The influence on the permittivity of thermodynamic (distribution constant K(d)) and dynamic (diffusion coefficient, chemical relaxation rate) parameters is discussed. In turn, this model is used to analyze experimental data obtained with Na-montmorillonite for two relative humidities. The values of the parameters extracted from these measurements, and their variation with water content, show that the proposed model is at least reasonable.

10.1021/jp051586k

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Citations (48)

New perspectives in the transport of electrolyte solutions

Pure and Applied Chemistry (1996)

Serge Durand-Vidal P. Turq Olivier Bernard Claude Treiner Lesser Blum

Abstract

10.1351/pac199668081583

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Citations (3)

Water Dynamics in Hectorite Clays: Infuence of Temperature Studied by Coupling Neutron Spin Echo and Molecular Dynamics

Environmental Science & Technology (2011)

Virginie Marry Emmanuelle Dubois Natalie Malikova Serge Durand-Vidal S. Longeville

Within the wider context of water behavior in soils, and with a particular emphasis on clays surrounding underground radioactive waste packages, we present here the translational dynamics of water in clays in low hydrated states as studied by coupling molecular dynamics (MD) simulations and quasielastic neutron scattering experiments by neutron spin echo (NSE). A natural montmorillonite clay of interest is modeled by a synthetic clay which allows us to understand the determining parameters from MD simulations by comparison with the experimental values. We focus on temperatures between 300 and 350 K, i.e., the range relevant to the highlighted application. The activation energy Ea experimentally determined is 6.6 kJ/mol higher than that for bulk water. Simulations are in good agreement with experiments for the relevant set of conditions, and they give more insight into the origin of the observed dynamics.

Neutron spin echo

Hectorite

Quasielastic neutron scattering

10.1021/es1031932

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Citations (104)

Effective charges of micellar species obtained from Brownian dynamics simulations and from an analytical transport theory

Molecular Physics (2006)

Marie Jardat Vincent Dahirel Serge Durand-Vidal Ivan T. Lucas Olivier Bernard

We focus here on the effective charge of ionic micelles in aqueous solutions. First, we show that this quantity may be obtained by using an analytical transport theory based on the continuous solvent model to fit the experimental electrical conductivity of micellar solutions. In particular, we demonstrate the robustness of the fitting procedure on the example of real aqueous solutions of n-dodecyltrimethylammonium bromide and n-tetradecyltrimethylammonium chloride. Moreover, the approximate theoretical results are validated by a comparison to numerical simulations of Brownian dynamics. On the other hand, we propose to investigate the condensation properties of counterions on the micellar species by using Brownian dynamics. For that purpose, we have performed simulations of aqueous solutions that contain micellar species carrying their structural charge and the adequate number of counterions. We obtain a qualitative agreement between the fitted effective charges and the ones obtained by computing the mean number of bound counterions from numerical simulations.

Brownian dynamics

Micellar solutions

10.1080/00268970600997564

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Citations (13)

Surface Charge Density of Maghemite Nanoparticles: Role of Electrostatics in the Proton Exchange

The Journal of Physical Chemistry C (2007)

Ivan T. Lucas Serge Durand-Vidal Emmanuelle Dubois Jean Chevalet Pierre Turq

In the present work, we focus on the surface charge properties of well-defined maghemite (γ-Fe2O3) nanoparticles dispersed in water. Because of the acidic properties of surface groups, the nanoparticles' surface can be positively or negatively charged depending on the pH. Consequently, there are electrostatic repulsion forces between particles that allow stabilizing the suspensions in water. Acid−base titrations of the surface groups starting from acidic, alkaline, and neutral pH are performed to access the dependence of the surface charge density with the pH. Titrations are followed by potentiometric and conductometric measurements. Simultaneous zetametry measurements by acoustophoresis are implemented. The experimental curves are analyzed using several hypotheses; in particular, we assume that the sites on the surface of the particles behave as weak diacids. The interpretation of the experimental determinations of the charge implies taking into account an electrostatic term due to the potential developed at the surface of the particles. Thanks to the complementarity of the potentio-conductometric titrations and of the zetametry measurements, it is possible to better understand the phenomena of protonation and deprotonation of the colloidal particles as a function of the medium of dispersion (acidic, alkaline, neutral pH, and nature of the counterions) and of the nature of the reagent.

Maghemite

Electrostatics

Surface charge

Charge density

Electrostatic induction

10.1021/jp0743119

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Citations (124)

Influence of the volume fraction on the electrokinetic properties of maghemite nanoparticles in suspension

Molecular Physics (2014)

Ivan T. Lucas Serge Durand-Vidal O. Bernard Vincent Dahirel Emmanuelle Dubois

We used several complementary experimental and theoretical tools to characterise the charge properties of well-defined maghemite nanoparticles in solution as a function of the volume fraction. The radius of the nanoparticles is equal to 6 nm. The structural charge was measured from chemical titration and was found high enough to expect some counterions to be electrostatically attracted to the surface, decreasing the apparent charge of the nanoparticle. Direct-current conductivity measurements were interpreted by an analytical transport theory to deduce the value of this apparent charge, denoted here by 'dynamic effective charge'. This dynamic effective charge is found to decrease strongly with the volume fraction. In contrast, the 'static' effective charge, defined thanks to the Bjerrum criterion and computed from Monte Carlo simulations turns out to be almost independent of the volume fraction. In the range of Debye screening length and volume fraction investigated here, double layers around nanoparticles actually interact with each other. This strong interaction between nanocolloidal maghemite particles is probably responsible for the experimental dependence of the electrokinetic properties with the volume fraction.

Maghemite

Suspension

Volume fraction

Fraction (chemistry)

10.1080/00268976.2014.906672

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Interpretation of Conductivity Results from 5 to 45 °C on Three Micellar Systems below and above the CMC

The Journal of Physical Chemistry B (2008)

G. Roger Serge Durand-Vidal Olivier Bernard Pierre Turq Tine-Martin Perger

Electrical conductivity has been used at different temperatures to study three micellar systems: tetradecyltrimethylammonium chloride (TTACl), dodecyltrimethylammonium chloride (DTACl), and decyltrimethylammonium chloride (DeTACl). A phenomenon of premicellization is observed for DeTACl and DTACl below the critical micellar concentration (CMC). Association constants are introduced in the MSA-transport theory to correctly reproduce experimental conductivity and also calculate the effective charge of the micelles and their degree of dissociation. Various mechanisms are considered to explain premicellization. The formation of a neutral pair followed by an association involving two monomers and a counterion appears to be the most probable first step in the premicellization process.

Aggregation number

Micellar solutions

Ion-association

10.1021/jp804971c

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Citations (17)

Brownian dynamics contribution to the study of ions in aqueous solutions, charged interfaces and magnetic colloids

HAL (Le Centre pour la Communication Scientifique Directe) (2006)

Marie Jardat Guillaume Mériguet Serge Durand-Vidal Pierre Turq

Brownian dynamics

Dynamics

Source

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Theoretical interpretation of conductivity data below and above the CMC: The case of alkaline ion decanoate solutions

Journal of Molecular Liquids (2020)

Serge Durand-Vidal Olivier Bernard Žiga Medoš Marija Bešter‐Rogač

Thermodynamics of micellization

Aggregation number

Carboxylate

10.1016/j.molliq.2020.112968

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Citations (5)

Reactivity of nanocolloidal particles γ-Fe2O3 at charged interfaces : Part 2. Electrochemical conversion. Role of the electrode material

Physical Chemistry Chemical Physics (2008)

Ivan T. Lucas Emmanuelle Dubois Jean Chevalet Serge Durand-Vidal S. Joiret

In this paper we are interested in the reactivity of magnetic nanoparticles at the electrode involved in the electrochemical synthesis of magnetic and conductive liquids. The reactivity of charged colloidal particles occurs in two steps, first the approach toward the electrode with a possible adsorption phenomenon and secondly the electron transfer. In this paper we focus on the electrochemical behaviour of well-defined γ-Fe2O3nanoparticles at a gold and at a mercury electrode. Particles can be electrochemically reduced at the two electrodes and can be dispersed into mercury at a highly negative potential. Here, we probe in particular the properties of nanoreactor of the particles, that is to say, the possible conservation of their size after they have undergone the electrochemical process. By correlating complementary techniques (here atomic force microscopy (AFM) observations, Raman spectroscopy and cyclic voltammetry on gold electrode) and by studying the magnetic properties of the material obtained after reduction of the particles on a mercury electrode, we are able to probe both the chemical nature and the physical state of the particles once transformed. Experimental results show that under specific conditions, the particles are individually converted into iron, which justifies their use for preparing a liquid with both magnetic properties and properties of electron conduction.

Reactivity

10.1039/b718738f

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Citations (9)