Chapter 11. Static and dynamic studies of the energetic surface heterogeneity of clay minerals

Villièras, Frédéric; Michot, Laurent J.; Cases, J. M.; Berend, I.; Bardot, F.; François, Michèle; Gérard, G.; Yvon, Jacques

doi:10.1016/s0167-2991(97)80074-2

Cited by 36 publications

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“…Using pressure sensors that work 293 14 at low pressures, this method allows the study of surface heterogeneity of solids under 294 appropriate conditions. In the case of phyllosilicates, it has been demonstrated that such 295 adsorption experiments, coupled with a careful analysis of experimental adsorption 296 isotherms, enable a derivation of a shape factor, i.e., lateral and basal surface areas (Bardot et 297 al., 1998;Cases et al, 1986Cases et al, , 2000Michot et al, 1994Sayed-Hassan et al, 2005, 298 2006, Villiéras et al, 1992, 1997a, 1997b, 2002. 299…”

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confidence: 99%

“…Then, from the recording of quasi-equilibrium 304 pressures (in the range of 10 -3 to 3 10 4 Pa) as a function of time, the adsorption isotherm was 305 derived. The set-up used has been described in Villiéras et al (1997b) and Marrocchi et al 306 (2005). For argon adsorption, 77 K sample temperature is insured by a dynamic and accurate 307 constant level of liquid nitrogen which was itself controlled by a home-made electronic 308 device.…”

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confidence: 99%

“…Lateral interactions are easily 349 detected through the shapes (half-height width) of the local derived isotherm. In fact, the 350 intensity of lateral interactions must be considered as a best-fit parameter, disclosing further 351 information about the heterogeneity of the considered adsorption domain (Bardot, 1998, 352 Bersillon et al, 2001Mamleev et al, 2002;Villiéras et al, 1997b) capacities can be converted to surface areas by taking into account the cross-sectional area of 358 adsorbed argon, 13.8 A² (McClellan and Harnsberger, 1967). 359…”

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confidence: 99%

“…The experimental information was analyzed using the Derivative Isotherm Summation (DIS) 318 procedure designed by Villiéras et al (1992Villiéras et al ( , 1997aVilliéras et al ( , 1997b, to examine the surface energetic 319 heterogeneity of the samples. Due to the large number of experimental data points acquired 320 by the quasi-equilibrium technique, the experimental derivative of the adsorbed quantity as a 321 function of the logarithm of relative pressure could be calculated accurately.…”

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confidence: 99%

“…DIS fitting procedure was then applied to the 343 first layer free energy adsorption distribution using the Bragg-William-Tempkin model as a 344 local adsorption isotherm (Villiéras et al, 1992(Villiéras et al, , 1997a(Villiéras et al, , 1997b. Each local isotherm is 345 characterized by three parameters.…”

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Towards a link between the energetic heterogeneities of the edge faces of smectites and their stability in the context of metallic corrosion

Perronnet

Villièras

Jullien

et al. 2007

Geochimica et Cosmochimica Acta

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… From a geometrical point of view, it is thought that clay destabilization is mainly 36 controlled by phenomena starting at the edge faces of the particles. 37In the present work, the rates of the smectite-Fe(0) reaction at 80°C was assessed by XRD, 38 Mössbauer and CEC analyses for three smectites. The investigations show marked 39 differences in the degree of stability, which can not be explained by the crystal-chemistry 40 rules established in previous studies. Therefore, the Fe(0)-smectite interactions were studied 41 in view of textural and energetic surface quantitative analyses. The studied smectites have 42 equivalent nitrogen BET specific surface areas, equivalent argon edge surface areas and 43 slightly different basal surface areas. This similarity in particle shape indicates that the edge 44 surface area can not be accounted for when explaining the observed differences in reactivity. 45However, a correlation is obtained between smectite reactivity and the energetic 46 heterogeneity of its edge faces. This is interpreted in terms of a multiplication of the number 47 of sites on the edge faces, where the electron transfer between Fe(0) and the smectite 48 structure can occur. 49 3 50 INTRODUCTION 51 52Iron-clay reactions are of great importance in soils and in sedimentary and diagenetic 53 processes. In soils, the evolution of clay minerals is mainly controlled by oxidation-reduction 54 reactions. Kaolinite is very reactive in media under varying redox conditions, but Fe-rich 55 TOT clay minerals are even more reactive, and great changes in their properties may occur 56 (e.g. Favre et al. 2002). Low temperature, iron-rich, clayey environments are also described 57 in sedimentary verdine facies (Bailey 1988; Odin 1988; Odin 1990), in diagenetic oolitic 58 ironstones (Bhattacharyya 1983; Bhattacharyya 1986) and in sandstones (Hornibrook and 59 Longstaffe 1996;Aagaard et al. 2000; Hillier and Velde 1992;Hillier 1994). In these natural 60 systems, iron is present as iron oxides and/ or hydroxides (e.g. Odin 1988;Buatier et al. 1989; 61 Walker and Thompson 1990;Hornibrook and Longstaffe 1996), although metallic iron, 62Fe(0), has only been identified in contact with clay in extraterrestrial materials, such as CM 63 carbonaceous chondrites. In this case, when heating of the asteroid induces fusion of accreted 64 ice, cronstedtite, a Fe-rich 7Å mineral, is formed by interaction between olivine and FeNi 65 metal (Zolensky and McSween 1988;Brearley 1997;Zega and Buseck. 2003 Other possible controlling parameters, which were not analyzed in Lantenois' work, are those 95 describing the surface properties. Indeed, phyllosilicate surfaces have strong differential 96 reactivity because of the extreme anisotropy of their structure (Cases et al., 1986; Bickmore 97 et al., 2001), the irregular surface topography (e.g., kinks, edges and adatoms) and the 98 5 presence of defects (Metz et al., 2005). For example, concerning the alkaline dissolution of 99 smectites (Sato et al. 2003), it has been confirmed t...

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confidence: 99%

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Towards a link between the energetic heterogeneities of the edge faces of smectites and their stability in the context of metallic corrosion

Perronnet

Villièras

Jullien

et al. 2007

Geochimica et Cosmochimica Acta

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Surface Heterogeneity of Minerals

Villièras¹,

Michot²,

Bardot³

et al. 2003

ChemInform

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Role of the surface heterogeneity in adsorption of hydrogen ions on metal oxides: Theory and simulations

2005

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In this article we study the effect of energetic heterogeneity of a crystalline surface on the adsorption of hydrogen ions (protons) from the liquid phase. In particular, we examine the influence of the shape of the adsorption energy distribution on the equilibrium isotherms of hydrogen ions. To that purpose, a few popular distribution functions, including rectangular, exponential, and asymmetric Gaussian are considered. Additionally, multimodal distribution functions, which may correspond to the adsorption on different crystal planes of the oxide, are also used. Lateral interactions between adsorbed charges are modeled using the potential function proposed by Borkovec et al., which accounts also for polarization of the liquid medium. The results presented here are obtained using both Monte Carlo (MC) simulations and theoretical calculations involving Mean Field Approximation (MFA). They indicate that increased energetic heterogeneity of the adsorbing surface may, in general, considerably change the behavior of the adsorption isotherms, regardless of the assumed distribution function. It is also shown that the predictions of the proposed theory are consistent with the data obtained from the MC simulations.

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Chapter 11. Static and dynamic studies of the energetic surface heterogeneity of clay minerals

Cited by 36 publications

References 53 publications

Towards a link between the energetic heterogeneities of the edge faces of smectites and their stability in the context of metallic corrosion

Towards a link between the energetic heterogeneities of the edge faces of smectites and their stability in the context of metallic corrosion

Surface Heterogeneity of Minerals

Role of the surface heterogeneity in adsorption of hydrogen ions on metal oxides: Theory and simulations

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