Advanced Analysis of Clay Microporosity Using High-Resolution N<sub>2</sub>-Ar Adsorption Isotherms Coupled with the Derivative Isotherm Summation Method

The textural properties of synthetic and natural clays in the sodium form and exchanged with tetramethylammonium cations (TMA<sup>+</sup>) were characterized using N<sub>2</sub> and Ar physisorption isotherms at cryogenic temperatures. Specific surface areas and micro/mesopor...

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Main Authors: Anwar El Azrak, Denys I. Grekov, Laurent Truche, Pascaline Pré
Format: Article
Language:English
Published: MDPI AG 2024-12-01
Series:Molecules
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Online Access:https://www.mdpi.com/1420-3049/29/24/6019
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author Anwar El Azrak
Denys I. Grekov
Laurent Truche
Pascaline Pré
author_facet Anwar El Azrak
Denys I. Grekov
Laurent Truche
Pascaline Pré
author_sort Anwar El Azrak
collection DOAJ
description The textural properties of synthetic and natural clays in the sodium form and exchanged with tetramethylammonium cations (TMA<sup>+</sup>) were characterized using N<sub>2</sub> and Ar physisorption isotherms at cryogenic temperatures. Specific surface areas and micro/mesoporous volumes were determined using the BET and the <i>t-plot</i> models. The <i>t-plot</i> analysis requires the use of reference isotherms measured at the same temperature on the surface of non-porous materials with an identical chemical composition. In order to better assess the effects of chemical heterogeneities in the clay particles, reference isotherms representative of silica surfaces were taken into account in the analysis of the <i>t-curve</i> and corrected to account for variations in curvature at the interface of the film adsorbed in the micropores. In addition, high-resolution Ar adsorption isotherms at 87 K were analyzed using the Derivative Isotherm Summation (DIS) method to quantify the energy contributions of adsorption sites and determine the fractions of basal and lateral surfaces of clay particles. The high-energy adsorption sites, identified in the low-pressure range, were attributed to intra-particle microporosity due to stacking defects and/or open inter-layer spaces. These sites were differentiated from those on the lateral and basal surfaces of the particles. A modification of the DIS method was proposed to measure these contributions and improve the fit with the experimental data. The results show that TMA<sup>+</sup> cation exchange significantly increases the microporosity of clays compared to their sodic form, which can be attributed to the increased contribution of intra-particle adsorption sites due to interlayer expansion.
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spelling doaj-art-22e0f4a557fb45bfb14da6f5d78d8a6c2024-12-27T14:42:57ZengMDPI AGMolecules1420-30492024-12-012924601910.3390/molecules29246019Advanced Analysis of Clay Microporosity Using High-Resolution N<sub>2</sub>-Ar Adsorption Isotherms Coupled with the Derivative Isotherm Summation MethodAnwar El Azrak0Denys I. Grekov1Laurent Truche2Pascaline Pré3IMT Atlantique, GEPEA, UMR CNRS 6144, F-44307 Nantes, FranceIMT Atlantique, GEPEA, UMR CNRS 6144, F-44307 Nantes, FranceUniv. Grenoble Alpes, CNRS, IRD, IFSTTAR, ISTerre, 38000 Grenoble, FranceIMT Atlantique, GEPEA, UMR CNRS 6144, F-44307 Nantes, FranceThe textural properties of synthetic and natural clays in the sodium form and exchanged with tetramethylammonium cations (TMA<sup>+</sup>) were characterized using N<sub>2</sub> and Ar physisorption isotherms at cryogenic temperatures. Specific surface areas and micro/mesoporous volumes were determined using the BET and the <i>t-plot</i> models. The <i>t-plot</i> analysis requires the use of reference isotherms measured at the same temperature on the surface of non-porous materials with an identical chemical composition. In order to better assess the effects of chemical heterogeneities in the clay particles, reference isotherms representative of silica surfaces were taken into account in the analysis of the <i>t-curve</i> and corrected to account for variations in curvature at the interface of the film adsorbed in the micropores. In addition, high-resolution Ar adsorption isotherms at 87 K were analyzed using the Derivative Isotherm Summation (DIS) method to quantify the energy contributions of adsorption sites and determine the fractions of basal and lateral surfaces of clay particles. The high-energy adsorption sites, identified in the low-pressure range, were attributed to intra-particle microporosity due to stacking defects and/or open inter-layer spaces. These sites were differentiated from those on the lateral and basal surfaces of the particles. A modification of the DIS method was proposed to measure these contributions and improve the fit with the experimental data. The results show that TMA<sup>+</sup> cation exchange significantly increases the microporosity of clays compared to their sodic form, which can be attributed to the increased contribution of intra-particle adsorption sites due to interlayer expansion.https://www.mdpi.com/1420-3049/29/24/6019claycation exchangeDIS methodmicroporosity<i>t-plot</i>
spellingShingle Anwar El Azrak
Denys I. Grekov
Laurent Truche
Pascaline Pré
Advanced Analysis of Clay Microporosity Using High-Resolution N<sub>2</sub>-Ar Adsorption Isotherms Coupled with the Derivative Isotherm Summation Method
Molecules
clay
cation exchange
DIS method
microporosity
<i>t-plot</i>
title Advanced Analysis of Clay Microporosity Using High-Resolution N<sub>2</sub>-Ar Adsorption Isotherms Coupled with the Derivative Isotherm Summation Method
title_full Advanced Analysis of Clay Microporosity Using High-Resolution N<sub>2</sub>-Ar Adsorption Isotherms Coupled with the Derivative Isotherm Summation Method
title_fullStr Advanced Analysis of Clay Microporosity Using High-Resolution N<sub>2</sub>-Ar Adsorption Isotherms Coupled with the Derivative Isotherm Summation Method
title_full_unstemmed Advanced Analysis of Clay Microporosity Using High-Resolution N<sub>2</sub>-Ar Adsorption Isotherms Coupled with the Derivative Isotherm Summation Method
title_short Advanced Analysis of Clay Microporosity Using High-Resolution N<sub>2</sub>-Ar Adsorption Isotherms Coupled with the Derivative Isotherm Summation Method
title_sort advanced analysis of clay microporosity using high resolution n sub 2 sub ar adsorption isotherms coupled with the derivative isotherm summation method
topic clay
cation exchange
DIS method
microporosity
<i>t-plot</i>
url https://www.mdpi.com/1420-3049/29/24/6019
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AT laurenttruche advancedanalysisofclaymicroporosityusinghighresolutionnsub2subaradsorptionisothermscoupledwiththederivativeisothermsummationmethod
AT pascalinepre advancedanalysisofclaymicroporosityusinghighresolutionnsub2subaradsorptionisothermscoupledwiththederivativeisothermsummationmethod