skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Characterisation of the surface thermodynamic properties of cement components by inverse gas chromatography at infinite dilution

Abstract

The surface thermodynamic properties of three main inorganic compounds formed during hydration of Portland cement: calcium hydroxide (Ca(OH){sub 2}), ettringite (3CaO.Al{sub 2}O{sub 3}.3CaSO{sub 4}.32H{sub 2}O) and calcium-silicate-hydrates (C-S-H), respectively, and one mineral filler: calcium carbonate (CaCO{sub 3}), have been characterised by inverse gas chromatography at infinite dilution (IGC-ID) at 35 deg. C. The thermodynamic properties have been investigated using a wide range of non-polar (n-alkane series), Lewis acidic (CH{sub 2}Cl{sub 2} and CHCl{sub 3}), Lewis basic (diethyl ether) and aromatic (benzene) and n-alkene series molecular probes, respectively. The tested samples are fairly high surface energy materials as judged by the high dispersive contribution to the total surface energy (the dispersive components {gamma} {sub s} {sup d} range from 45.6 up to 236.2 mJ m{sup -2} at 35 deg. C) and exhibit amphoteric properties, with a predominant acidic character. In the case of hydrated components (i.e. ettringite and C-S-H), the surface thermodynamic properties have been determined at various temperatures (from 35 up to 120 deg. C) in order to examine the influence of the water content. The changes of both dispersive and specific components clearly demonstrate that the material surface properties are activated with temperature. The changes in the acid-base propertiesmore » are correlated with the extent of the overall water loss induced by the thermal treatment as demonstrated by thermogravimetric analysis (TGA). The elemental surface composition of these compounds has been determined by X-ray photoelectron spectroscopy (XPS)« less

Authors:
 [1];  [1];  [1];  [2]
  1. Interfaces, Traitements, Organisation et Dynamique des Systemes (ITODYS) Universite Paris 7- Denis. Diderot, 1 Rue Guy de la Brosse, 75005 Paris (France)
  2. Laboratoire Central des Ponts et Chaussees (LCPC), 58 Boulevard Lefevre, 75732 Paris Cedex 15 (France). E-mail: benzarti@lcpc.fr
Publication Date:
OSTI Identifier:
20793271
Resource Type:
Journal Article
Resource Relation:
Journal Name: Cement and Concrete Research; Journal Volume: 36; Journal Issue: 2; Other Information: DOI: 10.1016/j.cemconres.2005.02.005; PII: S0008-8846(05)00080-3; Copyright (c) 2005 Elsevier Science B.V., Amsterdam, The Netherlands, All rights reserved; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; CALCIUM CARBONATES; CALCIUM HYDROXIDES; CALCIUM SILICATES; GAS CHROMATOGRAPHY; HYDRATES; HYDRATION; PORTLAND CEMENT; SURFACE ENERGY; THERMAL GRAVIMETRIC ANALYSIS; X-RAY PHOTOELECTRON SPECTROSCOPY

Citation Formats

Perruchot, Christian, Chehimi, Mohamed M., Vaulay, Marie-Josephe, and Benzarti, Karim. Characterisation of the surface thermodynamic properties of cement components by inverse gas chromatography at infinite dilution. United States: N. p., 2006. Web. doi:10.1016/J.CEMCONRES.2005.0.
Perruchot, Christian, Chehimi, Mohamed M., Vaulay, Marie-Josephe, & Benzarti, Karim. Characterisation of the surface thermodynamic properties of cement components by inverse gas chromatography at infinite dilution. United States. doi:10.1016/J.CEMCONRES.2005.0.
Perruchot, Christian, Chehimi, Mohamed M., Vaulay, Marie-Josephe, and Benzarti, Karim. Wed . "Characterisation of the surface thermodynamic properties of cement components by inverse gas chromatography at infinite dilution". United States. doi:10.1016/J.CEMCONRES.2005.0.
@article{osti_20793271,
title = {Characterisation of the surface thermodynamic properties of cement components by inverse gas chromatography at infinite dilution},
author = {Perruchot, Christian and Chehimi, Mohamed M. and Vaulay, Marie-Josephe and Benzarti, Karim},
abstractNote = {The surface thermodynamic properties of three main inorganic compounds formed during hydration of Portland cement: calcium hydroxide (Ca(OH){sub 2}), ettringite (3CaO.Al{sub 2}O{sub 3}.3CaSO{sub 4}.32H{sub 2}O) and calcium-silicate-hydrates (C-S-H), respectively, and one mineral filler: calcium carbonate (CaCO{sub 3}), have been characterised by inverse gas chromatography at infinite dilution (IGC-ID) at 35 deg. C. The thermodynamic properties have been investigated using a wide range of non-polar (n-alkane series), Lewis acidic (CH{sub 2}Cl{sub 2} and CHCl{sub 3}), Lewis basic (diethyl ether) and aromatic (benzene) and n-alkene series molecular probes, respectively. The tested samples are fairly high surface energy materials as judged by the high dispersive contribution to the total surface energy (the dispersive components {gamma} {sub s} {sup d} range from 45.6 up to 236.2 mJ m{sup -2} at 35 deg. C) and exhibit amphoteric properties, with a predominant acidic character. In the case of hydrated components (i.e. ettringite and C-S-H), the surface thermodynamic properties have been determined at various temperatures (from 35 up to 120 deg. C) in order to examine the influence of the water content. The changes of both dispersive and specific components clearly demonstrate that the material surface properties are activated with temperature. The changes in the acid-base properties are correlated with the extent of the overall water loss induced by the thermal treatment as demonstrated by thermogravimetric analysis (TGA). The elemental surface composition of these compounds has been determined by X-ray photoelectron spectroscopy (XPS)},
doi = {10.1016/J.CEMCONRES.2005.0},
journal = {Cement and Concrete Research},
number = 2,
volume = 36,
place = {United States},
year = {Wed Feb 15 00:00:00 EST 2006},
month = {Wed Feb 15 00:00:00 EST 2006}
}
  • Activity coefficients at infinite dilution of organic compounds in the ionic liquid (IL) trihexyl(tetradecyl) phosphonium bis(trifluoromethylsulfonyl)imide were determined using inverse gas chromatography at three temperatures, T ) (302.45, 322.35, and 342.45) K. Linear free energy relationship (LFER) correlations have been obtained for describing the gas-to-IL and water-to-IL partition coefficients.
  • The adsorption energy distributions (AEDs) of several molecular probes on two silica samples were determined from their chromatographic retention data. Adsorption data were obtained using the elution-by-characteristic points (ECP) method of capillary inverse gas chromatography at finite dilution. The diffuse rear profiles of the bands obtained with samples of different sizes overlay consistently. The numerical expectation-maximization (EM) method has been applied to the calculation of the AEDs from the unfitted experimental adsorption isotherms, using the Langmuir model for the local adsorption isotherm. Two silica samples, both unmodified and reacted with trimethylchlorosilane, were used. Results were obtained with methanol, diethyl ether,more » 1-chlorobutane, dichloromethane, and toluene. Their AEDs exhibit two high-energy peaks, around 45-60 and 50-70 kJ/mol, respectively. The differences observed for the specific capacities of adsorption and for the energy distributions of the unmodified and modified silicas are correlated with the chemical structure of the probe and the adsorbent surface. 17 refs., 10 figs., 4 tabs.« less
  • A semitheoretical expression for partial molar volumes at infinite dilution of aqueous nonelectrolyte solutes has been developed employing the collection of properties from fluctuation solution theory for use over wide ranges of temperature and pressure. The form of the solution expression was suggested by a comparison of solute/solvent and solvent/solvent direct correlations function integrals (DCFI). The selection of solvent density and compressibility as model variables provides a correct description in the critical region while second virial coefficients have been used to give a rigorous expression in the low density region. The formulation has been integrated to obtain analytic expressions formore » thermodynamic properties of hydration at supercritical temperatures. The equation is limited to solutes for which B{sub 12} (the second cross virial coefficient between water and a solute molecule) is known or can be estimated. Regression of the three remaining parameters gives good correlations of the available experimental data. A strategy for estimating these parameters allows prediction from readily available data.« less
  • The Raoult's-law activity coefficients of 3- to 7-carbon aliphatic aldehyde, ketone, ester, and alcohol solutes at infinite dilution in methanol, water, and mixtures of the two and in polydimethysiloxane, all at 293-308 K, have been determined for the first time by appropriate combination of GLC and LLC retention data. The latter data are reported in terms of mole factions, while the former are given in concentration units of molality. However, interpretation of the data is difficult because of the multiplicity of the retention mechanisms. Nevertheless, the combined GLC/LLC technique, which had been applied previously only to pure solvents, is saidmore » to offer a number of advantages over static techniques for the determination of solute infinite-dilution activity coefficients with volatile solvents, especially with mixtures of solvents.« less
  • Important problems, such as limited yield of oil recovery during petroleum exploitation, involve the interaction of pore filling fluids with the minerals which constitute the reservoir walls. The clay minerals, due to their specific surface area and electrical charge density, are the most active of those minerals. The surface properties of illites and kaolinites of various origins and formation conditions were measured by inverse gas chromatography (IGC) at infinite dilution conditions. The value of the dispersive component of the surface energy ({gamma}) determined by IGC is significantly higher for these clays than the {gamma} of amorphous silicas. This is explainedmore » by the partial insertion of a very small amount of injected alkane probes into structural defects located on the border layers of the clays. The use of branched bulky alkane probes allows the evaluation of the clay`s nanorugosity through the determination of a morphological index (I{sub M}). The relation between {gamma} and surface nanorugosity (I{sub M}) confirms that the high values of {gamma} of the clays are representative only of these particulate sites of adsorption.« less