Molecule–Surface Recognition between Heterocyclic Aromatic Compounds and Kaolinite in Toluene Investigated by Molecular Theory of Solvation and Thermodynamic and Kinetic Experiments

Abstract

Vous avez des questions? Nous pouvons vous aider. Pour communiquer directement avec un auteur, consultez la première page de la revue dans laquelle son article a été publié afin de trouver ses coordonnées. Si vous n'arrivez pas à les repérer, communiquez avec nous à PublicationsArchive-ArchivesPublications@nrc-cnrc.gc.ca. Questions? Contact the NRC Publications Archive team atPublicationsArchive-ArchivesPublications@nrc-cnrc.gc.ca. If you wish to email the authors directly, please see the first page of the publication for their contact information. NRC Publications Archive Archives des publications du CNRCThis publication could be one of several versions: author's original, accepted manuscript or the publisher's version. / La version de cette publication peut être l'une des suivantes : la version prépublication de l'auteur, la version acceptée du manuscrit ou la version de l'éditeur. For the publisher's version, please access the DOI link below./ Pour consulter la version de l'éditeur, utilisez le lien DOI ci-dessous.http://doi.org/10.1021/jp507393uAccess and use of this website and the material on it are subject to the Terms and Conditions set forth at Molecule-surface recognition between heterocyclic aromatic compounds and kaolinite in toluene investigated by molecular theory of solvation and thermodynamic and kinetic experiments Huang, WenJuan; Dedzo, Gustave Kenne; Stoyanov, Stanislav R.; Lyubimova, Olga; Gusarov, Sergey; Singh, Shashank; Lao, Hayes; Kovalenko, Andriy; Detellier, Christian http://nparc.cisti-icist.nrc-cnrc.gc.ca/fra/droits L'accès à ce site Web et l'utilisation de son contenu sont assujettis aux conditions présentées dans le site LISEZ CES CONDITIONS ATTENTIVEMENT AVANT D'UTILISER CE SITE WEB. NRC Publications Record / Notice d'Archives des publications de CNRC:http://nparc.cisti-icist.nrc-cnrc.gc.ca/eng/view/object/?id=7b90aae5-5f3a-4009-aa11-d27eb5d6926a http://nparc.cisti-icist.nrc-cnrc.gc.ca/fra/voir/objet/?id=7b90aae5-5f3a-4009-aa11-d27eb5d6926a ABSTRACT: Molecular recognition interactions between kaolinite and a series of heterocyclic aromatic compounds (HAC) representative of the N-and S-containing moieties in petroleum asphaltene macromolecules are investigated using the threedimensional reference interaction site model with the Kovalenko−Hirata closure approximation (3D-RISM-KH) theory of solvation and experimental techniques in toluene solvent. The statistical-mechanical 3D-RISM-KH molecular theory of solvation predicts the adsorption configuration and thermodynamics from the 3D site density distribution functions and total solvation free energy, respectively, for adsorption of HAC and toluene on kaolinite. Spectrophotometric measurements show that, among the HAC studied, only acridine and phenanthridine adsorb quantitatively on kaolinite. For these pyridinic HAC, the adsorption results fitted to the Langmuir isotherm in the monolayer domain suggest a uniform monolayer of HAC molecules. The 3D-RISM-KH studies predict that the aluminum hydroxide surface of kaolinite is preferred for...

Solvation Thermodynamics of Organic Molecules by the Molecular Integral Equation Theory: Approaching Chemical Accuracy

“…194 Therefore, 3D-SFED can provide useful information about different association/adsorption processes at complex biomolecule and supramolecule aggregate surfaces. 194,195,312 …”

Electric Interfacial Layer of Modified Cellulose Nanocrystals in Aqueous Electrolyte Solution: Predictions by the Molecular Theory of Solvation

“…The 3D-RISM-KH molecular theory of solvation yields the solvation thermodynamics by statistical mechanical sampling of equilibrium arrangements of solvent and ions around CNC particles, which is extremely challenging for molecular simulations. The 3D-RISM-KH method predicts molecular recognition interactions in solution 48 and could help improve the compatibilization of CNC with matrix polymers so as to enhance the CNC loading levels in composites, hydrogels, and foams. For example, insights from modeling into the mechanism of action of cationization agents 17 could help further enhance the dispersion, gelation, and rheological properties of modified CNC.…”

Adsorption of Bitumen Model Compounds on Kaolinite in Liquid and Supercritical Carbon Dioxide Solvents: A Study by Periodic Density Functional Theory and Molecular Theory of Solvation

“…68 The molecular recognition interactions of S-and N-containing heterocycles (relevant to asphaltenes) toward kaolinite have been investigated in a toluene solvent using the 3D-RISM−KH method to gain insight into this entropy-driven organization and correlated with experimental adsorption kinetic and thermodynamic studies. 69 In the present work, we study the adsorption of model bitumen compounds on kaolinite using the PW91 density functional and periodic boundary conditions (PBC). The mechanism of solvation of systems containing kaolinite platelet and bitumen molecules in a CO 2 solvent is explored using the 3D-RISM−KH molecular theory of solvation.…”

“…The interactions of C sites of CO 2 with the aluminum hydroxide surface of kaolinite are stronger than those of toluene solvent sites (0.6−0.8 kcal/ mol). 69 …”

“…Nonbonding parameters and partial charges for the kaolinite atoms are adopted from the CLAYFF general force field developed by Cygan et al 71 For the bitumen model compounds, we use the nonbonded parameters σ and ε from the OPLS all-atom force field 87,88 and atomic charges calculated using the MOPAC2012 computational chemistry software, 89 as in our previous studies. 68,69 ■ RESULTS AND DISCUSSION DFT in PBC Calculations. The PW91/DNP method implemented in the DMol 3 software was used to fully optimize the geometries of the bitumen model compounds on kaolinite.…”