Gutenberg Open


Personen: Kersten, Michael (Autor) 
Vlasova, Nataliya (Autor) 
Titel: Silicate adsorption by goethite at elevated temperatures
Quelle: Chemical geology. Bd. 262. H. 3/4. S. 336 - 343
Erscheinungsjahr:    2009
ISBN / ISSN: 0009-2541
URL der Originalveröffentlichung doi:10.1016/j.chemgeo.2009.02.002
Zeitschriftenaufsatz Zeitschriftenaufsatz
Sprache: Englisch
Open Access:
Person der Universität:    Kersten, Michael  In UnivIS suchen  
Einrichtung: Institut für Geowissenschaften
DDC-Sachgruppe:    Geowissenschaften
ID: 15411  Universitätsbibliothek Mainz
Informationen zu den Nutzungsrechten unserer Inhalte Informationen zu den Nutzungsrechten unserer Inhalte
Abstract: Batch adsorption experiments with relatively low silica concentrations between 10 mu M and 100 mu M were conducted at three different ionic strength (0.01 - 0.1 M), and four different temperatures between 10 degrees C and 75 degrees C, yielding in a total of 550 experimental data points. The residual concentration of monosilicic acid is controlled by an adsorption equilibrium which is dependent on pH. The % Si adsorbed vs. -log[H+] curves reveal an upward bend with a maximum at about a pH of 9. With acidification below pH 9 the residual Si concentration in the suspensions steadily increases, as well as in the increasingly alkaline pH range. The slope of the latter is becoming steeper with increasing temperature. A basic Stern layer and charge distribution approach was used for modelling surface charge. The -log[H+]-dependent Si adsorption at the goethite surface was modelled involving a single-site approach for both neutral and hydrolyzed silicate inner-sphere surface complexes. For both a binuclear bidentate C-2 complex was chosen according to spectroscopic information. Experimental data at all ionic strengths and temperatures are matched equally well by the adsorption model. The model output suggests a decrease in the pH where hydrolysis of the Si surface complex starts, and therefore an increasing importance of the hydrolyzed surface species with increasing temperature. The equilibrium adsorption constants could be well represented by a linear Van%27t Hoff logK(T) vs. 1/T plot, from which thermodynamic Delta H-r(298) and Delta(r)G(298) values of the adsorption reactions were derived. Adsorption of the silicate on the goethite surface is exothermic (Delta H-r(298) = -43.7 kJ mol(-1) for the dominating surface complex), and becomes therefore weaker with increasing temperature. (C) 2009 Elsevier B.V. All rights reserved.
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