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Molecular level picture of the interplay between pH and phosphate binding at the goethite-water interface

  • The soil pH plays a substantial role in controlling phosphorus (P) adsorption and mobilization. These processes are strongly affected by the phosphate interaction strength with P-fixing soil minerals such as goethite. The target of the current contribution is to draw a molecular level picture of the interplay between pH and phosphate binding at the goethite–water interface via a joint experimental–theoretical approach. Periodic density functional theory (DFT) calculations were carried out to provide a molecular level understanding of the pH dependence of P adsorption. To validate the modeling approach, adsorption experiments of phosphate at goethite were performed in the pH range of 4–12. There was agreement between experiments and simulations in the description of the adsorption behavior by two pH-dependent successive stages. The adsorption increases along the pH change from 4 to 8. A further increase of pH leads to a decrease of adsorption. By comparing with literature data it is concluded that the first stage will be observed onlyThe soil pH plays a substantial role in controlling phosphorus (P) adsorption and mobilization. These processes are strongly affected by the phosphate interaction strength with P-fixing soil minerals such as goethite. The target of the current contribution is to draw a molecular level picture of the interplay between pH and phosphate binding at the goethite–water interface via a joint experimental–theoretical approach. Periodic density functional theory (DFT) calculations were carried out to provide a molecular level understanding of the pH dependence of P adsorption. To validate the modeling approach, adsorption experiments of phosphate at goethite were performed in the pH range of 4–12. There was agreement between experiments and simulations in the description of the adsorption behavior by two pH-dependent successive stages. The adsorption increases along the pH change from 4 to 8. A further increase of pH leads to a decrease of adsorption. By comparing with literature data it is concluded that the first stage will be observed only if there is no significant change of the surface charge at low pH. Moreover, the molecular modeling results point to the abundance of the monodentate (M) binding motif at both extremely low and high pH ranges. Otherwise, the bidentate (B) one is predominant along the intermediate pH range. These observations could resolve the existing debate about the assignment of phosphate–goethite binding motifs. Furthermore, the results point to a decrease of pH upon phosphate sorption due to an induced acidification of soil solution. The present joint experimental–theoretical approach provides a better understanding and description of the existing phosphate sorption experiments and highlights new findings at the atomistic/molecular scale.show moreshow less

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Metadaten
Author: Ashour A. AhmedORCiD, Stella GypserORCiD, Dirk FreeseORCiD, Peter Leinweber, Oliver KühnORCiD
DOI:https://doi.org/10.1039/d0cp04698a
ISSN:1463-9084
Title of the source (English):Physical Chemistry Chemical Physics
Document Type:Scientific journal article peer-reviewed
Language:English
Year of publication:2020
Contributing Corporation:Brandenburgische Technische Universität Cottbus-Senftenberg
Tag:Adsorption; Goethite; Periodic density functional theory; Phosphate; pH
Volume/Year:22
Issue number:45
First Page:26509
Last Page:26524
Faculty/Chair:Fakultät 2 Umwelt und Naturwissenschaften / FG Bodenschutz und Rekultivierung
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