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Adsorption of alpha amino acids at the water/goethite interface
Umeå University, Faculty of Science and Technology, Department of Chemistry.
Umeå University, Faculty of Science and Technology, Department of Chemistry.
Umeå University, Faculty of Science and Technology, Department of Chemistry.
2008 (English)In: Journal of Colloid and Interface Science, ISSN 0021-9797, E-ISSN 1095-7103, Vol. 319, no 2, 416-428 p.Article in journal (Refereed) Published
Abstract [en]

The adsorption of amino acids onto mineral surfaces plays an important role in a wide range of areas, e.g., low-temperature aqueous geochemistry, bone formation and protein-bone interactions. In this work, the adsorption of three alpha aminoacids (sarcosine, MIDA and EDDA) onto goethite (α-FeOOH) was studied as a function of pH and background electrolyte concentration at 25.0 °C, and the molecular structures of the surface complexes formed were analyzed by means of ATR-FTIR spectroscopy. The results showed that adsorption of alpha amino acids were strongly dependent on the functionality and structure of the ligands. No adsorption was detected for the zwitterionic sarcosine indicating that simple alpha amino acids without other ionizable and/or functional groups display insignificant affinity for mineral surfaces such as goethite. With respect to the more complex amino acids, which are surface reactive, the number and relative positions of carboxylate and amine groups determine the types of surface interactions. These interactions range from non-specific outer-sphere to specific inner-sphere interactions as shown by the MIDA and EDDA results, respectively. The results presented herein suggest that isomerically-selective adsorption might only occur for amino acids that are capable of specific surface interactions, either through site-specific hydrogen bonding or inner-sphere complexation.

Place, publisher, year, edition, pages
San Diego: Academic Press, 2008. Vol. 319, no 2, 416-428 p.
Keyword [en]
Adsorption, Amino acids, water/mineral interface, Goethite, ATR-FTIR spectroscopy
National Category
Physical Chemistry
Identifiers
URN: urn:nbn:se:umu:diva-6920DOI: 10.1016/j.jcis.2007.11.046ISI: 000253259100005PubMedID: 18155715OAI: oai:DiVA.org:umu-6920DiVA: diva2:146590
Available from: 2008-01-31 Created: 2008-01-31 Last updated: 2017-05-26Bibliographically approved
In thesis
1. Coordination Chemistry of Monocarboxylate and Aminocarboxylate Complexes at the Water/Goethite Interface
Open this publication in new window or tab >>Coordination Chemistry of Monocarboxylate and Aminocarboxylate Complexes at the Water/Goethite Interface
2007 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

This thesis is a summary of five papers with focus on adsorption processes of various monocarboxylates and aminocarboxylates at the water/goethite interface. Interaction of organic acids at the water/mineral interfaces are of importance in biogeochemical processes, since such processes have potential to alter mobility and bioavailability of the acids and metal ions.

In order to determine the coordination chemistry of acetate, benzoate, cyclohexanecarboxylate, sarcosine, MIDA (methyliminediacetic acid), EDDA (ethylenediamine-N,N’-diacetic acid) and EDTA (ethylenediamine-N,N’-tetraacetic acid) upon adsorption to the goethite (alpha-FeOOH) surface, a combination of quantitative measurements with attenuated total reflectance Fourier transform infrared spectroscopy (ATR-FTIR) was utilized.

Over the pH range studied here (pH 3- 9) all ligands, except for sarcosine, have been found to form surface complexes with goethite. In general, theses were characterized as outer sphere surface complexes i.e. with no direct interaction with surface Fe(III) metal ions. Furthermore, two types of different outer-sphere complexes were identified, the solvent-surface hydration-separated ion pair, and hydration-shared ion pair. For the monocarboxylate surface complexes distinction between these two could be made. At high pH values the solvent-surface hydration-separated ion pair was the predominating complex, while at low pH the surface complex is stabilized through the formation of strong hydrogen bonds with the goethite surface. However, it was not possible to clearly separate between the two outer-sphere complexes for coordination of the aminocarboxylates with the surface of goethite. Additionally, EDDA also formed an inner-sphere surface complex at high pH values. The EDDA molecule was suggested to coordinate to the surface by forming a five membered ring with an iron at the goethite surface, through the amine and carboxylate groups.

Contrary to the other ligands studied, EDTA significantly induced dissolution of goethite. Some of the dissolved iron, in the form of the highly stable FeEDTA- solution complex, was indicated to re-adsorb to the mineral surface as a ternary complex. Similar ternary surface complexes were also found in the Ga(III)EDTA/goethite system, and quantitative and spectroscopic studies on adsorption of Ga(III) in presence and absence of EDTA showed that EDTA considerably effects speciation of gallium at goethite surface.

The collective results in this thesis show that the affinity of these ligands for the surface of goethite is primarily governed by their chemical composition and structure, and especially important are the types, numbers and relative position of functional groups within the molecular structure.

Place, publisher, year, edition, pages
Umeå: Kemi, 2007. 52 p.
Keyword
Acetate, benzoate, adsorption, surface complex, ternary surface complexes, ATR-FTIR spectroscopy, EXAFS spectroscopy., cyclohexanecarboxylate, sarcosine, MIDA, EDDA, EDTA, gallium(III), goethite, mineral surface
National Category
Other Basic Medicine
Identifiers
urn:nbn:se:umu:diva-1337 (URN)978-91-7264-320-8 (ISBN)
Public defence
2007-09-28, KB3A9, KBC, Umeå Universitet, Umeå, 13:00
Opponent
Supervisors
Available from: 2007-09-06 Created: 2007-09-06 Last updated: 2017-05-26Bibliographically approved

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