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Carbonate-induced structural perturbation of Al hydroxides

Published online by Cambridge University Press:  01 January 2024

G. Y. Zhang ,
Y. F. Hu ,
R. K. Xu ,
J. J. Dynes ,
R. I. R. Blyth ,
L. M. Kozak  and
P. M. Huang
G. Y. Zhang
Affiliation:
Department of Soil Science, University of Saskatchewan 51 Campus Drive S7N 5A8 Saskatoon SK Canada Department of Resources and Environmental Science, Agricultural University of Hebei Baoding China
Y. F. Hu
Affiliation:
Canadian Light Source 101 Perimeter Road S7N 0X4 Saskatoon SK Canada
R. K. Xu
Affiliation:
Department of Soil Science, University of Saskatchewan 51 Campus Drive S7N 5A8 Saskatoon SK Canada Institute of Soil Science, Chinese Academy of Sciences P.O. Box 821 Nanjing China
J. J. Dynes*
Affiliation:
Environment Canada 11 Innovation Boulevard S7N 3H5 Saskatoon SK Canada Department of Chemistry, McMaster University L8S 4M1 Hamilton ON Canada
R. I. R. Blyth
Affiliation:
Canadian Light Source 101 Perimeter Road S7N 0X4 Saskatoon SK Canada
L. M. Kozak
Affiliation:
Department of Soil Science, University of Saskatchewan 51 Campus Drive S7N 5A8 Saskatoon SK Canada
P. M. Huang
Affiliation:
Department of Soil Science, University of Saskatchewan 51 Campus Drive S7N 5A8 Saskatoon SK Canada
*
djames.dynes@usask.ca
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Abstract

The chemistry of Al transformation has been well documented, though little is known about the mechanisms of structural perturbation of Al precipitates by carbonates at a molecular level. The purpose of the present study was to investigate the structural perturbation of Al precipitates formed under the influence of carbonates. Initial carbonate/Al molar ratios (MRs) used were 0, 0.1, and 0.5 after aging for 32 days, then the samples were analyzed by X-ray absorption near edge structure spectroscopy (XANES), X-ray diffraction (XRD), Fourier-transform infrared absorption spectroscopy (FTIR), and chemical analysis. The XRD data were in accord with the FTIR results, which revealed that as the carbonate/Al MR was increased from 0 to 0.1, carbonate preferentially retarded the formation of gibbsite and had relatively little effect on the formation of bayerite. As the carbonate/Al MR was increased to 0.5, however, the crystallization of both gibbsite and bayerite was completely inhibited. The impact of carbonate on the nature of Al precipitates was also evident in the increase of adsorbed water and inorganic C contents with increasing carbonate/Al MR. The Al K- and L- edge XANES data provide the first evidence illustrating the change in the coordination number of Al from 6-fold to mixed 6- and 4-fold coordination in the structural network of short-range ordered (SRO) Al precipitates formed under the increasing perturbation of carbonate. The fluorescence yield spectra of the O K-edge show that the intensity of the peak at 534.5 eV assigned to σ* transitions of Al-O and O-H bonding decreased with increasing carbonate/Al MR. The XANES data, along with the evidence from XRD, FTIR, and chemical analysis showed clearly that carbonate caused the alteration of the coordination nature of the Al-O bonding through perturbation of the atomic bonding and structural configuration of Al hydroxides by complexation with Al in the SRO network of Al precipitates. The surface reactivity of an Al-O bond is related to its covalency and coordination geometry. The present findings were, therefore, of fundamental significance in understanding the low-temperature geochemistry of Al and its impacts on the transformation, transport, and fate of nutrients and pollutants in the ecosystem.

Keywords

Al transformationCarbonateComplexationCoordination NatureEcosystemShort-range Ordered Mineral ColloidsStructural DisorderXANES Spectroscopy

Information

Type
Article
Information
Clays and Clay Minerals , Volume 57 , Issue 6 , December 2009 , pp. 795 - 807
Copyright
© The Clay Minerals Society 2009

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