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Insights into sorption species of Eu(III) on γ-Al2O3 and bentonite under different pH: Studies at macro- and micro-scales

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Abstract

The sorption species of Eu(III) on γ-Al2O3 and bentonite was investigated by batch, surface complexation model (SCM), and X-ray absorption spectroscopy (XAS). The results showed that sorption edges of Eu(III) on γ-Al2O3 and bentonite were as expected shifted forward high pH with the increasing in Eu(III) concentration, and sorption of Eu(III) was strongly dependent on pH. In γ-Al2O3 system, sorption of Eu(III) was decreased above pH 8.5 at low concentration of Eu(III) because of water soluble carbonate species of Eu(III), however the decline did not appear at high concentration of Eu(III) possibly due to a offset effect of surface precipitation. Actually, the sorption species of Eu(III) on bentonite mainly referred to at least four kinds of species including ion exchange (>X3Eu0) at low pH, inner-sphere complexes (>AlOEu2+ and >SiOEu2+) at neutral condition, and hydrolysis species (>SiOEu(OH) 02 ) at alkaline condition. Linear combination fitting (LCF) in k space testified that hydrolysis of Eu(OH)3(s) and oxide of Eu2O3 species were major for Eu(III) sorption on γ-Al2O3, whereas Eu3+(aq) and hydrolysis species comprised sorption species on bentonite. Extended X-ray absorption fine structure (EXAFS) analysis further confirmed the prediction from SCM and LCF. In addition, the typical shells of Eu–Al in R range of 3.0–3.4 Å and Eu–Si at ~4.0 Å were found in radial structure functions, which was possibly identified to edge-shared bidentate of Eu(III) on Al2O3 and bentonite.

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Acknowledgments

This study was jointly supported by the National Natural Science Foundation of China (Grant No. 11075006, 91026010), Special Foundation for High-level Waste Disposal (2007-840, 2012-851), the Fundamental Research Funds for the Central Universities, Analysis foundation of Peking University (16–19), and the National Synchrotron Radiation Innovation Foundation of Chinese Education Ministry (20090137S). We greatly acknowledge Dr. Bo He (NSRL, USTC) for helpful technical assistance of EXAFS experiments.

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Authors and Affiliations

  1. Beijing National Laboratory for Molecular Sciences, Fundamental Science Laboratory on Radiochemistry & Radiation Chemistry, College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871, China

    Qiaohui Fan, Zhong Zheng & Chunli Liu

  2. School of Nuclear Science and Technology, Lanzhou University, Lanzhou, 730000, China

    Qiaohui Fan, Ping Li & Wangsuo Wu

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  1. Qiaohui Fan
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  2. Ping Li
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Correspondence to Chunli Liu.

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Fan, Q., Li, P., Zheng, Z. et al. Insights into sorption species of Eu(III) on γ-Al2O3 and bentonite under different pH: Studies at macro- and micro-scales. J Radioanal Nucl Chem 299, 1767–1775 (2014). https://doi.org/10.1007/s10967-013-2819-x

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  • DOI: https://doi.org/10.1007/s10967-013-2819-x

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