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Sorption of Eu(III) on Granite: EPMA, LA–ICP–MS, Batch and Modeling Studies

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† Institute of Nature and Environmental Technology, Kanazawa University, Kakuma, Kanazawa, Ishikawa 920-1192, Japan
‡ Division of Earth and Environmental Sciences, Graduate School of Natural Science and Technology, Kanazawa University, Kakuma, Kanazawa, Ishikawa 920-1192, Japan
§ Japan Atomic Energy Agency, Mizunami, Gifu 509-6132, Japan
∥ Center for Membrane and Film Technology, Department of Chemical Science and Engineering, Kobe University, 1-1 Rokkodai-cho, Nada-ku, Kobe 657-8501, Japan
*Phone: +81-76-264-6520, e-mail: [email protected]
Cite this: Environ. Sci. Technol. 2013, 47, 22, 12811–12818
Publication Date (Web):October 9, 2013
https://doi.org/10.1021/es402676n
Copyright © 2013 American Chemical Society
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Abstract

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Eu(III) sorption on granite was assessed using combined microscopic and macroscopic approaches in neutral to acidic conditions where the mobility of Eu(III) is generally considered to be high. Polished thin sections of the granite were reacted with solutions containing 10 μM of Eu(III) and were analyzed using EPMA and LA–ICP–MS. On most of the biotite grains, Eu enrichment up to 6 wt % was observed. The Eu-enriched parts of biotite commonly lose K, which is the interlayer cation of biotite, indicating that the sorption mode of Eu(III) by the biotite is cation exchange in the interlayer. The distributions of Eu appeared along the original cracks of the biotite. Those occurrences indicate that the prior water–rock interaction along the cracks engendered modification of biotite to possess affinity to the Eu(III). Batch Eu(III) sorption experiments on granite and biotite powders were conducted as functions of pH, Eu(III) loading, and ionic strength. The macroscopic sorption behavior of biotite was consistent with that of granite. At pH > 4, there was little pH dependence but strong ionic strength dependence of Eu(III) sorption. At pH < 4, the sorption of Eu(III) abruptly decreased with decreased pH. The sorption behavior at pH > 4 was reproducible reasonably by the modeling considering single-site cation exchange reactions. The decrease of Eu(III) sorption at pH < 4 was explained by the occupation of exchangeable sites by dissolved cationic species such as Al and Fe from granite and biotite in low-pH conditions. Granites are complex mineral assemblages. However, the combined microscopic and macroscopic approaches revealed that elementary reactions by a single mineral phase can be representative of the bulk sorption reaction in complex mineral assemblages.

Supporting Information

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An optical image and a corresponding mineral distribution map of the granite examined in this study (Figure S1), XRD patterns of the bulk granite sample (Figure S2), results of EPMA analysis of biotite grain before reaction with Eu(III) (Figure S3), results of EPMA analysis of biotite grain after reaction with Eu(III) (Figure S4), BSE image and elemental distributions of alteration minerals formed in plagioclase grain (Figure S5), sorption kinetics of Eu(III) on the granite (Figure S6), results of EPMA analysis of biotite grain after reaction with Eu(III) at pH 6 (Figure S7), LA–ICP–MS spectra of major constituent minerals in granite before Eu(III) sorption (Figure S8), results of leaching tests of Fe and Al from granite powder as a function of pH (Figure S9), operating conditions for the LA–ICP–MS method (Table S1), some measured properties and model parameters for Eu(III) sorption on granite and biotite (Table S2), aqueous reactions, and these constants used in the sorption modeling (Table S3). This material is available free of charge via the Internet at http://pubs.acs.org.

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Cited By

This article is cited by 16 publications.

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  2. Keisuke Fukushi, Haruka Sakai, Taeko Itono, Akihiro Tamura, and Shoji Arai . Desorption of Intrinsic Cesium from Smectite: Inhibitive Effects of Clay Particle Organization on Cesium Desorption. Environmental Science & Technology 2014, 48 (18) , 10743-10749. https://doi.org/10.1021/es502758s
  3. Han Zhang, Hanyi He, Jun Liu, Honghui Li, Shuaiwei Zhao, Meilan Jia, Jijun Yang, Ning Liu, Yuanyou Yang, Jiali Liao. Sorption behavior of Eu(Ⅲ) on Tamusu clay under strong ionic strength: Batch experiments and BSE/EDS analysis. Nuclear Engineering and Technology 2021, 53 (1) , 164-171. https://doi.org/10.1016/j.net.2020.06.009
  4. Hiroki Mukai, Yoshiaki Kon, Kenzo Sanematsu, Yoshio Takahashi, Motoo Ito. Microscopic analyses of weathered granite in ion-adsorption rare earth deposit of Jianxi Province, China. Scientific Reports 2020, 10 (1) https://doi.org/10.1038/s41598-020-76981-8
  5. J. Neumann, H. Brinkmann, S. Britz, J. Lützenkirchen, F. Bok, M. Stockmann, V. Brendler, T. Stumpf, M. Schmidt. A comprehensive study of the sorption mechanism and thermodynamics of f-element sorption onto K-feldspar. Journal of Colloid and Interface Science 2020, https://doi.org/10.1016/j.jcis.2020.11.041
  6. Wanqiang Zhou, Dongfan Xian, Xuebin Su, Yao Li, Weimin Que, Yanlin Shi, Jingyi Wang, Chunli Liu. Macroscopic and spectroscopic characterization of U(VI) sorption on biotite. Chemosphere 2020, 255 , 126942. https://doi.org/10.1016/j.chemosphere.2020.126942
  7. K. Molodtsov, S. Schymura, J. Rothe, K. Dardenne, M. Schmidt. Sorption of Eu(III) on Eibenstock granite studied by µTRLFS: A novel spatially-resolved luminescence-spectroscopic technique. Scientific Reports 2019, 9 (1) https://doi.org/10.1038/s41598-019-42664-2
  8. Hong Li, Bihong He, Ping Li, Qiaohui Fan, Hanyu Wu, Jianjun Liang, Chunli Liu, Tao Yu. Adsorption behaviors of Eu(III) on granite: batch, electron probe micro-analysis and modeling studies. Environmental Earth Sciences 2019, 78 (8) https://doi.org/10.1007/s12665-019-8170-y
  9. Chunfang Wu, Yawen Cai, Lin Xu, Jian Xie, Zhiyong Liu, Shitong Yang, Shuao Wang. Macroscopic and spectral exploration on the removal performance of pristine and phytic acid-decorated titanate nanotubes towards Eu(III). Journal of Molecular Liquids 2018, 258 , 66-73. https://doi.org/10.1016/j.molliq.2018.02.110
  10. Ping Li, Hanyu Wu, Jianjun Liang, Zhuoxin Yin, Duoqiang Pan, Qiaohui Fan, Di Xu, Wangsuo Wu. Sorption of Eu(III) at feldspar/water interface: effects of pH, organic matter, counter ions, and temperature. Radiochimica Acta 2017, 105 (12) https://doi.org/10.1515/ract-2017-2797
  11. Yawen Cai, Fang Yuan, Xiaomei Wang, Zhuang Sun, Yang Chen, Zhiyong Liu, Xiangke Wang, Shitong Yang, Shuao Wang. Synthesis of core–shell structured [email protected] cellulose magnetic composite for highly efficient removal of Eu(III). Cellulose 2017, 24 (1) , 175-190. https://doi.org/10.1007/s10570-016-1094-8
  12. Qiang Jin, Lin Su, Gilles Montavon, Yufeng Sun, Zongyuan Chen, Zhijun Guo, Wangsuo Wu. Surface complexation modeling of U(VI) adsorption on granite at ambient/elevated temperature: Experimental and XPS study. Chemical Geology 2016, 433 , 81-91. https://doi.org/10.1016/j.chemgeo.2016.04.001
  13. Takashi Munemoto, Kazuaki Ohmori, Teruki Iwatsuki. Rare earth elements (REE) in deep groundwater from granite and fracture-filling calcite in the Tono area, central Japan: Prediction of REE fractionation in paleo- to present-day groundwater. Chemical Geology 2015, 417 , 58-67. https://doi.org/10.1016/j.chemgeo.2015.09.024
  14. Toshihiko Ohnuki, Mingyu Jiang, Fuminori Sakamoto, Naofumi Kozai, Shinya Yamasaki, Qianqian Yu, Kazuya Tanaka, Satoshi Utsunomiya, Xiaobin Xia, Ke Yang, Jianhua He. Sorption of trivalent cerium by a mixture of microbial cells and manganese oxides: Effect of microbial cells on the oxidation of trivalent cerium. Geochimica et Cosmochimica Acta 2015, 163 , 1-13. https://doi.org/10.1016/j.gca.2015.04.043
  15. Q. H. Fan, X. L. Zhao, X. X. Ma, Y. B. Yang, W. S. Wu, G. D. Zheng, D. L. Wang. Comparative adsorption of Eu( iii ) and Am( iii ) on TPD. Environmental Science: Processes & Impacts 2015, 17 (9) , 1634-1640. https://doi.org/10.1039/C5EM00240K
  16. Qiang Jin, Gang Wang, Mengtuan Ge, Zongyuan Chen, Wangsuo Wu, Zhijun Guo. The adsorption of Eu(III) and Am(III) on Beishan granite: XPS, EPMA, batch and modeling study. Applied Geochemistry 2014, 47 , 17-24. https://doi.org/10.1016/j.apgeochem.2014.05.004

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