Abstract
Purpose
There is a large quantity of contaminated soil with radionuclides due to the accident of Fukushima Daiichi Nuclear Power Plant in Japan. Some previous studies reported that Cs+ could be desorbed from soil with high efficiency; however, these methods required huge input energy for operating. Therefore, we focused on oxalic acid, which has shown relatively high desorption efficiency in previous thermal treatment, and evaluated the potential of oxalic acid as a leaching reagent to reduce the volume of contaminated soil without heating.
Methods
Stable isotope Cs+ contaminated biotite was retained in a plastic bag for 3 months for aging. Oxalic acid was added to the contaminated biotite, and the mixture was maintained around 20 °C. After each leaching time, the mixture was separated using filter paper, and the concentration of Cs+ in filtrate was measured. Structural changes in biotite before and after leaching were also analyzed. LiNO3 was also used for comparison studies.
Results
The desorption efficiency of Cs+ from biotite by leaching with oxalic acid was 94.9% after 2 weeks, and the intensity of the specific reflection for biotite in the X-ray diffractograms decreased with leaching time. These results indicate that oxalic acid can remove Cs+ from biotite through the decomposition of the biotite structure. Since LiNO3 desorbed only 32.2% of Cs+ as ion-exchangeable form after 2 weeks, oxalic acid can desorb Cs+, which has a strong interaction with biotite such as the inner-sphere complex, without heating.
Conclusion
Although the desorption of Cs+ from biotite by leaching with oxalic acid leaching takes a long time, it is a great advantage that this leaching method does not require external energy such as heating. Therefore, oxalic acid leaching has high potential to reduce the volume of contaminated soil with radionuclides.
This is a preview of subscription content, log in via an institution to check access.
Availability of data and materials
The datasets used and/or analyzed during the current study are available from the corresponding author on reasonable request.
References
Akemoto Y, Iwamura T, Takahashi S, Kan M, Tanaka S (2021a) Desorption of Cs+ from contaminated biotite with a low molecular mass organic acid. J Environ Chem Eng 9:106101. https://doi.org/10.1016/j.jece.2021.106101
Akemoto Y, Sakti SCW, Kan M, Tanaka S (2021b) Interpretation of the interaction between cesium ion and some clay minerals based on their structural features. Environ Sci Pollut Res 28:14121–14130. https://doi.org/10.1007/s11356-020-11476-7
Bernard E, Zucha WJ, Lothenbach B, Mäder U (2022) Stability of hydrotalcite (Mg-Al layered double hydroxide) in presence of different anions. Cem Concr Res 152:106674. https://doi.org/10.1016/j.cemconres.2021.106674
da Costa LG, Brocco VF, Paes JB, Kirker GT, Bishell AB (2022) Biological and chemical remediation of CCA treated eucalypt poles after 30 years in service. Chemosphere 286:131629. https://doi.org/10.1016/j.chemosphere.2021.131629
Fan Q, Yamaguchi N, Tanaka M, Tsukada H, Takahashi Y (2014) Relationship between the adsorption species of cesium and radiocesium interception potential in soils and minerals : an EXAFS study. J Environ Radioact 138:92–100. https://doi.org/10.1016/j.jenvrad.2014.08.009
Huang M, Zhu C, Zhu F, Fang G, Zhou D (2021) Mechanism of significant enhancement of VO2-Fenton-like reactions by oxalic acid for diethyl phthalate degradation. Sep Purif Technol 279:119671. https://doi.org/10.1016/j.seppur.2021.119671
Japan Ministry of the Environment (2018) Volume reduction and recycling technology development strategy. http://josen.env.go.jp/chukanchozou/facility/effort/investigative_commission/pdf/proceedings_181217_04.pdf. Accessed 29 Nov 2021
Japan Ministry of the Environment (2019) Volume reduction and recycling technology development strategy for intermediate storage and removal soil, etc. Review to achieve strategic goals. http://josen.env.go.jp/chukanchozou/facility/effort/investigative_commission/pdf/investigative_commission_review_1903.pdf. Accessed 29 Nov 2021
Kim S-M, Yoon I-H, Kim I-G, Park C-W, Shin Y-H, Kim J-H, Park S-J (2020) Cs desorption behavior during hydrothermal treatment of illite with oxalic acid. Environ Sci Pollut Res 27:35580–35590. https://doi.org/10.1007/s11356-020-09675-3
Kitayama R, Yanai J, Nakao A (2020) Ability of micaceous minerals to adsorb and desorb caesium ions: effects of mineral type and degree of weathering. Eur J Soil Sci 71:641–653. https://doi.org/10.1111/ejss.12913
Kogure T, Morimoto K, Tamura K, Sato H, Yamagishi A (2012) XRD and HRTEM evidence for fixation of cesium ions in vermiculite clay. Chem Lett 41:380–382. https://doi.org/10.1246/cl.2012.380
Lee SO, Tran T, Park YY, Kim SJ, Kim MJ (2006) Study on the kinetics of iron oxide leaching by oxalic acid. Int J Miner Process 80:144–152. https://doi.org/10.1016/j.minpro.2006.03.012
Ma JF, Zheng SJ, Matsumoto H, Hiradate S (1997) Detoxifying aluminium with buckwheat. Nature 390:569–570. https://doi.org/10.1038/37518
Miyata S (1983) Anion-exchange properties of hydrotalcite-like compounds. Clays Clay Miner 31:305–311. https://doi.org/10.1346/CCMN.1983.0310409
Mukai H, Tamura K, Kikuchi R, Takahashi Y, Yaita T, Kogure T (2018) Cesium desorption behavior of weathered biotite in Fukushima considering the actual radioactive contamination level of soils. J Environ Radioact 190–191:81–88. https://doi.org/10.1016/j.jenvrad.2018.05.006
Parajuli D, Takahashi A, Tanaka H, Sato M, Fukuda S, Kamimura R, Kawamoto T (2015) Variation in available cesium concentration with parameters during temperature induced extraction of cesium from soil. J Environ Radioact 140:78–83. https://doi.org/10.1016/j.jenvrad.2014.11.005
Shimoyama I, Hirano N, Baba Y, Izumi T, Okamoto Y, Yaita T, Suzuki S (2014) Low-pressure sublimation method for cesium decontamination of clay minerals. Clay Sci 18:71–77. https://doi.org/10.11362/jcssjclayscience.18.3_71
Tamura K, Yamashita H, Kogure T, Motita M, Yamagishi A, Sato H (2021) Removal of ceisum ions from radioactively contaminated soils using microwave treatment. Clay Sci 25:7–11. https://doi.org/10.11362/jcssjclayscience.MS-21-2
Yin X, Wang X, Wu H, Ohnuki T, Takeshita K (2017) Enhanced desorption of cesium from collapsed interlayer regions in vermiculite by hydrothermal treatment with divalent cations. J Hazard Mater 326:47–53. https://doi.org/10.1016/j.jhazmat.2016.12.017
Acknowledgements
The analysis of biotite was performed by using an XRF and XRD at the “Joint-use Facilities: Laboratory of Nano-Micro Material Analysis,” and “The High Brilliance X-Ray Laboratory”, Hokkaido University, supported by “Material Analysis and Structure Analysis Open Unit (MASAOU)”. We would like to thank Editage (www.editage.com) for the English language editing.
Author information
Authors and Affiliations
Contributions
Yasuhiro Akemoto: conceptualization, methodology, formal analysis and investigation, writing — original draft preparation, visualization. Seira Takahashi: methodology, investigation Toko Iwamura: methodology, investigation Masahiko Kan: writing —review and editing Shunitz Tanaka: methodology, writing —review and editing, supervision
Corresponding authors
Ethics declarations
Competing interests
The authors declare no competing interests.
Additional information
Responsible editor: Peng Cai
Publisher's Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Supplementary information
Below is the link to the electronic supplementary material.
Rights and permissions
About this article
Cite this article
Akemoto, Y., Takahashi, S., Iwamura, T. et al. Extraction of Cs bound with biotite by addition of oxalic acid without heating. J Soils Sediments 22, 1787–1791 (2022). https://doi.org/10.1007/s11368-022-03196-x
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s11368-022-03196-x