Nanocrystalline Ce(OH)4-based materials: ruthenium selective adsorbent for highly alkaline radioactive liquid waste
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Jayaprakasam Selvakumar
, Kumari Anshul
, Padala A. Nishad , Bhaskarapillai Anupkumar , Subramanian Srinivasan , Nethapakkam R. Jawahar , Appadurai L. Rufus , Jayantha K. Gayen and Tulasi V. Krishna Mohan
Abstract
Cerium hydroxide, Ce(OH)4 (Ce), has been synthesised and assessed as a Ru-selective adsorbent for treating alkaline radioactive liquid waste. Infrared spectroscopy, thermal analysis, scanning electron microscopy, and energy-dispersive X-ray spectroscopy investigations confirmed the successful formation of nanocrystalline Ce from Ce(NO3)3·6H2O. Selective removal of 106Ru from the ion-exchange effluent of intermediate-level liquid waste (ILW) by Ce was assessed using a high-pure germanium (HPGe) gamma-ray spectrometer. The calculated average distribution coefficient (kD) was ∼200 mL/g. The percentage removal of 106Ru using Ce by varying time, [106Ru] and [Ce] was calculated. The adsorption of 106Ru on Ce follows pseudo-second-order and Freundlich isotherms. The calculated Qmax was 93,584 Bq/g. Accelerated leaching studies of the Ru-laden Ce cement product were carried out and found suitable for transport and disposal. Further, Ce-Polyether sulphone (Ce-PES) and Ce-Chitosan (CeC) composites were prepared and assessed for their Ru-uptake capacity for engineering scale application.
Acknowledgments
The authors are grateful to G. Suneel Superintendent (O), WIP-K, NRB, for his encouragement during the experiments.
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Research ethics: Not applicable.
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Author contributions: The authors have accepted responsibility for the entire content of this manuscript and approved its submission.
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Competing interests: The authors state no conflict of interest.
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Research funding: None declared.
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Data availability: Not applicable.
References
1. Selvakumar, J., Raghukumar, P., Usha, K., Chitra, S., Gayen, J. K., Ravi, K. V. Sn–Al–P–O, cerium, and zirconium-based materials for the treatment of low-level radioactive liquid waste. In Proceedings of the 8th DAE-BRNS Interdisciplinary Symposium on Materials Chemistry, Bhabha Atomic Research Centre, Mumbai, India, June 17–19, 2021.Search in Google Scholar
2. Sonika, G., Selvakumar, J., Rajasekaran, S., Gayen, J. K., Roy, A., Sonavane, M. S. Study on treatment of intermediate level waste. In Proceedings of the 12th DAE-BRNS National Symposium on Nuclear and RadioChemistry. Bhabha Atomic Research Centre, Mumbai, India, February 9–13, 2015.Search in Google Scholar
3. National Institute of Advanced Industrial Science and Technology Atlas of Eh-pH Diagrams, Intercomparison of Thermodynamic Databases, Geological Survey of Japan Open File Report No. 419; Research Center for Deep Geological Environments: Naoto Takeno, 2005.Search in Google Scholar
4. Verma, P. K., Mohapatra, P. K. Ruthenium speciation in radioactive wastes and state-of-the-art strategies for its recovery: a review. Sep. Purif. Technol. 2021, 275, 119148; https://doi.org/10.1016/j.seppur.2021.119148.Search in Google Scholar
5. Motoki, R., Motoishi, S., Izumo, M., Onoma, K., Sato, T. Method of processing radioactive liquid wastes containing radioactive ruthenium. U.S. Patent, 4,622,176, November 11, 1986.Search in Google Scholar
6. Siczek, A. A., Steindler, M. J. The chemistry of ruthenium and zirconium in the PUREX solvent extraction process. At. Energy Rev. 1978, 16, 575.Search in Google Scholar
7. Boswell, G. G. J., Soentono, S. Ruthenium nitrosyl complexes in nitric acid solutions. J. Inorg. Nucl. Chem. 1981, 43, 1625; https://doi.org/10.1016/0022-1902(81)80350-8.Search in Google Scholar
8. Lefebvre, C., Dumas, T., Tamain, C., Ducres, T., Solari, P. L., Charbonnel, M. C. Addressing ruthenium speciation in tri-n-butyl-phosphate solvent extraction process by Fourier transform infrared, extended X-ray absorption fine structure, and single crystal X-ray diffraction. Ind. Eng. Chem. Res. 2017, 56, 11292; https://doi.org/10.1021/acs.iecr.7b02973.Search in Google Scholar
9. Das, D., Biswas, S., Dumpala, R. M. R., Pente, A. S., Manohar, S. Separation of radioactive ruthenium from alkaline solution: a solvent extraction and detailed mechanistic approach. ACS Omega 2022, 48, 43803; https://doi.org/10.1021/acsomega.2c04903.Search in Google Scholar PubMed PubMed Central
10. Madic, C., Mun, C., Cantrel, L. Review of literature on ruthenium behaviour in nuclear power plant severe accidents. Nucl. Technol. 2017, 156, 332.10.13182/NT156-332Search in Google Scholar
11. Samanta, S. K., Theyyunni, T. K. Removal of Radio-Ruthenium from Alkaline Intermediate-Level Radioactive Waste Solution: A Laboratory Investigation; BARC Technical Report, 1994; p. 1.Search in Google Scholar
12. Balarama Krishna, M. V., Arunachalam, J., Prabhu, D. R., Manchanda, V. K., Kumar, S. Removal of 106Ru from actual low-level radioactive waste solutions using polyaniline as anion–exchanger. Sep. Sci. Technol. 2005, 40, 1313; https://doi.org/10.1081/ss-200053317.Search in Google Scholar
13. Lee, S. H., Chung, H. Ion exchange characteristics of palladium and ruthenium from a simulated radioactive liquid waste. Sep. Sci. Technol. 2003, 38, 3459; https://doi.org/10.1081/ss-120023411.Search in Google Scholar
14. Verma, P. K., Mohapatra, P. K. Highly efficient separation of ruthenium from alkaline radioactive feeds using an anion exchange resin. Radiochim. Acta 2020, 108, 603; https://doi.org/10.1515/ract-2019-3182.Search in Google Scholar
15. Sun, Q., Zhu, L., Aguila, B., Thallapally, P. K., Xu, C., Chen, J., Wang, S., Roger, D., Ma, S. Optimizing radionuclide sequestration in anion nanotraps with record pertechnetate sorption. Nat. Commun. 2019, 10, 1646; https://doi.org/10.1038/s41467-019-09630-y.Search in Google Scholar PubMed PubMed Central
16. Niu, X., Elakneswaran, Y., Raudhatul, C., Provis, J. L., Sato, T. Adsorption behaviour of simulant radionuclide cations and anions in metakaolin-based geopolymer. J. Hazard. Mater. 2022, 429, 128373; https://doi.org/10.1016/j.jhazmat.2022.128373.Search in Google Scholar PubMed
17. Yang, J., Tai, W., Wu, F., Shi, K., Jia, T., Su, Y., Liu, T., Mocilac, P., Hou, X., Chen, X. Enhanced removal of radioactive iodine anions from wastewater using modified bentonite: experimental and theoretical study. Chemosphere 2022, 292, 133401; https://doi.org/10.1016/j.chemosphere.2021.133401.Search in Google Scholar PubMed
18. Hamed, M. M., Holiel, M., El-Aryan, Y. F. Removal of selenium and iodine radionuclides from waste solutions using synthetic inorganic ion exchanger. J. Mol. Liq. 2017, 242, 722; https://doi.org/10.1016/j.molliq.2017.07.035.Search in Google Scholar
19. Jiang, M., Fang, Z., Liu, Z., Huang, X., Wei, H., Yu, C. Y. Application of membrane distillation for purification of radioactive liquid. Clean. Eng. Technol. 2023, 12, 100589; https://doi.org/10.1016/j.clet.2022.100589.Search in Google Scholar
20. Hassan, R. S., Abass, M. R., Eid, M. A., Abdel-Galil, E. A. Sorption of some radionuclides from liquid waste solutions using anionic clay hydrotalcite sorbent. Appl. Radiat. Isot. 2021, 178, 109985; https://doi.org/10.1016/j.apradiso.2021.109985.Search in Google Scholar PubMed
21. Hamed, M. M., Ahmed, I. M., Holiel, M. Retention behavior of anionic radionuclides using metal hydroxide sludge. Radiochim. Acta 2019, 107, 1161; https://doi.org/10.1515/ract-2019-0010.Search in Google Scholar
22. Zhang, X., Ma, J., Lu, X., Huangfu, X., Zou, J. High efficient removal of molybdenum from water by Fe2(SO4)3: effects of pH and affecting factors in the presence of co-existing background constituents. J. Hazard. Mater. 2015, 300, 823; https://doi.org/10.1016/j.jhazmat.2015.08.026.Search in Google Scholar PubMed
23. Wu, C. H., Lo, S. L., Lin, C. F. Competitive adsorption of molybdate, chromate, sulfate, selenate, and selenite on γ-Al2O3. Colloids Surf. A: Physicochem. Eng. 2000, 166, 251; https://doi.org/10.1016/s0927-7757(99)00404-5.Search in Google Scholar
24. Xu, M., Cai, Y., Chen, G., Li, B., Chen, Z., Hu, B., Wang, X. Efficient selective removal of radionuclides by sorption and catalytic reduction using nanomaterials. Nanomaterials 2022, 12, 1443; https://doi.org/10.3390/nano12091443.Search in Google Scholar PubMed PubMed Central
25. Yu, Y., Yu, L., Koh, K. Y., Wang, C., Chen, J. P. Rare-earth metal-based adsorbents for effective removal of arsenic from water: a critical review. Crit. Rev. Environ. Sci. Technol. 2018, 48, 1127; https://doi.org/10.1080/10643389.2018.1514930.Search in Google Scholar
26. Moeller, T., Ferrus, R. Observations on the rare earths – LXXIII the heat and entropy of formation of the 1:1 chelates of N-hydroxyethylethylenediaminetriacetic acid with the tri-positive cations. J. Inorg. Nucl. Chem. 1961, 20, 261; https://doi.org/10.1016/0022-1902(61)80275-3.Search in Google Scholar
27. Li, R., Li, Q., Gao, S., Shang, J. K. Exceptional arsenic adsorption performance of hydrous cerium oxide nanoparticles: part A. Adsorption capacity and mechanism. Chem. Eng. J. 2012, 185–186, 127; https://doi.org/10.1016/j.cej.2012.01.061.Search in Google Scholar
28. Kurian, M. Cerium oxide-based materials for water treatment – a review. J. Environ. Chem. Eng. 2020, 8, 104439; https://doi.org/10.1016/j.jece.2020.104439.Search in Google Scholar
29. Koh, K. Y., Yang, Y., Chen, J. P. Critical review on lanthanum-based materials used for water purification through adsorption of inorganic contaminants. Crit. Rev. Environ. Sci. Technol. 2021, 52, 1773; https://doi.org/10.1080/10643389.2020.1864958.Search in Google Scholar
30. Psaras, D., Gao, Y., Haneline, M., Lupo, J., Landi, C. Removal of arsenic from aqueous streams with cerium (IV) oxide compositions. U.S. Patent, 1,0577,259 B2, March 3, 2020.Search in Google Scholar
31. Sonar, N. L., De, V., Pardeshi, V. Analysis of 99Tc in the radioactive liquid waste after extraction into suitable solvent. J. Radioanal. Nucl. Chem. 2012, 294, 185; https://doi.org/10.1007/s10967-011-1583-z.Search in Google Scholar
32. Selvakumar, J., Rajasekaran, S., Chitra, S., Biplop, P. Simulated studies on optimisation and characterisation of feed and product of melter for safe disposal of high-level liquid waste. Prog. Nucl. Energy 2020, 118, 103136; https://doi.org/10.1016/j.pnucene.2019.103135.Search in Google Scholar
33. Ansari, A. A., Kaushik, A. Synthesis and optical properties of nanostructured Ce(OH)4. J. Semicond. 2010, 31, 033001; https://doi.org/10.1088/1674-4926/31/3/033001.Search in Google Scholar
34. Ma, J., Wang, C., Xi, W., Zhao, Q., Wang, S., Qiu, M., Wang, J., Wang, X. Removal of radionuclides from aqueous solution by manganese dioxide-based nanomaterials and mechanism research: a review. ACS EST Eng. 2021, 4, 685; https://doi.org/10.1021/acsestengg.0c00268.Search in Google Scholar
35. Da̧browski, A. Adsorption – from theory to practice. Adv. Colloid Interface Sci. 2001, 93, 135.10.1016/S0001-8686(00)00082-8Search in Google Scholar
36. Boparai, H. K., Joseph, M., O’Carroll, D. M. Kinetics and thermodynamics of cadmium ion removal by adsorption onto nano zerovalent iron particles. J. Hazard. Mater. 2011, 186, 458; https://doi.org/10.1016/j.jhazmat.2010.11.029.Search in Google Scholar PubMed
37. Worch, E. Adsorption equilibrium I: general aspects and single-solute adsorption. In Adsorption Technology in Water Treatment, Fundamental, Processes, and Modeling; De Gruyter: Berlin/Boston, 2012.Search in Google Scholar
38. Ayawei, N., Angaye, S. S., Wankasi, D., Dikio, E. D. Synthesis, characterization and application of Mg/Al layered double hydroxide for the degradation of Congo-red in aqueous solution. Open J. Phys. Chem. 2015, 5, 56; https://doi.org/10.4236/ojpc.2015.53007.Search in Google Scholar
39. Ho, Y. S., McKay, G. A comparison of chemisorption kinetic models applied to pollutant removal on various sorbents. Process Saf. Environ. Prot. 1998, 76, 332; https://doi.org/10.1205/095758298529696.Search in Google Scholar
© 2023 Walter de Gruyter GmbH, Berlin/Boston
Articles in the same Issue
- Frontmatter
- Preface
- NUCAR-2023: Foreword
- Research Articles
- Theoretical analysis of light and heavy-ion induced reactions: production of medically relevant 97Ru
- Excitation functions of alpha-particle induced nuclear reactions on nat Sn
- Non-destructive assay of plutonium in absence of gamma-ray spectrometry
- Catalytic destruction of oxalate in the supernatant stream generated during plutonium reconversion process
- Quantification of Zr in simulated dissolver solution of U–Zr fuel by laser-induced breakdown spectroscopy
- Radiochemical and chemical characterization of fuel, salt, and deposit from the electrorefining of irradiated U-6 wt% Zr in hot cells
- Zirconium sponge production: an integrated approach for chemical characterization of process intermediates using ICP-OES
- Determination of 10B/11B in boric acid and B4C using LA-ICPMS
- Evaluating sustainability of Bhuj aquifer system, Western India using nuclear dating techniques
- Nanocrystalline Ce(OH)4-based materials: ruthenium selective adsorbent for highly alkaline radioactive liquid waste
- Production and radiochemical separation of 68Ge from irradiated Ga–Ni alloy target in 30 MeV cyclotron
- Preparation of [64Cu]Cu–NOTA complex as a potential renal PET imaging agent using 64Cu produced via the direct activation route
- Total chemical synthesis of PSMA-617: an API for prostate cancer endotherapeutic applications
- Rapid screening technique for gross α and gross β estimations in aqueous samples during radiation emergency
- Development of Dy3+ doped lithium magnesium borate glass system for thermoluminescence based neutron dosimetry applications
Articles in the same Issue
- Frontmatter
- Preface
- NUCAR-2023: Foreword
- Research Articles
- Theoretical analysis of light and heavy-ion induced reactions: production of medically relevant 97Ru
- Excitation functions of alpha-particle induced nuclear reactions on nat Sn
- Non-destructive assay of plutonium in absence of gamma-ray spectrometry
- Catalytic destruction of oxalate in the supernatant stream generated during plutonium reconversion process
- Quantification of Zr in simulated dissolver solution of U–Zr fuel by laser-induced breakdown spectroscopy
- Radiochemical and chemical characterization of fuel, salt, and deposit from the electrorefining of irradiated U-6 wt% Zr in hot cells
- Zirconium sponge production: an integrated approach for chemical characterization of process intermediates using ICP-OES
- Determination of 10B/11B in boric acid and B4C using LA-ICPMS
- Evaluating sustainability of Bhuj aquifer system, Western India using nuclear dating techniques
- Nanocrystalline Ce(OH)4-based materials: ruthenium selective adsorbent for highly alkaline radioactive liquid waste
- Production and radiochemical separation of 68Ge from irradiated Ga–Ni alloy target in 30 MeV cyclotron
- Preparation of [64Cu]Cu–NOTA complex as a potential renal PET imaging agent using 64Cu produced via the direct activation route
- Total chemical synthesis of PSMA-617: an API for prostate cancer endotherapeutic applications
- Rapid screening technique for gross α and gross β estimations in aqueous samples during radiation emergency
- Development of Dy3+ doped lithium magnesium borate glass system for thermoluminescence based neutron dosimetry applications