Abstract
In this study, the effect of light on the kinetics and speciation of plutonium at its interaction with particles of TiO2 under different light conditions is shown for the first time. It was found that sorption was followed by reduction of the plutonium to Pu(IV). In this, the reduction reaction and sorption in conditions of the presence of light proceed significantly more rapidly due to the photocatalytic activity of titanium dioxide, providing a source of electrons for the reaction. Spectral methods (XAFS and TEM) showed that plutonium forms nanoclusters with the structure of PuO2, which decorate the surface of the solid phase.
Funding source: Russian Science Foundation
Award Identifier / Grant number: 14-13-01279
Funding statement: This work was supported by the Russian Science Foundation (project 14-13-01279). We also acknowledge the “Nanochemistry and nanomaterials” user facility of the Department of Chemistry of MSU for providing the HRTEM measurements.
Acknowledgments
This work was supported by the Russian Science Foundation (project 14-13-01279). We also acknowledge the “Nanochemistry and nanomaterials” user facility of the Department of Chemistry of MSU for providing the HRTEM measurements.
References
1. Geckeis, H., Rabung, T.: Actinide geochemistry: From the molecular level to the real system. J. Contam. Hydrol. 102, 187 (2008).10.1016/j.jconhyd.2008.09.011Search in Google Scholar PubMed
2. Clark, D. L., Hecker, S. S., Jarvinen, G. D., Neu, M. P.: Plutonium. In: L. R. Morss, N. M. Edelstein, J. Fuger (Eds.), The Chemistry of the Actinide and Transactinide Elements, (2006) Springer, Dordrecht, The Netherlands.10.1007/1-4020-3598-5_7Search in Google Scholar
3. Hixon, A. E., Arai, Y., Powell, B. A.: Examination of the effect of alpha radiolysis on plutonium(V) sorption to quartz using multiple plutonium isotopes. J. Colloid Interf. Sci. 403, 105 (2013).10.1016/j.jcis.2013.04.007Search in Google Scholar PubMed
4. Powell, B. A., Fjeld, R. A., Kaplan, D. I., Coates, J. T., Serkiz, S. M.: Pu(V)O2+ adsorption and reduction by synthetic hematite and goethite. Environ. Sci. Technol. 39, 2107 (2005).10.1021/es0487168Search in Google Scholar PubMed
5. Romanchuk, A. Yu., Kalmykov, S. N., Aliev, R. A.: Plutonium sorption onto hematite colloids onto femto- and nanomolar concentrations. Radiochim. Acta 99, 137 (2011).10.1524/ract.2011.1808Search in Google Scholar
6. Romanchuk, A. Yu., Kalmykov, S. N., Egorov, A. V., Zubavichus, Y. V., Shiryaev, A. A., Batuk, O. N., Conradson, S. D., Pankratov, D. A., Presnyakov, I. A.: Formation of crystalline PuO2+x·nH2O nanoparticles upon sorption of Pu(V,VI) onto hematite. Geochim. Cosmochim. Acta 121, 29 (2013).10.1016/j.gca.2013.07.016Search in Google Scholar
7. Zavarin, M., Powell, B. A., Bourbin, M., Zhao, P., Kersting, A. B.: Np(V) and Pu(V) ion exchange and surface-mediated reduction mechanisms on montmorillonite. Environ. Sci. Technol. 46, 2692 (2012).10.1021/es203505gSearch in Google Scholar PubMed
8. Novikov, A. P., Kalmykov, S. N., Utsunomiya, S., Ewing, R. C., Horreard, F., Merkulov, A., Clark, S. B., Tkachev, V. V., Myasoedov, B. F.: Colloid transport of plutonium in the far-field of the Mayak Production Association, Russia. Science 314, 638 (2006).10.1126/science.1131307Search in Google Scholar PubMed
9. Payne, T. E., Davis, J. A., Lumpkin, G., Chisari, R., Waite, T. D.: Surface complexation model of uranyl sorption on Georgia kaolinite. Appl. Clay Sci. 64, 151 (2004).10.1016/j.clay.2003.08.013Search in Google Scholar
10. Wold, A.: Photocatalytic properties of titanium dioxide (TiO2). Chem. Mater. 5, 280 (1993).10.1021/cm00027a008Search in Google Scholar
11. Yu, J., Low, J., Xiao, W., Zhou, P., Jaroniec, M.: Enhanced photocatalytic CO2-reduction activity of anatase TiO2 by coexposed {001} and {101} facets. J. Am. Chem. Soc. 136, 8839 (2014).10.1021/ja5044787Search in Google Scholar PubMed
12. Eliet, V., Bidoglio, G.: Kinetics of the laser-induced photoreduction of U(VI) in aqueous suspensions of TiO2 particles. Environ. Sci. Technol. 32, 3155 (1998).10.1021/es970929sSearch in Google Scholar
13. Gracheva, N. N., Romanchuk, A. Y., Smirnov, E. A., Meledina, M. A., Garshev, A. V., Shirshin, E. A., Fadeev, V. V., Kalmykov, S. N.: Am(III) sorption onto TiO2 samples with different crystallinity and varying pore size distributions. Appl. Geochem. 42, 69 (2014).10.1016/j.apgeochem.2014.01.006Search in Google Scholar
14. Roof, R. B.: X-ray diffraction data for plutonium compounds. Los Alamos National LAboratory, Report LA-11619 (1989).10.2172/7257520Search in Google Scholar
15. Neck, V., Altmaier, M., Fanghanel, T.: Solubility of plutonium hydroxides/hydrous oxides under reducing conditions and in the presence of oxygen. C. R. Chim. 10, 959 (2007).10.1016/j.crci.2007.02.011Search in Google Scholar
Supplemental Material:
The online version of this article (DOI: 10.1515/ract-2015-2494) offers supplementary material, available to authorized users.
©2016 Walter de Gruyter GmbH, Berlin/Boston
Articles in the same Issue
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Articles in the same Issue
- Frontmatter
- Influence of the goethite (α-FeOOH) surface on the stability of distorted PuO2 and PuO2–x phases
- Photoreduction of Pu(V,VI) by TiO2
- Experimental measurements of U24Py nanocluster behavior in aqueous solution
- Comparision in the solvent extraction behavior of uranium (VI) in some trialkyl phosphates in ionic liquid
- Sorption behavior of cesium, cobalt and europium radionuclides onto hydroxyl magnesium silicate
- Separation of no-carrier-added 203Pb, a surrogate radioisotope, from proton irradiated natTl2CO3 target using calcium alginate hydrogel beads
- Synthesis and in vitro evaluation of no-carrier-added 2-(3-(4-(4-[18F]fluorobenzyl)piperazin-1-yl)propyl)benzo[d]thiazole, a potential dopamine D4 receptor radioligand
- Silver-based getters for 129I removal from low-activity waste