Hostname: page-component-78c5997874-t5tsf Total loading time: 0 Render date: 2024-11-08T15:30:17.429Z Has data issue: false hasContentIssue false
  • English
  • Français

Direct mass analysis of water absorption onto ceria thin films

Published online by Cambridge University Press:  05 January 2017

D. Laventine ,
R. Wilbraham ,
C. Boxall ,
R. Taylor  and
R. Orr.
D. Laventine*
Affiliation:
University of Lancaster, Department of Engineering, Lancaster, LA1 4YR, UK
R. Wilbraham
Affiliation:
University of Lancaster, Department of Engineering, Lancaster, LA1 4YR, UK
C. Boxall
Affiliation:
University of Lancaster, Department of Engineering, Lancaster, LA1 4YR, UK
R. Taylor
Affiliation:
National Nuclear Laboratory, Central laboratory, B170, Sellafield, CA20 1PG, UK
R. Orr.
Affiliation:
National Nuclear Laboratory, Central laboratory, B170, Sellafield, CA20 1PG, UK
*
*(Email: [email protected])
Get access

Abstract

Plutonium oxide (PuO2) is one of the most highly radioactive components of nuclear fuel waste streams and its storage poses particular challenges due to the high temperatures produced by its decay and the production of gases (particularly H2 and steam). Its high radiotoxicity necessitates the use of analogues, such as CeO2, to allow the comprehensive study of its interaction with water under storage conditions.

We have developed a method which enables direct gravimetric measurement of water adsorption onto CeO2 thin films with masses in the microgram region. Porous CeO2 films were fabricated from a surfactant based precursor solution. The absorption of water onto the CeO2 coating at different relative humidities was studied in a closed reactor. Quartz Crystal Microbalance (QCM) gravimetry was used as a signal transducer, as changes in crystal resonant frequency due to absorbed mass are directly and linearly related to mass changes occurring at the crystal surface. Using this method, we have determined the enthalpy of absorption of water onto CeO2 to be 49.7 kJmol–1 at 75°C, 11 kJmol-1 greater than the enthalpy of evaporation. This enthalpy is within the range predicted for the absorption of water onto PuO2, indicating this method allows for investigation of water absorption using microgram samples.

Keywords

nuclear materialspiezoelectricwaste management
Type
Articles
Information
MRS Advances , Volume 2 , Issue 12: Scientific Basis for Nuclear Waste Management XL , 2017 , pp. 649 - 654
Copyright
Copyright © Materials Research Society 2017 

Access options

Get access to the full version of this content by using one of the access options below. (Log in options will check for institutional or personal access. Content may require purchase if you do not have access.)

References

REFERENCES

I. A. E. Agency, Annual Report for: International Atomic Energy Agency., 1998.Google Scholar
Stakebake, J. L., McClard, J., and Szempruch, R. W., Abstracts of Papers of the American Chemical Society, vol. 219, pp. U70–U70, 2000.Google Scholar
Hyatt, N. C., Energy Policy , 2016.Google Scholar
Kim, H. S., Joung, C. Y., Lee, B. H., Oh, J. Y., Koo, Y. H., and Heimgartner, P., J. Nucl. Mater., vol. 378, pp. 98–104, 2008.Google Scholar
Sakai, N., Yamaji, K., Horita, T., Yokokawa, H., Hirata, Y., Sameshima, S., et al. ., Solid State Ionics, vol. 125, pp. 325–331, 10, 1999.CrossRefGoogle Scholar
Prin, M., Pijolat, M., Soustelle, M., and Touret, O., Thermochimica Acta, vol. 186, pp. 273–283, 1991.Google Scholar
Stakebake, J. L., Journal of Physical Chemistry, vol. 77, pp. 581–586, 1973.Google Scholar
Stakebake, J. L. and Steward, L. M., Journal of Colloid and Interface Science, vol. 42, pp. 328–333, 1973.Google Scholar
Paffett, M. T., Kelly, D., Joyce, S. A., Morris, J., and Veirs, K., Journal of Nuclear Materials, vol. 322, pp. 45–56, 2003.CrossRefGoogle Scholar
Haschke, J. M. and Ricketts, T. E., Plutonium Dioxide Storage: Conditions for Preparation and Handling, 1995.Google Scholar
Haschke, J. M., Allen, T. H., and Stakebake, J. L., Journal of Alloys and Compounds, vol. 243, pp. 23–35, 1996.Google Scholar
Murphy, P., Boxall, C., Taylor, R., and Woodhead, D., ECS Trans., vol. 53, pp. 81–94, 14 pp., 2013.CrossRefGoogle Scholar
Nottbohm, C. T. and Hess, C., Catalysis Communications, vol. 22, pp. 39–42, 2012.Google Scholar
Patnaik, P., Handbook of Inorganic Chemicals: McGraw-Hill, 2003.Google Scholar