Laventine, Dominic Michael and Wilbraham, Richard James and Boxall, Colin and Taylor, Robin J and Orr, R. (2017) Direct mass analysis of water absorption onto ceria thin films. MRS Advances, 2 (12). pp. 649-654. ISSN 2059-8521
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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.