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Instruments / Technical Area	Publication Details	Published
I07-Surface & interface diffraction	The role of crystal orientation in the dissolution of uo2 thin films S. Rennie , E. Lawrence Bright , J. E. Sutcliffe , J. E. Darnbrough , R. Burrows , J. Rawle , C. Nicklin , G. H. Lander , R. Springell Corrosion Science DOI: 10.1016/j.corsci.2018.09.012 Diamond Proposal Number(s): [13089] Show Abstract ▼ Abstract: Single crystal [0 0 1], [1 1 0], and [1 1 1]-oriented UO2 thin films were utilised to investigate the orientational dependence of radiolytic dissolution. The films were exposed to water in the presence of a synchrotron x-ray source to induce dissolution, with X-ray Reflectivity (XRR) used to observe changes in morphology as a function of exposure time. The [0 0 1] and [1 1 0]-oriented films were found to corrode at comparable rates, however, the [1 1 1] film was significantly more corrosion resistant, passivating after the initial 90 s dissolution period. This result shows the orientational dependence of UO2 dissolution, which may have important consequences for theoretical dissolution models.	Sep 2018
I12-JEEP: Joint Engineering, Environmental and Processing	An investigation on the persistence of uranium hydride during storage of simulant nuclear waste packages C. A. Stitt , N Harker , K Hallam , C Paraskevoulakos , A Banos , S Rennie , J. Jowsey , T. B. Scott Plos One 10 (7) DOI: 10.1371/journal.pone.0132284 PMID: 26176551 Diamond Proposal Number(s): [9127, 10569] Open Access Show Abstract ▼ Abstract: Synchrotron X-rays have been used to study the oxidation of uranium and uranium hydride when encapsulated in grout and stored in de-ionised water for 10 months. Periodic synchrotron X-ray tomography and X-ray powder diffraction have allowed measurement and identification of the arising corrosion products and the rates of corrosion. The oxidation rates of the uranium metal and uranium hydride were slower than empirically derived rates previously reported for each reactant in an anoxic water system, but without encapsulation in grout. This was attributed to the grout acting as a physical barrier limiting the access of oxidising species to the uranium surface. Uranium hydride was observed to persist throughout the 10 month storage period and industrial consequences of this observed persistence are discussed.	Jul 2015
I07-Surface & interface diffraction	Water corrosion of spent nuclear fuel: radiolysis driven dissolution at the UO2/water interface Ross Springell , Sophie Rennie , Leila Costelle , James Darnbrough , Milly Stitt , Elizabeth Cocklin , Christopher Lucas , Robert Burrows , Howard E. Sims , Didier Wermeille , Jonathan Rawle , Chris Nicklin , William Nuttall , Thomas Scott , Gerard Lander Faraday Discussions DOI: 10.1039/C4FD00254G Diamond Proposal Number(s): [10570] Open Access Show Abstract ▼ Abstract: X-ray diffraction has been used to probe the radiolytic corrosion of uranium dioxide. Single crystal thin films of UO2 were exposed to an intense x-ray beam at a synchrotron source in the presence of water, in order to simultaneously provide the radiation fields required to split the water into highly oxidising radiolytic products, and to probe the crystal structure and composition of the UO2 layer, and the morphology of the UO2/water interface. By modeling the electron density, the surface roughness and layer thickness, we have been able to reproduce the observed reflectivity and diffraction profiles and detect changes in oxide composition and rate of dissolution at the Ångström level, over a timescale of several minutes. A finite element calculation of the highly oxidising hydrogen peroxide product suggests that a more complex surface interaction than simple reaction with H2O2 is responsible for an enhancement in the corrosion rate directly at the interface of water and UO2, and this may impact on models of long-term storage of spent nuclear fuel.	Jan 2015

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