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Water corrosion of spent nuclear fuel: radiolysis driven dissolution at the UO2/water interface

DOI: 10.1039/C4FD00254G DOI Help

Authors: Ross Springell (University of Bristol) , Sophie Rennie (University of Bristol) , Leila Costelle (University of Bristol) , James Darnbrough (University of Bristol) , Milly Stitt (University of Bristol) , Elizabeth Cocklin (University of Liverpool) , Christopher Lucas (University of Liverpool) , Robert Burrows (National Nuclear Laboratory) , Howard E. Sims (National Nuclear Laboratory) , Didier Wermeille (European Synchrotron Radiation Facility) , Jonathan Rawle (Diamond Light Source) , Chris Nicklin (Diamond Light Source) , William Nuttall (The Open University) , Thomas Scott (Interface Analysis Centre, University of Bristol) , Gerard Lander (European Commission, Joint Research Centre, Institute for Transuranium Elements)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Faraday Discussions

State: Published (Approved)
Published: January 2015
Diamond Proposal Number(s): 10570

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.

Subject Areas: Materials, Physics, Energy

Instruments: I07-Surface & interface diffraction

Other Facilities: ESRF

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