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Instruments / Technical Area	Publication Details	Published	Actions
I07-Surface & interface diffraction	Structure of the electrochemical interface: Ag(hkl) in an alkaline electrolyte Angeline Kasina , Elizabeth Cocklin , Sarah Horswell , Yvonne Grunder , Christopher A. Lucas The Journal Of Physical Chemistry C 9 DOI: 10.1021/acs.jpcc.4c03154 Diamond Proposal Number(s): [9653, 12715, 22272] Open Access Show Abstract ▼ Abstract: The structure of the electrochemical double layer at the interface between Ag(hkl) electrodes and 0.1 M NaOH electrolyte has been probed using in situ surface X-ray diffraction (SXRD) measurements. The three low-index Ag(hkl) surfaces were prepared and characterized under ultra-high vacuum (UHV) conditions before being transferred into the electrochemical environment. Crystal truncation rod (CTR) measurements were made at negative potentials (just negative of the pzc), where there is no specific adsorption onto the electrode surfaces, and at more positive potentials, where hydroxide species is specifically adsorbed. The measurements quantify the relaxation at the metal electrode surfaces and, through the specular CTR, give information about layering on the electrolyte side of the interface. Strong layering effects are observed on the Ag(111) and Ag(110) surfaces, whereas on Ag(001) the layering is much weaker and we attribute this to the symmetry mismatch to the adsorbing water network. The effect of saturating the electrolyte with carbon monoxide (CO) was also examined, and structural changes were only observed on the Ag(110) surface. The changes observed suggest a stabilization of a coadsorbed CO–OH adlayer due to charge redistribution that delays the onset of CO oxidation.	Jul 2024
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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