Reaction mechanisms of La3+ and Zr4+ in LiCl-KCl eutectic molten salt - cyclic and square wave voltammetry data simulations

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dc.contributor.authorFabian, CPen_AU
dc.contributor.authorChamelot, Pen_AU
dc.contributor.authorMassot, Len_AU
dc.contributor.authorCaravaca, Cen_AU
dc.contributor.authorLuca, Ven_AU
dc.contributor.authorLumpkin, GRen_AU
dc.date.accessioned2023-01-13T00:50:21Zen_AU
dc.date.available2023-01-13T00:50:21Zen_AU
dc.date.issued2011-05-01en_AU
dc.date.statistics2022-10-17en_AU
dc.description.abstractNuclear energy increasingly represents an important option for generating clean CO2-free electricity. This has generated a nuclear renaissance with increased interest in both innovative nuclear reactors and fuel cycle technologies. The innovative reactor concepts proposed have mainly involved closed fuel cycles with implied recycling of irradiated fuel. Pyroelectrochemical processes based on a molten alkali chloride/fluoride electrolyte system show considerable promise, and as such have received considerable attention for fuel reprocessing. Lanthanum and zirconium are two fission products that are expected to be present in irradiated fuels. The present investigation addresses the electrochemical reduction of La3+ and Zr4+ in LiCl - KCl eutectic molten salt using transient techniques such as cyclic voltammetry (CV), square wave voltammetry (SWV) and chronopotentiometry (CP) from 425 to 550° C, at two concentration levels. Experimental CV data from 50 to 500 mV/sec appears to indicate that the lanthanum reaction mechanism involve a single step reduction process, i.e., La3+ + 3e- ↔ La. Hence a theoretical simulation of this experimental data should be straightforward as verification of the reaction mechanism. However, zirconium experimental CV data also from 50 to 500 mV/sec appears to indicate that its reduction proceeds through an ab initio sluggish charge-transfer step coupled with an adsorption/underpotential deposition: Zr4+ + 2e- ↔ Zr2+ followed by a second and faster step where two electrons further are transferred: Zr2+ + 2e- ↔ Zr. A theoretical simulation of the experimental voltammograms has been also conducted to verify this reaction mechanism. We show the parameter Λ in their potential separation, ∆Epp and scan rate plot to indicate the reversibility of their electrochemical process, and evaluate their standard electrochemical rate constant. Deconvolution of the SWV data for lanthanum and zirconium confirms that the reduction of La3+ proceeds through three-electron one-step reaction mechanism while that of Zr4+ proceeds through two two-electron step reactions independent of temperature and concentrations levels. © 2011 The Electrochemical Societyen_AU
dc.identifier.booktitleECS Meeting Abstractsen_AU
dc.identifier.citationFabian, C. P., Chamelot, P., Massot, L., Caravaca, C., Luca, V., & Lumpkin, G. (2011). Reaction mechanisms of La3+ and Zr4+ in LiCl-KCl eutectic molten salt - cyclic and square wave voltammetry data simulations. Paper presented at the 219th ECS Meeting, Montreal, Quebec, Canada, May 1-6, 2011. In ECS Meeting Abstracts, MA2011-01(41),1910. doi:10.1149/MA2011-01/41/1910en_AU
dc.identifier.conferenceenddate6 May 2011en_AU
dc.identifier.conferencename219th ECS Meetingen_AU
dc.identifier.conferenceplaceQuebec, Canadaen_AU
dc.identifier.conferencestartdate1 May 2011en_AU
dc.identifier.issue41en_AU
dc.identifier.otherAbstract no. 1910en_AU
dc.identifier.pagination1910en_AU
dc.identifier.urihttps://doi.org/10.1149/MA2011-01/41/1910en_AU
dc.identifier.urihttps://apo.ansto.gov.au/dspace/handle/10238/14333en_AU
dc.identifier.volumeMA2011-01en_AU
dc.language.isoenen_AU
dc.publisherIOP Publishingen_AU
dc.subjectSimulationen_AU
dc.subjectElectrochemistryen_AU
dc.subjectFuel cycleen_AU
dc.subjectIrradiationen_AU
dc.subjectZirconiumen_AU
dc.subjectLanthanumen_AU
dc.titleReaction mechanisms of La3+ and Zr4+ in LiCl-KCl eutectic molten salt - cyclic and square wave voltammetry data simulationsen_AU
dc.typeConference Abstracten_AU
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