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NO2-mediated voloxidation for iodine separation from cesium iodide surrogates

Journal Article · · Separation Science and Technology

Heterogeneous NO2-mediated oxidation of uranium, also known as advanced voloxidation, is a proposed head-end reprocessing method for used nuclear fuel. An advantage of advanced voloxidation is the removal of volatile fission products, which complicate downstream separation and containment challenges leading to increased processing economics. Iodine, one of the volatile species of interest, has exhibited varied results in this process. Using CsI as a surrogate material, this work mimics the effect of NO2-based voloxidation on iodine and sheds light on the factors that influence the solid–gas phase reaction. Solid-state analysis using Fourier transform infrared attenuated total reflectance spectroscopy and scanning electron microscopy with energy-dispersive X-ray spectroscopy confirmed the conversion of CsI to CsNO3. Iodine separation ranged from 46% to 100% across multiple tests. Iodine separation was most effective when multiple recharges of NO2 were administered. In conclusion, at the bench scale, liberating iodine from CsI appears to occur within 1 h, but the presence of surface H2O and the composition of the NOx reagent mixtures greatly influence its success.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Nuclear Energy (NE)
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
2480049
Journal Information:
Separation Science and Technology, Journal Name: Separation Science and Technology; ISSN 0149-6395
Publisher:
Taylor & FrancisCopyright Statement
Country of Publication:
United States
Language:
English

References (41)

Voloxidation: removal of volatile fission products from spent LMFBR fuels. report January 1973
NOx Reduction in Ag/Al2O3-SiO2 Converters in the Exhaust of a Compression-Ignition Engine journal December 2020
The Thermal Decomposition of Sodium Nitrate and the Effects of Several Oxides on the Decomposition journal May 1981
The diffusion of iodine and caesium in the UO2±x lattice journal March 2000
Iodine stability as a function of pH and its implications for simultaneous multi-element ICP-MS analysis of marine carbonates for paleoenvironmental reconstructions journal September 2022
Fractional Release Behavior of Volatile and Semivolatile Fission Products During a Voloxidation and OREOX Treatment of Spent PWR Fuel journal May 2008
Measurement of Tritium during Voloxidation of Zircaloy-2 Cladding journal November 2011
NOx Storage on BaTi0.8Cu0.2O3 Perovskite Catalysts: Addressing a Feasible Mechanism journal August 2021
A Diffuse Reflectance Infrared Fourier Transform Spectroscopic Study of the Surface Reaction of NaCl with Gaseous NO2 and HNO3 journal April 1994
Oxidation kinetics for conversion of U3O8 to ε-UO3 with NO2 journal July 2017
A Combined DRIFTS and DR-UV–Vis Spectroscopic In Situ Study on the Trapping of CH 3 I by Silver-Exchanged Faujasite Zeolite journal August 2016
Theoretical Basis of Protocols for Seed Storage journal November 1990
The thermal decomposition of sodium nitrate journal January 1966
On-Line Monitoring of Gas-Phase Molecular Iodine Using Raman and Fluorescence Spectroscopy Paired with Chemometric Analysis journal January 2021
Dynamic Adsorption/Desorption of NOx on MFI Zeolites: Effects of Relative Humidity and Si/Al Ratio journal December 2022
Approaching Equilibrium in the N2O4-NO2 System: A Common Mistake in Textbooks journal December 2000
The Kinetics of the Thermal Decomposition of Sodium Nitrate and of the Reaction between Sodium Nitrite and Oxygen journal November 1956
A review of the selective reduction of NOx with hydrocarbons under lean-burn conditions with non-zeolitic oxide and platinum group metal catalysts journal December 2002
Materials and processes for the effective capture and immobilization of radioiodine: A review journal March 2016
The heterogeneous hydrolysis of NO2 in laboratory systems and in outdoor and indoor atmospheres: An integrated mechanism journal December 2002
Nitrous acid formation in the urban atmosphere: Gradient measurements of NO 2 and HONO over grass in Milan, Italy journal January 2002
Insights into iodine behaviour and speciation in the Phébus primary circuit journal November 2013
Site preference and binding of iodine and caesium in uranium dioxide journal April 1992
Reaction of NO 2 (g) with NaCl(100) journal January 1996
Simulation of Cs behavior during the high temperature voloxidation process using the HSC chemistry code journal November 2012
Infrared Spectra and Characteristic Frequencies of Inorganic Ions journal August 1952
Recent advances in the removal of radioactive iodine by bismuth-based materials journal January 2023
Revaporization Behavior of Cesium and Iodine Compounds from Their Deposits in the Steam–Boron Atmosphere journal November 2021
Thermodynamics of soluble fission products cesium and iodine in the Molten Salt Reactor journal April 2018
Elucidating the Composition and Structure of Uranium Oxide Powders Produced via NO2 Voloxidation journal February 2024
Performance of radio-iodine discharge control methods of nuclear reprocessing plants journal August 2021
Selective Trapping of Volatile Fission Products with an Off-Gas Treatment System journal July 2008
Solid sorbents for gaseous iodine capture and their conversion into stable waste forms journal May 2022
The influence of nitrogen dioxide on the oxidation of UO2 in air at temperatures below 275°C journal June 1998
A photometric study of the N2O4-NO2 equilibrium. A physical chemistry experiment journal August 1972
Fission Product Iodine and Cesium Release Behavior Under Light Water Reactor Accident Conditions journal April 1988
Ionization of N 2 O 4 in Contact with Water: Mechanism, Time Scales and Atmospheric Implications journal September 2009
Direct Dissolution of Used Nuclear Fuel in PUREX Solvent: Review and Flowsheet Development journal February 2022
Kinetics of the reaction nitrogen dioxide gas + iodide ion in molten alkali metal nitrates journal October 1968
Capture of Iodine from Nuclear-Fuel-Reprocessing Off-Gas: Influence of Aging on a Reduced Silver Mordenite Adsorbent after Exposure to NO/NO 2 journal October 2020
Radioactive Iodine Capture in Silver-Containing Mordenites through Nanoscale Silver Iodide Formation journal July 2010