Airborne Release Fraction of Dissolved Materials During the Combustion of Liquids Representative of Nuclear Waste Treatment Process

Abstract Experimental results are reported on the airborne release, under fire conditions, of hazardous materials dissolved in a mixture of organic solvents [tributylphosphate (TBP) and hydrogenated tetrapropylene (HTP)] representative of the nuclear fuel recycling process. Cerium and ruthenium have been considered, respectively, as stable and volatile fission products that eventually could be released as airborne particles during thermal degradation of contaminated and inflammable liquids. Airborne release fractions (ARFs) and their experimental uncertainties have been determined. Considering fire involving contaminated organic solvents, higher ARFs are reported for ruthenium Ru(+III) (0.99 ± 1.20%) in comparison with cerium [0.22 ± 0.31% and 0.20 ± 0.28% for Ce(+III) and Ce(+IV), respectively]. This discrepancy is partially due to the volatility of ruthenium formed under these conditions. Considering configurations involving an aqueous nitric acid phase placed below contaminated solvents, boiling of this phase enhances the release of contaminant materials: 1.78 ± 1.06% and 1.01 ± 1.31% for Ce(+III) and Ce(+IV), respectively, and 12.41 ± 29.45% for Ru(+III). Analysis of the size distribution, morphology, and chemical composition of the released particles and droplets emitted during HTP/TBP bubble collapse are reported, highlighting the contribution of bubble bursting at the solvent surface to airborne release.

[1]  Alexander L. Brown,et al.  Airborne Release Fractions from Surrogate Nuclear Waste Fires Containing Lanthanide Nitrates and Depleted Uranium Nitrate in 30% Tributyl Phosphate in Kerosene , 2020, Nuclear Technology.

[2]  T. Gélain,et al.  Airborne release of hazardous micron-sized metallic/metal oxide particles during thermal degradation of polycarbonate surfaces contaminated by particles: Towards a phenomenological description. , 2019, Journal of hazardous materials.

[3]  T. Loiseau,et al.  Influence of Light and Temperature on the Extractability of Cerium(IV) as a Surrogate of Plutonium(IV) and its Effect on the Simulation of an Accidental Fire in the PUREX Process , 2019, ACS omega.

[4]  Eugenia Valsami-Jones,et al.  Impact of particle size, oxidation state and capping agent of different cerium dioxide nanoparticles on the phosphate-induced transformations at different pH and concentration , 2019, PloS one.

[5]  Ying Zhen Li,et al.  Scale effect of mass loss rates for pool fires in an open environment and in tunnels with wind , 2019, Fire Safety Journal.

[6]  Ross J Ellis,et al.  Third phase inversion, red oil formation, and multinuclear speciation of tetravalent cerium in the tri-n-butyl phosphate–n-dodecane solvent extraction system , 2018 .

[7]  Thidarat Wongsawa,et al.  The experimental investigations on viscosity, surface tension, interfacial tension and solubility of the binary and ternary systems for tributyl phosphate (TBP) extractant in various organic solvents with water: Thermodynamic NRTL model and molecular interaction approach , 2018 .

[8]  Sheng-Hsiu Huang,et al.  Characterization of aerosol emissions from single bubble bursting , 2017 .

[9]  M. Miguirditchian,et al.  Experimental and modelling study of ruthenium extraction with tri-n-butylphosphate in the purex process , 2017 .

[10]  Alexander L. Brown,et al.  Multicomponent Evaporation Effects on Particulate Release in a Liquid Fuel Fire , 2017 .

[11]  J. Reid,et al.  Effect of crystallization kinetics on the properties of spray dried microparticles , 2016 .

[12]  P. Lemaître,et al.  Measurement and modeling of pressure drop of HEPA filters clogged with ultrafine particles , 2016 .

[13]  Alexander L. Brown,et al.  Contaminant Entrainment in a Liquid Fuel Fire , 2016 .

[14]  T. Dumas,et al.  Speciation of Ruthenium in Organic TBP/TPH Organic Phases: A Study about Acidity of Nitric Solutions☆ , 2016 .

[15]  Alexander L. Brown,et al.  Contaminant Entrainment from a Gasoline Pool Fire. , 2015 .

[16]  S. Musić,et al.  Formation of RuO2 nanoparticles by thermal decomposition of Ru(NO)(NO3)3 , 2015 .

[17]  S. Pontreau,et al.  Physicochemical properties of aerosol released in the case of a fire involving materials used in the nuclear industry. , 2015, Journal of hazardous materials.

[18]  L. Cantrel,et al.  Theoretical study of plutonium(IV) complexes formed within the PUREX process: a proposal of a plutonium surrogate in fire conditions. , 2014, The journal of physical chemistry. A.

[19]  A. Coppalle,et al.  Increase in thermophoretic velocity of carbon aggregates as a function of particle size , 2014 .

[20]  S. Matsumoto,et al.  Clogging of HEPA Filters by Soot during Fire Events in Nuclear Fuel Cycle Facilities , 2014 .

[21]  Ofodike A. Ezekoye,et al.  Soot Deposition and Gravitational Settling Modeling and the Impact of Particle Size and Agglomeration , 2014 .

[22]  A. Coppalle,et al.  Contribution to the study of particle resuspension kinetics during thermal degradation of polymers. , 2013, Journal of hazardous materials.

[23]  F. Menegalli,et al.  Image analysis: Statistical study of particle size distribution and shape characterization , 2011 .

[24]  E. Villermaux,et al.  Bursting bubble aerosols , 2011, Journal of Fluid Mechanics.

[25]  V. M. Mocho,et al.  Clogging of industrial pleated high efficiency particulate air (HEPA) filters in the event of fire , 2011 .

[26]  Gregg J. Lumetta,et al.  Advanced separation techniques for nuclear fuel reprocessing and radioactive waste treatment , 2011 .

[27]  P. M. Schumacher,et al.  Plutonium Release Fractions from Accidental Fires , 2008 .

[28]  N. Hyatt,et al.  The use of surrogates in waste immobilization studies : a case study of plutonium , 2008 .

[29]  L. Russell,et al.  Submicron Salt Particle Production in Bubble Bursting , 2006 .

[30]  G. Adachi,et al.  Characterization and thermal behavior of amorphous rare earth phosphates , 2004 .

[31]  Per Blomqvist,et al.  Particles from fires—a screening of common materials found in buildings , 2003 .

[32]  Axel Günther,et al.  Transport of salts and micron-sized particles entrained from a boiling water pool , 2003 .

[33]  Bijan Najafi,et al.  History of Fire Events in the U.S. Commercial Nuclear Industry , 2002 .

[34]  W. L. Cowley,et al.  Estimating Risk Using Bounding Calculations and Limited Data , 2002 .

[35]  Jin Wu Production Functions of Film Drops by Bursting Bubbles , 2001 .

[36]  Klaus Willeke,et al.  Aerosol Measurement: Principles, Techniques, and Applications , 2001 .

[37]  Kevin B. McGrattan,et al.  In Situ Burning of Oil Spills , 2001, Journal of research of the National Institute of Standards and Technology.

[38]  J. Starflinger,et al.  Radionuclide re-entrainment at bubbling water pool surfaces , 2000 .

[39]  J. Quintiere A Review of Experiments on the Airborne Release of Simulated Radioactive Compounds from Fire , 1998 .

[40]  D. E. Spiel On the births of film drops from bubbles bursting on seawater , 1998 .

[41]  Laurent Bouilloux Étude de la mise en suspension physico-chimique des oxydes de plutonium et d'uranium lors de la combustion de polycarbonate, et de ruthénium lors de la combustion des solvants de retraitement du combustible irradié , 1998 .

[42]  Y. Fernandez,et al.  Radioactive Aerosols Emission in Fires , 1995 .

[43]  F. Resch,et al.  Film drop distributions from bubbles bursting in seawater , 1991 .

[44]  G. Nishio,et al.  Release of radioactive materials in simulation tests of a postulated solvent fire in a nuclear fuel reprocessing plant , 1989 .

[45]  D. Blanchard The ejection of drops from the sea and their enrichment with bacteria and other materials: A review , 1989 .

[46]  P. C. Owczarski,et al.  Aerosols Released in Accidents in Reprocessing Plants , 1988 .

[47]  D. Blanchard,et al.  Film drop production as a function of bubble size , 1988 .

[48]  Halverson,et al.  Combustion Aerosols Formed During Burning of. Radioactively Contaminated Materials - .Experimental Results , 1987 .

[49]  H. Bunz,et al.  Resuspension of fission products during severe accidents in light-water reactors , 1986 .

[50]  P. C. Owczarski,et al.  Radioactive Source Term Models in a Compartment Fire Code , 1985 .

[51]  H. Seehars Release of pu-containing materials during a kerosene fire , 1983 .

[52]  S. Trasatti,et al.  Interfacial properties of oxides used as anodes in the electrochemical technology , 1983 .

[53]  P. Duvigneaud,et al.  DTA study of RuO2 formation from the thermal decomposition of ruthenium(III) hydrate , 1981 .

[54]  C. Bruneau,et al.  Thermal degradation of tri-n-butyl phosphate , 1981 .

[55]  D. J. Pruett,et al.  The Solvent Extraction Behavior of Ruthenium I - The Nitric Acid-Tri-n-Butyl Phosphate System , 1980 .

[56]  S. L. Sutter,et al.  Fractional airborne release of strontium during the combustion of 30 percent normal tributyl phosphate in a kerosine-type diluent , 1974 .

[57]  L. Schwendiman,et al.  Some experimental measurements of airborne uranium (representing plutonium) in transportation accidents , 1973 .

[58]  L. Schwendiman,et al.  Interim report: the fractional airborne release of dissolved radioactive materials during the combustion of 30 percent normal tributyl phosphate in a kerosene-type diluent , 1973 .

[59]  J. M. Fletcher,et al.  NITRATO NITROSYLRUTHENIUM COMPLEXES AND THEIR EXTRACTION FROM NITRIC ACID SYSTEMS BY TRIBUTYL PHOSPHATE. PART I. LABORATORY STUDIES , 1957 .