Influence of fission products on ruthenium oxidation and transport in air ingress nuclear accidents

Abstract In separate effect tests at 1000–1200 °C Ru oxidation rate and content of Ru in escaping air flow have been studied with special emphasis on effects of other fission product elements on the Ru oxidation and transport. The results showed that in the decreasing temperature section (1100–600 °C) most of the RuO 3 and RuO 4 (≈95%) decomposed and formed RuO 2 crystals; while the partial pressure of RuO 4 in the escaping air was in the range of 10 −6 bar. The re-evaporation of deposited RuO 2 resulted in about 10 −6 bar partial pressure in the outlet gas as well. Measurements demonstrated the importance of surface quality in the decreasing temperature area on the heterogeneous phase decomposition of ruthenium oxides to RuO 2 . On the other hand water or molybdenum oxide vapour in air appears to decrease the surface catalyzed decomposition of RuO x to RuO 2 and increases RuO 4 concentration in the escaping air. High temperature reaction with caesium changed the form of the released ruthenium and caused a time delay in appearance of maximum concentration of ruthenium oxides in the ambient temperature escaping gas, while reaction with barium and rare earth oxides extended Ru escape from the high temperature area.

[1]  T. Kärkelä,et al.  Progress on ruthenium release and transport under air ingress conditions , 2008 .

[2]  M. Inghram,et al.  POLYMERIC GASEOUS SPECIES IN THE SUBLIMATION OF MOLYBDENUM TRIOXIDE. Period covered: To June 30, 1956. Technical Report No. 2 on THERMODYNAMICS OF REFRACTORY MATERIALS AS DETERMINED WITH A MASS SPECTROMETER , 1956 .

[3]  C. Madic,et al.  Review of Literature on Ruthenium Behavior in Nuclear Power Plant Severe Accidents , 2006 .

[4]  J. Ehrhardt,et al.  XPS investigations of ruthenium deposited onto representative inner surfaces of nuclear reactor containment buildings , 2007 .

[5]  Unto Tapper,et al.  On the transport and speciation of ruthenium in high temperature oxidising conditions , 2005 .

[6]  W. Bell,et al.  HIGH-TEMPERATURE CHEMISTRY OF THE RUTHENIUM—OXYGEN SYSTEM1 , 1963 .

[7]  L. Cantrel,et al.  Radiolytic Oxidation of Ruthenium Oxide Deposits , 2008 .

[8]  W. Kim,et al.  Determination of Ru, Rh, Pd, Te, Mo and Zr in spent pressurized water reactor fuels by ion exchange and extraction chromatographic separations and inductively coupled plasma atomic emission spectrometric analysis , 2003 .

[9]  Laurent Cantrel,et al.  Study of RuO4 decomposition in dry and moist air , 2007 .

[10]  Oxidation of ruthenium oxide deposits by ozone , 2008 .

[11]  H. Kleykamp,et al.  The Chemical State of Fission Products in Oxide Fuels at Different Stages of the Nuclear Fuel Cycle , 1988 .

[12]  J. Cara,et al.  Oxidation-enhanced Emission of Ruthenium From Nuclear-fuel , 1995 .

[13]  E. Westrum,et al.  RECENT THERMOCHEMICAL RESEARCH ON REACTOR MATERIALS AND FISSION PRODUCTS , 1989 .

[14]  Y. Pontillon,et al.  Ruthenium release at high temperature from irradiated PWR fuels in various oxidising conditions; main findings from the VERCORS program , 2005 .

[15]  J. Bart,et al.  The Binary Oxide System TeO2 ? MoO3 , 1975 .

[16]  B. Bowsher Fission-product chemistry and aerosol behaviour in the primary circuit of a pressurized water reactor under severe accident conditions , 1987 .

[17]  H. Schäfer,et al.  Zur Chemie der Platinmetalle. V Gleichgewichte mit Ru(f)5 RuO2(f)5 RuO3(g) und RuO4(g) , 1963 .

[18]  R. P. Larsen,et al.  SPECTROPHOTOMETRIC DETERMINATION OF RUTHENIUM , 1959 .

[19]  R. Konings,et al.  Vapour pressures of some caesium compounds. II. Cs2MoO4 and Cs2RuO4 , 1992 .

[20]  R. Sharpe,et al.  Metallic fission-product inclusions in irradiated oxide fuels , 1968 .