Abstract:The corrosion of uranium in water vapor is a key issue in nuclear industry, and it has been paid much attention for long time. Uranium can react with water vapor to form hydrogen, which has a great security threat. Meanwhile, hydrogen can react with uranium, leading to serious hydrogenation corrosion. The understanding of corrosion mechanism and kinetics of uranium in water vapor is helpful to evaluate the corrosion state of uranium more accurately and guide the safe storage of uranium fuel. Therefore, this paper analyzed the reaction characteristics between uranium and water, summarized the research methods for uranium corrosion process, and discussed the reaction processes occurring in the two different kinetic stages including the parabolic and the linear stages. Moreover, the physical and chemical characteristics of uranium corrosion products in water vapor were summarized. The formation conditions and detection methods of uranium hydride (UH3) were emphatically discussed. Several mechanism models for uranium corrosion in water vapor were summarized systematically, and the similarities and differences of models were also compared. Finally, the factors affecting the corrosion process of uranium in water vapor, such as oxygen, pretreatment process of uranium sample, and impurity content, were discussed in detail.
[1] Haschke J M.Corrosion of uranium in air and water vapor:Consequences for environmental dispersal[J].Journal of Alloys and Compounds,1998,278(1-2):149-160. [2] Haschke J M.Reactions of plutonium and uranium with water:kinetics and potential hazards[R].Los Alamos National Laboratory,LA-13069-MS,1995. [3] Santon J.A kinetic study of the reaction of water vapor and carbon dioxide on uranium[R].CEA Grennoble,CEA-R-259,1964. [4] Allen G C,Tucker P M,Lewis R A.X-ray photoelectron spectroscopy study of the initial oxidation of uranium metal in oxygen + water-vapour mixtures[J].Journal of the Chemical Society Farady Transactions,1984,80:991-1000. [5] Baker M M,Less L N,Orman S.Uranium+water reaction.Part 1.-Kinetics,products and mechanism[J].Transactions of the Faraday Society,1966,62:2513-2524. [6] Colmenares C A.Oxidation mechanisms and catalytic properties of the actinides[J].Progress in Solid State Chemistry,1984,15(4):257-364. [7] Fuller E L,Smyrl N R,Condon J B,et al.Uranium oxidation:Characterization of oxides formed by reaction with water by infrared and sorption analyses[J].Journal of Nuclear Materials,1984,120(2-3):174-194. [8] Danon A,Koresh J E,Mintz M H.Temperature programmed desorption characterization of oxidized uranium surfaces:Relation to some gas-uranium reactions[J].Langmuir,1999,15(18):5913-5920. [9] Shamir N,Tiferet E,Zalkind S,et al.Interactions of water vapor with polycrystalline uranium surfaces[J].Surface Science,2006,600(3):657-664. [10] Tiferet E,Mintz M H,Zalkind S,et al.Heat treatment effects on the surface chemisorption behavior of strained uranium:The H2O/U reaction[J].Journal of Alloys and Compounds,2007,444:177-183. [11] Tiferet E,Zalkind S,Mintz M H,et al.Interactions of water vapor with polycrystalline uranium surfaces-The low temperature regime[J].Surface Science, 2007,601(4):936-940. [12] Winer K,Colmenares C A,Smith R L,et al.Interaction of water vapor with clean and oxygen-covered uranium surfaces[J].Surface Science,1987,183(1-2):67-99. [13] Pointurier F,Marie O.Identification of the chemical forms of uranium compounds in micrometer-size particles by means of micro-Raman spectrometry and scanning electron microscope[J].Spectrochimica Acta Part B,2010,65:797-804. [14] Allen G C,Crofts J A,Griffith A J.Infrared spectroscopy of the uranium/oxygen system[J].Journal of Nuclear Materials,1976,62(2-3):273-281. [15] Manner W L,Lloyd J A,Paffett M T.Reexamination of the fundamental interactions of water with uranium[J].Journal of Nuclear Materials,1999,275(1):37-46. [16] Zalkind S,Eshkenazy R,Harush S,et al.Stress corrosion cracking of U-0.1% Cr in humid helium atmosphere[J].Journal of Nuclear Materials,1994,209(2):169-173. [17] Senanayake S D,Waterhouse G I N,Chan A S Y,et al.The reactions of water vapour on the surfaces of stoichiometric and reduced uranium dioxide:A high resolution XPS study[J].Catalysis Today,2007,120(2):151-157. [18] Senanayake S D,Idriss H.Water reactions over stoichiometric and reduced UO2(111) single crystal surfaces[J].Surface Science,2004,563(1-3):135-144. [19] Sabioni A C S,Ferraz W B,Millot F.Effect of grain-boundaries on uranium and oxygen diffusion in polycrystalline UO2[J].Journal of Nuclear Materials,2000, 278(2-3):364-369. [20] Chernia Z,BenEliyahu Y,Kimmel G,et al.The initial stage of uranium oxidation:Mechanism of UO2 scale formation in the presence of a native lateral stress field[J]. Journal of Physical Chemistry B,2006,110(46):23041-23051. [21] Stultz J,Paffett M T,Joyce S A.Thermal evolution of hydrogen following water adsorption on defective UO2(100)[J].Journal of Physical Chemistry B, 2004,108(7):2362-2364. [22] Mintz M H,Shamir N.The use of direct recoil spectrometry (DRS) for the study of water vapor interactions on polycrystalline metallic surfaces-the H2O/U and H2O/Ti systems[J].Applied Surface Science,2005,252(3):633-640. [23] Ritchie A G.A review of the rates of reaction of uranium with oxygen and water vapour at temperatures up to 300 ℃[J].Journal of Nuclear Materials,1981,102(1-2):170-182. [24] Ritchie A G.The kinetics and mechanism of the uranium-water vapour reaction-an evaluation of some published work[J].Journal of Nuclear Materials,1984,120:143-153. [25] Allen G C,Tucker P M,Tyler J W.Oxidation of uranium dioxide at 298 K studied by using X-ray photoelectron spectroscopy[J].Journal of Physical Chemistry,1982,86(2):224-228. [26] Schroeder J B,Vaughan D A,Schwartz C M.Aqueous uranium corrosion at 100 ℃[J].Journal of the Electrochemical Society,1959,106(6):486-489. [27] Mcgillivray G W,Geeson D A,Greenwood R C.Studies of the kinetics and mechanism of the oxidation of uranium by dry and moist air:A model for determining the oxidation rate over a wide range of temperatures and water vapour pressures[J].Journal of Nuclear Materials,1994,208(1-2):81-97. [28] Harker R M.The influence of oxide thickness on the early stages of the massive uranium-hydrogen reaction[J].Journal of Alloys and Compounds,2006,426(1-2): 106-117. [29] Colmenares C,Howell R,Mccreary T.Oxidation of uranium studied by gravimetric and positron annihilation techniques[R].Lawrence Livermore National Laboratory,UCRL-85549,1981. [30] Sinkov S I,Delegard C H,Schmidt A J.Preparation and characterization of uranium oxides in support of the K basin sludge treatment project[R].Pacific Northwest National Laboratory,PNNL-17678,2008. [31] Kondo T,Verink E D,Fontana M G,et al.Gas chromatographic and gravimetric studies of uranium oxidation mechanism[J].Corroison,1964,20(10):t314-t320. [32] Kondo T,Beck F H,Fontana M G.A gas chromatographic study on the kinetics of uranium oxidation in moist environments[J].Corrosion,1974,30(9):330-341. [33] Banos A,Hallam K R,Scott T B.Corrosion of uranium in liquid water under vacuum contained conditions.Part 1:The initial binary U+H2O(1) system[J].Corrosion Science,2019,152:249-260. [34] Greenholt C J,Weirick L J.The oxidation of uranium-0.75 wt% titanium in environments containing oxygen and/or water vapor at 140 ℃[J].Journal of Nuclear Materials,1987,144(1-2):110-120. [35] Wood D H,Snowden S A,Howe H J,et al.Regarding the chemistry of metallic uranium stored in steel drums[J].Journal of Nuclear Materials,1994,209(1):113-115. [36] Banos A,Hallam K R,Scott T B.Corrosion of uranium in liquid water under contained conditions with a headspace deuterium overpressure.Part 2:The ternary U+H2O(1)+D2 system[J].Corrosion Science,2019,152:261-270. [37] Taylor P,Wood D D,Owen D G.Microstructures of corrosion films on UO2 fuel oxidized in air-steam mixtures at 225 ℃[J].Journal of Nuclear Materials,1995, 223(3):316-320. [38] Abrefah J,Sell R L.Oxidation of K-West basin spent nuclear fuel in moist helium atmosphere[R].Pacific Northwest National Lab,PNNL-12167,1999. [39] Martin T L,Coe C,Bagot P a J,et al.Atomic-scale studies of uranium oxidation and corrosion by water vapour[J].Scientific Reports,2016,6(1):25618. [40] Banos A,Scott T B.Statistical analysis of UH3 initiation using electron back-scattered diffraction (EBSD)[J].Solid State Ionics,2016,296:137-145. [41] Banos A,Stitt C A,Scott T B.The effect of sample preparation on uranium hydriding[J].Corrosion Science,2016,113:91-103. [42] Morrall P,Price D W,Nelson A J,et al.ToF-SIMS characterization of uranium hydride[J].Philosophical Magazine Letters,2007,87(8):541-547. [43] Draley J E,Ruther W E.Some unusual effects of hydrogen in corrosion reactions[J].Journal of the Electrochemical Society,1957,104(6):329-333. [44] Hopkinson B E.Kinetics of the uranium-steam reaction[J].Journal of the Electrochemical Society,1959,106(2):102-106. [45] Delegard C H,Schmidt A J.Uranium metal reaction behavior in water, sludge,and grout matrices[R].Pacific Northwest National Laboratory,PNNL-17815,2008. [46] Bennett M J,Myatt B L,Silvester D R V,et al.The oxidation behaviour of uranium in air at 50-300 ℃[J].Journal of Nuclear Materials,1975,57(2):221-236. [47] Colby L J.Kinetics of the reaction of uranium monocarbide with water[J].Journal of the Less Common Metals,1966,10(6):425-431. [48] Banos A,Scott T B.A review of the reaction rates of uranium corrosion in water[J].Journal of Hazardous Materials,2020,399:122763. [49] Ritchie A G,Greenwood R C,Randles S J,et al.Measurements of the rate of the uranium-water vapour reaction[J].Journal of Nuclear Materials,1986,140(3):197-201. [50] Baker M M,Less L N,Orman S.Uranium + water reaction. Part 2.-Effect of oxygen and other gases[J].Transactions of the Faraday Society,1966,62:2525-2530. [51] Ritchie A G,Greenwood R C,Randles S J.The kinetics of the uranium oxygen water-vapor reaction between 40 ℃ and 100 ℃[J].Journal of Nuclear Materials,1986,139(2):121-136. [52] Allen G C,Crofts J A,Curtis M T,et al.Xray photoelectron spectroscopy of some uranium oxide phases[J].Journal of the Chemical Society,Dalton Transactions,1974(12):1296-1301. [53] Raveh A,Arkush R,Zalkind S,et al.Passivation of uranium metal by radio-frequency plasma nitriding against gas phase (H2,H2O) corrosion[J].Surface & Coatings Technology,1996,82(1-2):38-41. [54] Corcoran V J,Johnston C,Metcalfe W,et al.The water vapour corrosion of uranium and its prevention[R].Atomic Weapons Research Establishment,AWRE-O-42/65,1965. [55] Manner W L,Lloyd J A,Hanrahan R J,et al.An examination of the initial oxidation of a uranium-base alloy (U-14.1 at.% Nb) by O2 and D2O using surface-sensitive techniques[J].Applied Surface Science,1999,150(1-4):73-88. [56] Larson D T.Oxidation of a ternary uranium alloy[J].Jouranl of Vacuum Science & Technology,1971,8(1):80-83. [57] Bennett M J,Price J B.The oxidation behaviour of uranium in air at 348-765 K[J]. Journal of Nuclear Materials,1981,101(1-2):44-55. [58] Pearce R J,Bennett M J,Price J B.Oxidation of irradiated uranium in moist air[J]. Nucl.Energy,1988,27(5):305-309.