Transpiration studies on the volatilities of PuO3(g) and PuO2(OH)2(g) from PuO2(s) in the presence of steam and oxygen and application to plutonium volatility in mixed-waste thermal oxidation processors

Krikorian, O.H.; Fontes, A.S.; Ebbinghaus, B B; Adamson, M.G.

doi:10.1016/s0022-3115(97)00043-3

Cited by 12 publications

(21 citation statements)

References 1 publication

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“…The vaporization yields reported by Domanov are in clear contradiction to our experimental results and also to the vapor pressure data measured by Krikorian [7] and Ronchi [10].…”

Section: Discussioncontrasting

confidence: 99%

“…The results of the thermochromatographic studies presented here are in agreement with the data reported by Krikorian [7], Haschke [8], and Ronchi [10].…”

Section: Discussionsupporting

confidence: 92%

“…Krikorian et al. studied the volatility of PuO 2(s) in the presence of humid oxygen and explained the plutonium volatility data by the formation of PuO 3(g) and PuO 2 (OH) 2(g) [7]. They measured total vapor pressures of Pu species over PuO 2 to a superstoichiometric solid solution denoted as PuO 2+x (x ≤ 0.27) [8].…”

Section: Introductionmentioning

confidence: 99%

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Thermochromatographic studies of plutonium oxides

Hübener¹,

Taut²,

Vahle³

et al. 2008

Radiochimica Acta

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Plutonium oxides / Thermochromatography / Oxidation / VolatilitySummary. Trace amounts of oxidic plutonium species were studied by thermochromatography in silica glass columns in comparison to oxidic species of Th, Pa, U, Np, and Am. Humid oxygen was used as reactive admixture to the carrier gas helium. The thermochromatographic behavior of plutonium provides evidence for the oxidation of Pu(IV) to Pu(VI) with humid oxygen. The gas chromatographic transport of U, Np, and Pu is governed by the surface reactionwith M = U, Np, and Pu in the hexavalent state and competitive reactions of the actinide oxides with silica to nonvolatile compounds or solid solutions. There is good agreement with earlier volatility studies and the reported oxidation of PuO 2 with water. The oxidation to PuO 4 as claimed by Domanov [1] could not be confirmed.

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“…The vaporization yields reported by Domanov are in clear contradiction to our experimental results and also to the vapor pressure data measured by Krikorian [7] and Ronchi [10].…”

Section: Discussioncontrasting

confidence: 99%

“…The results of the thermochromatographic studies presented here are in agreement with the data reported by Krikorian [7], Haschke [8], and Ronchi [10].…”

Section: Discussionsupporting

confidence: 92%

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Thermochromatographic studies of plutonium oxides

Hübener¹,

Taut²,

Vahle³

et al. 2008

Radiochimica Acta

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“…This vaporized plutonium would be expected to essentially completely condense as the gas cooled to 2000EF, possibly even within the melter. A similar conclusion was derived by Krikorian et al from their experimental work on the volatilization of plutonium oxides in the presence of steam and oxygen (12). Figure 14 shows the relative split in plutonium between the condensed and vapor phases in the flame at 2800EF as functions of the plutonium in the waste material and the flame stoichiometry.…”

Section: Volatilization Of Plutonium Componentssupporting

confidence: 82%

Thermodynamic modeling of volatile hazardous metal behavior in the Vortec Vitrification System

Nowok¹,

Hurley²

2000

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“…Their partial pressure is more than 1000 times lower than that of gallium oxide [9], and their formation does not affect the removal of gallium.…”

mentioning

confidence: 96%

Gallium removal during pyrochemical reprocessing of weapons plutonium into oxide fuel

2009

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It is well known that plutonium is a long-lived and renewable source of energy. In France, power plutonium obtained mainly after regeneration of irradiated oxide fuel is used as a mixed fuel. However, the use of such fuel in thermal reactors is too inefficient [1]. Ultimately, fast reactors which will make it possible to use plutonium cost-effectively and in an ecologically well-substantiated manner as well as weapons and tailings uranium in the form of mixed fuel will play the dominant role in nuclear power.Weapons plutonium is a plutonium-gallium alloy [2][3][4][5]. The addition of several percent gallium to plutonium is necessary to stabilize the δ modification of plutonium and to impart the required mechanical properties to weapons plutonium. The utilization of weapons plutonium in nuclear fuel and, specifically, its conversion into oxide fuel is a topical problem [6]. The reprocessing of weapons plutonium into a disperse PuO 2 powder by a water-chemical method involves a large number of operations and a large amount of wastes. A more efficient method of reprocessing weapons plutonium is the pyrochemical process, which contains an intermediate operation where weapons plutonium is hydrided by hydrogen and the plutonium hydride is oxidized by the oxygen present in the mixture together with inert gases and nitrogen. The gallium present in weapons plutonium is oxidized to Ga 2 O 3 .The effect of gallium oxide impurities on the fuel-element cladding materials (radiation-and corrosion-resistant steel and zirconium alloys) when mixed uranium-plutonium fuel is used has not been adequately studied. Consequently, it is recommended that its content in mixed fuel not exceed 0.001 mass% to prevent cladding corrosion inside fuel elements [4]. In this connection it useful to evaluate the possibility of removing gallium during pyrochemical treatment of PuO 2 -Ga 2 O 3 powder and sintering of mixed uranium-plutonium oxide fuel kernels in a hydrogen atmosphere.Thermodynamic Analysis of Hydrogen Reduction of Gallium Oxides. A thermodynamic analysis of the reduction of gallium oxide was performed to evaluate the possible removal of gallium from plutonium oxide by heat-treatment in a hydrogen atmosphere. Figure 1 shows two variants of the pyrochemical reprocessing of weapons plutonium into plutonium dioxide powders. One variant consists in hydriding weapons plutonium by hydrogen (at comparatively low temperature to 500 K) and oxidizing the products so formed in a mixture with inert gases to PuO 2 and Ga 2 O 3 . In the other variant, nitriding plutonium by nitrogen, which yields plutonium nitride, followed by oxidation can be added to increase safety. Thermodynamic modeling was performed using the IVTANTERMO (Russia) program system [7]. The data published in the handbook [8] were used for the thermodynamic calculations.

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Transpiration studies on the volatilities of PuO3(g) and PuO2(OH)2(g) from PuO2(s) in the presence of steam and oxygen and application to plutonium volatility in mixed-waste thermal oxidation processors

Cited by 12 publications

References 1 publication

Thermochromatographic studies of plutonium oxides

Thermochromatographic studies of plutonium oxides

Thermodynamic modeling of volatile hazardous metal behavior in the Vortec Vitrification System

Gallium removal during pyrochemical reprocessing of weapons plutonium into oxide fuel

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