Volatile molecule PuO3 observed from subliming plutonium dioxide

Ronchi, C.; Capone, F.; Colle, Jean‐Yves; Hiernaut, J.-P.

doi:10.1016/s0022-3115(00)00058-1

Cited by 33 publications

(40 citation statements)

References 6 publications

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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%

“…The report by Haschke et al stimulated numerous studies dealing with the oxide chemistry of plutonium, e.g. mass spectrometric measurements by Ronchi et al [10], investigation of plutonium oxide cluster ions by Gibson and Haire [11], thermochromatography experiments by Domanov et al [1,12], and, only recently, redox reaction studies of Pu(IV) hydrous oxide by Neck et al [13]. In the mass spectrometric measurements carried out by Ronchi et al [10] above 1800 K PuO 3 became measurable.…”

Section: Introductionmentioning

confidence: 99%

“…mass spectrometric measurements by Ronchi et al [10], investigation of plutonium oxide cluster ions by Gibson and Haire [11], thermochromatography experiments by Domanov et al [1,12], and, only recently, redox reaction studies of Pu(IV) hydrous oxide by Neck et al [13]. In the mass spectrometric measurements carried out by Ronchi et al [10] above 1800 K PuO 3 became measurable. Already in 1997, long before the publication by Haschke et al, Domanov et al [1,12] studied trace amounts of 238 Pu and 239 Pu which were deposited on silica powder and heated up to 650…”

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%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Thermochromatographic studies of plutonium oxides

Hübener¹,

Taut²,

Vahle³

et al. 2008

Radiochimica Acta

View full text Add to dashboard Cite

show abstract

“…It is known, for instance, that in the presence of steam and oxygen, plutonium is released primarily as PuO 3 (g) and PuO 2 (OH) 2 (g), and less probably as PuO 2 (g) [5], meaning that these could be a potentially important source of radioactive aerosols and transported over long distances.…”

Section: Introductionmentioning

confidence: 99%

On the multi-reference nature of plutonium oxides: PuO₂²⁺, PuO₂, PuO₃ and PuO₂(OH)₂

Boguslawski

Réal

Tecmer

et al. 2017

Phys. Chem. Chem. Phys.

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Actinide-containing complexes present formidable challenges for electronic structure methods due to the large number of degenerate or quasi-degenerate electronic states arising from partially occupied 5f and 6d shells. Conventional multi-reference methods can treat active spaces that are often at the upper limit of what is required for a proper treatment of species with complex electronic structures, leaving no room for verifying their suitability. In this work we address the issue of properly defining the active spaces in such calculations, and introduce a protocol to determine optimal active spaces based on the use of the Density Matrix Renormalization Group algorithm and concepts of quantum information theory. We apply the protocol to elucidate the electronic structure and bonding mechanism of volatile plutonium oxides (PuO 3 and PuO 2 (OH) 2 ), species associated with nuclear safety issues for which little is known about the electronic structure and energetics. We show how, within a scalar relativistic framework, orbital-pair correlations can be used to guide the definition of optimal active spaces which provide an accurate description of static/non-dynamic electron correlation, as well as to analyse the chemical bonding beyond a simple orbital model. From this bonding analysis we are able to show that the addition of oxo-or hydroxo-groups to the plutonium dioxide species considerably changes the pi-bonding mechanism with respect to the bare triatomics, resulting in bent structures with considerable multi-reference character.

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Plutonium and Plutonium Compounds

Clark

Hecker

Jarvinen

et al. 2006

Kirk-Othmer Encyclopedia of Chemical Technology

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The discovery of plutonium, its economic and military importance, sources, production, and nuclear properties are reviewed. The economic aspects of weapons‐ and reactor‐grade plutonium are outlined. The preparation and properties of plutonium metal and its alloys are discussed in detail. A presentation of the physical and chemical properties of atomic plutonium and stable plutonium ions is given. The complexation and hydrolysis properties of these ions are recapitulated. Analytical chemistry, separations technology, and metallurgy (including pyrometallurgical processing) are described. There is a brief treatment of storage and disposal of excess weapons plutonium. The chemistry of several classes of plutonium compounds is described: oxides, halides, oxyhalides, hydrides, carbides, silicides, nitrides, sulfides, and oxalates. The article concludes with a treatment of environmental, health, and safety aspects of plutonium.

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Volatile molecule PuO3 observed from subliming plutonium dioxide

Cited by 33 publications

References 6 publications

Thermochromatographic studies of plutonium oxides

Thermochromatographic studies of plutonium oxides

On the multi-reference nature of plutonium oxides: PuO₂²⁺, PuO₂, PuO₃ and PuO₂(OH)₂

Plutonium and Plutonium Compounds

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Volatile molecule PuO3 observed from subliming plutonium dioxide

Cited by 33 publications

References 6 publications

Thermochromatographic studies of plutonium oxides

Thermochromatographic studies of plutonium oxides

On the multi-reference nature of plutonium oxides: PuO22+, PuO2, PuO3 and PuO2(OH)2

Plutonium and Plutonium Compounds

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On the multi-reference nature of plutonium oxides: PuO₂²⁺, PuO₂, PuO₃ and PuO₂(OH)₂