On Studtite and Lts Composition
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Paulscherrerite from the Number 2 Workings, Mount Painter Inlier, Northern Flinders Ranges, South Australia: “Dehydrated Schoepite” Is a Mineral After All
American Mineralogist, Volume 96, pages 229–240, 2011 Paulscherrerite from the Number 2 Workings, Mount Painter Inlier, Northern Flinders Ranges, South Australia: “Dehydrated schoepite” is a mineral after all JOËL BRUGGER,1,2,* NICOLAS MEISSER,3 BAR B ARA ETSCH M A nn ,1 STEFA N AN SER M ET ,3 A N D ALLA N PRI N G 2 1Tectonics, Resources and Exploration (TRaX), School of Earth and Environmental Sciences, University of Adelaide, SA-5005 Adelaide, Australia 2Division of Mineralogy, South Australian Museum, SA-5000 Adelaide, Australia 3Musée Géologique and Laboratoire des Rayons-X, Institut de Minéralogie et de Géochimie, UNIL—Anthropole, CH-1015 Lausanne-Dorigny, Switzerland AB STRACT Paulscherrerite, UO2(OH)2, occurs as an abundant dehydration product of metaschoepite at the Number 2 Workings at Radium Ridge, Northern Flinders Ranges, South Australia. The mineral name honors the contribution of Swiss physicist Paul Scherrer (1890–1969) to mineralogy and nuclear physics. Individual paulscherrerite crystals are tabular, reaching a maximum of 500 nm in length. Paulscherrerite has a canary yellow color and displays no fluorescence under UV light. Chemically, paulscherrerite is a pure uranyl hydroxide/hydrate, containing only traces of other metals (<1 wt% in total). Bulk (mg) samples always contain admixtures of metaschoepite (purest samples have ~80 wt% paulscherrerite). A thermogravimetric analysis corrected for the presence of metaschoepite contamina- tion leads to the empirical formula UO3·1.02H2O, and the simplified structural formula UO2(OH)2. Powder diffraction shows that the crystal structure of paulscherrerite is closely related to that of synthetic orthorhombic α-UO2(OH)2. However, splitting of some X-ray diffraction lines suggests a monoclinic symmetry for type paulscherrerite, with a = 4.288(2), b = 10.270(6), c = 6.885(5) Å, β = 3 90.39(4)°, V = 303.2(2) Å , Z = 4, and possible space groups P2, P21, P2/m, or P21/m. -
Mineral Processing
Mineral Processing Foundations of theory and practice of minerallurgy 1st English edition JAN DRZYMALA, C. Eng., Ph.D., D.Sc. Member of the Polish Mineral Processing Society Wroclaw University of Technology 2007 Translation: J. Drzymala, A. Swatek Reviewer: A. Luszczkiewicz Published as supplied by the author ©Copyright by Jan Drzymala, Wroclaw 2007 Computer typesetting: Danuta Szyszka Cover design: Danuta Szyszka Cover photo: Sebastian Bożek Oficyna Wydawnicza Politechniki Wrocławskiej Wybrzeze Wyspianskiego 27 50-370 Wroclaw Any part of this publication can be used in any form by any means provided that the usage is acknowledged by the citation: Drzymala, J., Mineral Processing, Foundations of theory and practice of minerallurgy, Oficyna Wydawnicza PWr., 2007, www.ig.pwr.wroc.pl/minproc ISBN 978-83-7493-362-9 Contents Introduction ....................................................................................................................9 Part I Introduction to mineral processing .....................................................................13 1. From the Big Bang to mineral processing................................................................14 1.1. The formation of matter ...................................................................................14 1.2. Elementary particles.........................................................................................16 1.3. Molecules .........................................................................................................18 1.4. Solids................................................................................................................19 -
Uraninite Alteration in an Oxidizing Environment and Its Relevance to the Disposal of Spent Nuclear Fuel
TECHNICAL REPORT 91-15 Uraninite alteration in an oxidizing environment and its relevance to the disposal of spent nuclear fuel Robert Finch, Rodney Ewing Department of Geology, University of New Mexico December 1990 SVENSK KÄRNBRÄNSLEHANTERING AB SWEDISH NUCLEAR FUEL AND WASTE MANAGEMENT CO BOX 5864 S-102 48 STOCKHOLM TEL 08-665 28 00 TELEX 13108 SKB S TELEFAX 08-661 57 19 original contains color illustrations URANINITE ALTERATION IN AN OXIDIZING ENVIRONMENT AND ITS RELEVANCE TO THE DISPOSAL OF SPENT NUCLEAR FUEL Robert Finch, Rodney Ewing Department of Geology, University of New Mexico December 1990 This report concerns a study which was conducted for SKB. The conclusions and viewpoints presented in the report are those of the author (s) and do not necessarily coincide with those of the client. Information on SKB technical reports from 1977-1978 (TR 121), 1979 (TR 79-28), 1980 (TR 80-26), 1981 (TR 81-17), 1982 (TR 82-28), 1983 (TR 83-77), 1984 (TR 85-01), 1985 (TR 85-20), 1986 (TR 86-31), 1987 (TR 87-33), 1988 (TR 88-32) and 1989 (TR 89-40) is available through SKB. URANINITE ALTERATION IN AN OXIDIZING ENVIRONMENT AND ITS RELEVANCE TO THE DISPOSAL OF SPENT NUCLEAR FUEL Robert Finch Rodney Ewing Department of Geology University of New Mexico Submitted to Svensk Kämbränslehantering AB (SKB) December 21,1990 ABSTRACT Uraninite is a natural analogue for spent nuclear fuel because of similarities in structure (both are fluorite structure types) and chemistry (both are nominally UOJ. Effective assessment of the long-term behavior of spent fuel in a geologic repository requires a knowledge of the corrosion products produced in that environment. -
Studtite UO4 • 4H2O C 2001-2005 Mineral Data Publishing, Version 1
Studtite UO4 • 4H2O c 2001-2005 Mineral Data Publishing, version 1 Crystal Data: Monoclinic, pseudohexagonal. Point Group: 2/m, m, or 2. Needlelike crystals, elongated along [001], to 1 mm, in radial fibrous aggregates and crusts. Physical Properties: Tenacity: Flexible. Hardness = Soft. D(meas.) = 3.58 (synthetic). D(calc.) = 3.64 Radioactive. Optical Properties: Translucent to transparent. Color: Yellow to pale yellow; nearly colorless in transmitted light. Luster: Vitreous. Optical Class: Biaxial (+). Orientation: Z = elongation. α = 1.537–1.551 β = 1.555–1.686 γ = 1.680–1.690 2V(meas.) = Small. Cell Data: Space Group: C2/m, Cm, or C2. a = 11.85(2) b = 6.80(1) c = 4.25(1) β =93◦51(20)0 Z=2 X-ray Powder Pattern: Menzenschwand, Germany. 5.93 (10), 3.40 (8), 2.96 (6), 2.23 (6), 2.02 (5), 1.970 (5b), 4.27 (4) Chemistry: Qualitative microchemical and electron microprobe analyses typically show major U with traces of Pb, H2O, CO3 attributed to impurities. Characterization of naturally-occurring material thus rests on equivalence of the X-ray pattern and optical properties with the synthetic compound, and chemical behavior as a peroxide. Occurrence: A very rare mineral in the oxidized zone of some uranium-bearing mineral deposits. Association: Uranophane, rutherfordine, lepersonnite (Shinkolobwe, Congo); billietite, uranophane, rutherfordine, barite, quartz, hematite, “limonite” (Menzenschwand, Germany); tengchongite, calcurmolite, kivuite (Tengchong Co., China). Distribution: From Shinkolobwe, Katanga Province, Congo (Shaba Province, Zaire). At Menzenschwand, Black Forest, Germany. From Mitterberg, Salzburg, Austria. In France, at Davignac, Corr`eze,and from the Mas-d’Alary uranium deposit, three km south-southeast of Lod`eve, H´erault.In Tengchong Co., and at Tongbiguan village, Yingjiang Co., Yunnan Province, China. -
Thermodynamics of Uranyl Minerals: Enthalpies of Formation of Rutherfordine, UO2CO3
American Mineralogist, Volume 90, pages 1284–1290, 2005 Thermodynamics of uranyl minerals: Enthalpies of formation of rutherfordine, UO2CO3, andersonite, Na2CaUO2(CO3)3(H2O)5, and grimselite, K3NaUO2(CO3)3H2O KARRIE-ANN KUBATKO,1 KATHERYN B. HELEAN,2 ALEXANDRA NAVROTSKY,2 AND PETER C. BURNS1,* 1Department of Civil Engineering and Geological Sciences, University of Notre Dame, 156 Fitzpatrick Hall, Notre Dame, Indiana 46556, U.S.A. 2Thermochemistry Facility and NEAT ORU, University of California at Davis, One Shields Avenue, Davis, California 95616, U.S.A. ABSTRACT Enthalpies of formation of rutherfordine, UO2CO3, andersonite, Na2CaUO2(CO3)3(H2O)5, and grimselite, K3NaUO2(CO3)3(H2O), have been determined using high-temperature oxide melt solution Δ calorimetry. The enthalpy of formation of rutherfordine from the binary oxides, Hr-ox, is –99.1 ± 4.2 Δ kJ/mol for the reaction UO3 (xl, 298 K) + CO2 (g, 298 K) = UO2CO3 (xl, 298 K). The Hr-ox for ander- sonite is –710.4 ± 9.1 kJ/mol for the reaction Na2O (xl, 298 K) + CaO (xl, 298 K) + UO3 (xl, 298 K) Δ + 3CO2 (g, 298 K) + 5H2O (l, 298 K) = Na2CaUO2(CO3)3(H2O)6 (xl, 298 K). The Hr-ox for grimselite is –989.3 ± 14.0 kJ/mol for the reaction 1.5 K2O (xl, 298 K) + 0.5Na2O (xl, 298 K) + UO3 (xl, 298 K) + 3CO2 (g, 298 K) + H2O (l, 298 K) = K3NaUO2(CO3)3H2O (xl, 298 K). The standard enthalpies of Δ formation from the elements, Hº,f are –1716.4 ± 4.2, –5593.6 ± 9.1, and –4431.6 ± 15.3 kJ/mol for rutherfordine, andersonite, and grimselite, respectively. -
Periodic DFT Study of the Structure, Raman Spectrum and Mechanical
Periodic DFT Study of the Structure, Raman Spectrum and Mechanical Properties of Schoepite Mineral Francisco Colmeneroa*, Joaquín Cobosb and Vicente Timóna aInstituto de Estructura de la Materia (IEM-CSIC). C/ Serrano, 113. 28006 – Madrid, Spain. bCentro de Investigaciones Energéticas, Medioambientales y Tecnológicas (CIEMAT). Avda/ Complutense, 40. 28040 – Madrid, Spain. Orcid Francisco Colmenero: https://orcid.org/0000-0003-3418-0735 Orcid Joaquín Cobos: https://orcid.org/0000-0003-0285-7617 Orcid Vicente Timón: https://orcid.org/0000-0002-7460-7572 *E-mail: [email protected] 1 ABSTRACT The structure and Raman spectrum of schoepite mineral, [(UO2)8O2(OH)12] · 12 H2O, was studied by means of theoretical calculations. The computations were carried out by using Density Functional Theory with plane waves and pseudopotentials. A norm-conserving pseudopotential specific for the uranium atom developed in a previous work was employed. Since it was not possible to locate hydrogen atoms directly from X-ray diffraction data by structure refinement in the previous experimental studies, all the positions of the hydrogen atoms in the full unit cell were determined theoretically. The structural results, including the lattice parameters, bond lengths, bond angles and X-ray powder pattern were found in good agreement with their experimental counterparts. However, the calculations performed using the unit cell designed by Ostanin and Zeller in 2007, involving half of the atoms of the full unit cell, leads to significant errors in the computed X-ray powder pattern. Furthermore, Ostanin and Zeller’s unit cell contains hydronium ions, + H3O , that are incompatible with the experimental information. Therefore, while the use of this schoepite model may be a very useful approximation requiring a much smaller amount of computational effort, the full unit cell should be used to study this mineral accurately. -
Study of the Thermal Stability of Studtite by in Situ Raman Spectroscopy And
Study of the thermal stability of studtite by in situ Raman spectroscopy and DFT calculations Francisco Colmeneroa*, Laura J. Bonalesb, Joaquín Cobosb, Vicente Timóna aInstituto de Estructura de la Materia, CSIC. C/ Serrano, 113. 28006 Madrid, Spain bCentro de Investigaciones Energéticas, Medioambientales y Tecnológicas, CIEMAT. Avda/ Complutense, 40. 28040 Madrid, Spain * Corresponding author. Tel.+34 915616800 Ext. 941033 E-mail address: [email protected] Abstract The design of a safe spent nuclear fuel repository requires the knowledge of the stability of the secondary phases which precipitate when water reaches the fuel surface. Studtite is recognized as one of the secondary phases that play a key-role in the mobilization of the radionuclides contained in the spent fuel. Thereby, it has been identified as a product formed under oxidation conditions at the surface of the fuel, and recently found as a corrosion product in the Fukushima-Daiichi nuclear plant accident. Thermal stability is one of the properties that should be determined due to the high temperature of the fuel. In this work we report a detailed analysis of the structure and thermal stability of studtite. The structure has been studied both by experimental techniques (SEM, TGA, XRD and Raman spectroscopy) and theoretical DFT electronic structure and spectroscopic calculations. The comparison of the results allows us to perform for the first time the Raman bands assignment of the whole spectrum. The thermal stability of studtite has been analyzed by in situ Raman spectroscopy, with the aim of studying the effect of the heating rate and the presence of water. -
Identification and Occurrence of Uranium and Vanadium Minerals from the Colorado Plateaus
SpColl £2' 1 Energy I TEl 334 Identification and Occurrence of Uranium and Vanadium Minerals from the Colorado Plateaus ~ By A. D. Weeks and M. E. Thompson ~ I"\ ~ ~ Trace Elements Investigations Report 334 UNITED STATES DEPARTMENT OF THE INTERIOR GEOLOGICAL SURVEY IN REPLY REFER TO: UNITED STATES DEPARTMENT OF THE INTERIOR GEOLOGICAL SURVEY WASHINGTON 25, D. C. AUG 12 1953 Dr. PhilUp L. Merritt, Assistant Director Division of Ra1'r Materials U. S. AtoTILic Energy Commission. P. 0. Box 30, Ansonia Station New· York 23, Nei< York Dear Phil~ Transmitted herewith are six copies oi' TEI-334, "Identification and occurrence oi' uranium and vanadium minerals i'rom the Colorado Plateaus," by A , D. Weeks and M. E. Thompson, April 1953 • We are asking !41'. Hosted to approve our plan to publish this re:por t as a C.i.rcular .. Sincerely yours, Ak~f777.~ W. H. ~radley Chief' Geologist UNCLASSIFIED Geology and Mineralogy This document consists or 69 pages. Series A. UNITED STATES DEPARTMENT OF TEE INTERIOR GEOLOGICAL SURVEY IDENTIFICATION AND OCCURRENCE OF URANIUM AND VANADIUM MINERALS FROM TEE COLORADO PLATEAUS* By A• D. Weeks and M. E. Thompson April 1953 Trace Elements Investigations Report 334 This preliminary report is distributed without editorial and technical review for conformity with ofricial standards and nomenclature. It is not for public inspection or guotation. *This report concerns work done on behalf of the Division of Raw Materials of the u. s. Atomic Energy Commission 2 USGS GEOLOGY AllU MINEFALOGY Distribution (Series A) No. of copies American Cyanamid Company, Winchester 1 Argulllle National La:boratory ., ., ....... -
SIMPLE URANIUM OXIDES, HYDROXIDES U4+ + U6+, SIMPLE and COMPLEX URANYL HYDROXIDES in ORES Andrey A
New Data on Minerals. 2011. Vol. 46 71 SIMPLE URANIUM OXIDES, HYDROXIDES U4+ + U6+, SIMPLE AND COMPLEX URANYL HYDROXIDES IN ORES Andrey A. Chernikov Fersman Mineralogical Museum, Russian Academy of Sciences, Moscow, [email protected], [email protected] The review of published and new own data of simple uranium oxides revealed that the formation of five simple oxides is probable: nasturan, sooty pitchblende, uraninite, uranothorianite, and cerianite. Among simple oxides, nasturan, sooty pitchblende, and uraninite are the most abundant in ores varied in genesis and mineralogy. Uranothorianite or thorium uraninite (aldanite) is occasional in the ores, while cerianite is believed in U-P deposits of Northern Kazakhstan. Hydrated nasturan is the most abundant among three uranium (IV+VI) hydroxides in uranium ores. Insignificant ianthinite was found in few deposits, whereas cleusonite was indentified only in one deposit. Simple uranyl hydroxides, schoepite, metaschoepite, and paraschoepite, are widespread in the oxidized ores of the near-surface part of the Schinkolobwe deposit. They are less frequent at the deeper levels and other deposits. Studtite and metastudtite are of insignificant industrial importance, but are of great inter- est to establish genesis of mineral assemblages in which they are observed, because they are typical of strongly oxidized conditions of formation of mineral assemblages and ores. The X-ray amorphous urhite associated with hydrated nasturan and the X-ray amorphous hydrated matter containing ferric iron and U6+ described for the first time at the Lastochka deposit, Khabarovsk krai, Russia are sufficiently abundant uranyl hydroxides in the oxidized uranium ores. Significant complex uranyl hydroxides with interlayer K, Na, Ca, Ba, Cu, Pb, and Bi were found basically at a few deposits: Schinkolobwe, Margnac, Wölsendorf, Sernyi, and Tulukuevo, and are less frequent at the other deposits, where quite large monomineralic segregations of nasturan and crystals of uraninite were identified. -
Thermodynamic Properties of Uranyl Containing Materials Based On
Thermodynamic Properties of Uranyl Containing Materials Based on Density Functional Theory Francisco Colmeneroa*, Ana María Fernándezb, Joaquín Cobosb and Vicente Timóna aInstituto de Estructura de la Materia (CSIC). C/ Serrano, 113. 28006 – Madrid, Spain. bCentro de Investigaciones Energéticas, Medioambientales y Tecnológicas (CIEMAT). Avda/ Complutense, 40. 28040 – Madrid, Spain. Orcid Francisco Colmenero: https://orcid.org/0000-0003-3418-0735 Orcid Ana María Fernández: https://orcid.org/0000-0002-8392-0165 Orcid Joaquín Cobos: https://orcid.org/0000-0003-0285-7617 Orcid Vicente Timón: https://orcid.org/0000-0002-7460-7572 *E-mail: [email protected] 1 ABSTRACT The thermodynamic properties of uranyl containing materials, including dehydrated schoepite, metastudtite, studtite, soddyite, rutherfordine and γ − UO3 were studied. These materials are among the most important secondary phases arising from corrosion of spent nuclear fuel under the final geological disposal conditions, and γ − UO3 is the main oxide of hexavalent uranium. The crystal structures of the dehydrated schoepite and metastudtite were determined by means of density functional theory using a new norm-conserving pseudopotential for uranium atom. The resulting structural properties and X-Ray powder patterns were found to be in very good agreement with the experimental data. By using the optimized structures of these materials, as well as of those obtained in previous works for studtite and soddyite, the thermodynamic properties of dehydrated schoepite, metastudtite, studtite and soddyite were determined, including specific heats, entropies, enthalpies and Gibbs free energies. Finally, the computed thermodynamic properties of these materials together with those reported previously for rutherfordine and γ − UO3 were used to determine their enthalpies and free energies of formation, and their variation with temperature. -
Additional Studies on Mixed Uranyl Oxide-Hydroxide Hydrate
t45 TheC anadian M brc rala gis t Vol.35, pp. 145-r5r (1997) ADDITIONALSTUDIES ON MIXEDURANYL OXIDE-HYDROXIDE HYDRATE ALTERATIONPRODUCTS OF URANINITEFROM THE PALERMOAND RUGGLESGRANITIC PEGMATITES. GRAFTON COUNTV, NEW HAMPSHIRE EUGENEE. FOORD1 IJ.S. Geolagical Survey, Denver Fedzral Center,.Box 25M6, Mail Stop 905, Dewer, Colarado 80225, U.S-L STANLEYL. KORZEB 13993East Arkona Avmuz, Aurora, CoLorado80012, U.S.A. FREDERICKE. LICHTE U.S.GeoLogical Suney, DenverFederal Cewer,Box 25M6, Mail Snp 973, Denver, Colorado80225, U.SA. JOANJ. FIT?ATRICK U.S.Geolagical Survey, Dmver Fedcral Cewen Box 25M6, Mail Stop912, Denver, Colorado80225, U.SA- ABSTRACT Additional studieson an incompletely characterizedsecondary uranium 'hineral" from the Rugglesand Palermogranitic Fgmatites, New HampshAe,refened to as mineral "A' by Frondel (1956), reveal a mixnre of schoepit€-goupminerals and related nranyl oxide-hydroxide hydrated compounds.A compositechemical analysis yielded (in wt-Vo):PbO 4,85 (EMP), UOa 83.5 (EMP), BaO 0.675 (av. of EMP and ICP), CaO 0.167 (av. of EMP and ICP), KzO 2.455 (av. of EMP and ICP), SrO 021 (ICP), ThO20.85 (CP), HzO 6.9, D9.61. Powder-diffractionX-ray studiesindicaJe a closeresemblance in paffemsbetween mineral "A" atrd severaluranyl oxide-hydroxidehydrated minerals, including the schoepitefamily of mineralsand UOz(OFI)2. The powderdiffraction data for mineral "A" are most similar to those for syntheticUOzrlSHzO and UOz(OII), but other phasesare likely presentas well, TGA analysisof both mineral 'A' and metaschoepiteshow similar weigbt-loss and first derivativecurves. The dominantlosses are at 100'C, with secondaryevents aJ 4{Do and 6@"C. IR spectrashow the prasenceof (OII) andHzO. -
Leaching of Actinides and Other Radionuclides from Matrices of Chernobyl ‘‘Lava” As Analogues of Vitrified HLW ⇑ Bella Yu
J. Chem. Thermodynamics 114 (2017) 25–29 Contents lists available at ScienceDirect J. Chem. Thermodynamics journal homepage: www.elsevier.com/locate/jct Leaching of actinides and other radionuclides from matrices of Chernobyl ‘‘lava” as analogues of vitrified HLW ⇑ Bella Yu. Zubekhina, Boris E. Burakov V.G. Khlopin Radium Institute (KRI), 2nd Murinsky av. 28, St. Petersburg 194021, Russia article info abstract Article history: The paper commemorates the 30th anniversary of the severe nuclear accident at the Fourth Unit of the Received 11 July 2016 Chernobyl Nuclear Power Plant. Results of the investigation of radioactive glassy lava-like materials Accepted 25 August 2016 formed as a result of the accident are presented. Leaching of Pu, Am and Cs in distilled water and sodium Available online 26 August 2016 carbonate solution at 25 °C from matrices of black and brown Chernobyl ‘‘lava” is comparable, however, leaching of Cs from black ‘‘lava” in seawater at 25 and 90 °C is almost 2 times higher than that for brown Keywords: ‘‘lava”. Chemical alteration of black and brown ‘‘lava” in seawater is much more intensive that in distilled Chernobyl ‘‘lava” water and sodium carbonate solution. Comparison of leaching behavior of Chernobyl ‘‘lava” and aged Actinides samples of nuclear glass is not clear so far because of the lack of data. Further study of Chernobyl ‘‘lava” Leaching Nuclear glass as analogues of vitrified high level waste (HLW) and possibly, Fukushima’s corium is needed. Ó 2016 Elsevier Ltd. 1. Introduction inclusions of uranium oxide phases containing up to several wt% zirconium [10]. Black ‘‘lava” contains fewer inclusions and its color The severe nuclear accident at the Fourth Unit of the Chernobyl can be related to uranium dissolved in the glass matrix and to radi- Nuclear Power Plant (ChNPP) on 26 April 1986 was accompanied ation defects.