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HANDBOOK ON THE PHYSICS AND CHEMISTRY OF RARE EARTHS Advisory Editorial Board GIN-YA ADACHI Kobe, Japan WILLIAM J. EVANS Irvine, USA YURI GRIN Dresden, Germany SUZAN M. KAUZLARICH Davis, USA MICHAEL F. REID Canterbury, New Zealand CHUNHUA YAN Beijing, P.R. China Editors Emeritus KARL A. GSCHNEIDNER, JR Ames, USA LEROY EYRINGw Tempe, USA w Deceased (2005) North-HollandisanimprintofElsevier Radarweg29,POBox211,1000AEAmsterdam, TheNetherlands TheBoulevard,LangfordLane,Kidlington,OxfordOX51GB,UK Copyright©2015Elsevier B.V.Allrightsreserved Nopart ofthispublicationmaybereproducedortransmittedinanyformorbyany means,electronic ormechanical, includingphotocopying,recording, orany informationstorageandretrieval system, withoutpermissioninwritingfromthe publisher.Detailsonhowtoseekpermission,furtherinformationaboutthePublisher’s permissionspoliciesandourarrangementswithorganizationssuchastheCopyright Clearance CenterandtheCopyrightLicensingAgency, canbefoundatourwebsite: www.elsevier.com/permissions. Thisbookandtheindividualcontributionscontainedinit areprotected under copyrightbythePublisher (otherthanasmaybenotedherein). 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ISBN:978-0-444-63483-2 ISSN:0168-1273 ForinformationonallNorth-Hollandpublications visitourwebsite athttp://store.elsevier.com/ Contributors NumbersinParenthesesindicatethepagesonwhichtheauthor’scontributionsbegin. Christopher L. Cahill (163), Department of Chemistry, The George Washington University, Washington, Districtof Columbia,USA Marek Daszkiewicz (109), Institute of Low Temperature and Structure Research, PolishAcademy ofSciences, Wrocław,Poland Olivier Q. De Clercq (1), LumiLab, Department of Solid State Sciences, Ghent University, Ghent, Belgium Lubomir D. Gulay (109), Department of Ecology and Protection of Environment, Eastern European NationalUniversity, Lutsk,Ukraine Qiong Jia(287),College ofChemistry, JilinUniversity, Changchun, China WupingLiao(287),StateKeyLaboratoryofRareEarthResourceUtilization,ERCfor the Separation and Purification of REs and Thorium, Changchun Institute of Applied Chemistry,Chinese Academyof Sciences, Changchun, China Oleg V. Marchuk (109), Department of Inorganic and Physical Chemistry, Eastern European NationalUniversity, Lutsk,Ukraine Dirk Poelman (1), LumiLab, Department of Solid State Sciences, Ghent University, Ghent, Belgium PhilippeF.Smet(1),LumiLab,DepartmentofSolidStateSciences,GhentUniversity, Ghent, Belgium Robert G. Surbella III (163), Department of Chemistry, The George Washington University, Washington, Districtof Columbia,USA Koen Van den Eeckhout (1), LumiLab, Department of Solid State Sciences, Ghent University, Ghent, Belgium ZhifengZhang(287),StateKeyLaboratoryofRareEarthResourceUtilization,ERC for the Separation and Purification of REs and Thorium, Changchun Institute of Applied Chemistry,Chinese Academyof Sciences, Changchun, China vii Preface These elements perplex us in our reaches [sic], baffle us in our speculations, and haunt us in our very dreams. They stretch like an unknown sea before us—mocking,mystifying,andmurmuringstrangerevelationsandpossibilities. SirWilliamCrookes(February 16,1887) Volume 48 of the Handbook on the Physics and Chemistry of Rare Earths adds four chapters to the series, covering broadly different, but timely, sub- jects ranging from luminescent materials to properties of chalcogenides, ura- nyl hybrid materials, and separation processes. Featured themes include persistent luminescence, a phenomenon used in emerging applications such as signage and bioimaging, the phase diagrams, structure, and physical prop- erties of quaternary rare earth/lead/group IV (Si, Ge, Sn)/sulfur or selenium compounds, structural chemistry of crystalline uranyl-containing compounds obtained via hydrothermal synthesis, as well as description of state-of-the- artinseparationandpurificationprocessesofrareearthsalongwiththeprep- aration of high-purity rare-earth and thorium metals. The first chapter (Chapter 274) is devoted to persistent luminescence, a phenomenon whereby a compound keeps emitting light for a long time after excitation is switched off. Ancient civilizations knew about this curious phenomenon, but the first account of it in the Western world dates back to the seventeenth century when the Bologna stone, obtained by calcining barite, wasdescribed.Theemissionoflightinsuchmaterialsdependsontrapsgener- atedbytinyamountsofimpurities;hence,differentsyntheticconditionsleadto widelydifferentemissioncolors.Studyingthisfascinatingphenomenonisdiffi- cultsothatitremainedacuriosityuntilthetwentiethcenturywhenzincsulfide dopedwithtransitionmetals(cobalt,copper)startedtoplayanimportantrolein luminous paints. Contributions of lanthanides to the field started at the end of the1960swhenstrontiumaluminatedopedwithdivalenteuropiumwasdiscov- ered.Afurtheranddecisiveimpetusoccurredinthemid-1990sinitiatedbythe finding that co-doping trivalent dysprosium in this material produced a much brighterpersistentphosphor. Thechapterreviewsallaspectsoflanthanideper- sistentluminescencealongwithacriticalevaluationofpotentialapplicationsin marking, solar energy conversion, and biosciences. Quaternary rare-earth chalcogenide systems R X dPbXdZX (X¼S, 2 3 2 Se; Z¼Si, Ge, Sn) are the subject of Chapter 275. These compounds are of broad interest in both basic and applied sciences due to their intriguing ix x Preface thermal, optical, electrical, and magnetic properties. The design of increas- ingly complex chalcogenide compounds is indeed vital for modern materials science, primarily in reference to the development of nonlinear optical devices.Thesystemsbasedonlead,sulfur,andseleniumareofspecialimpor- tance because substitution of lead with rare earths results in modified optical and magnetic properties that can be modulated while preserving the parent crystal structure. These new phases can also be obtained at the nanoscale, whichconsiderablybroadenstheirpotentialapplications,forinstanceincatal- ysis, biotechnology, or medicine. In this review, synthetic conditions are detailed, followed by a systematic presentation of known phase diagrams, structures, and magnetic properties. Chapter276dealswithcrystallinehybridmaterialsofuranyl.Thesemateri- alscombineasubstrate(organicorinorganic)withuranylionoritscomplexes that are blended on the molecular scale. Generally speaking, hybrid materials arefoundinnumeroussystemsandcanbebroadlydividedintosol–gel(glasses, silica, organically modified xerogels), porous (metal-organic frameworks), mesoporous(silicates,zeolites),polymeric,intercalation(layereddoublehydro- xides), and nanocomposite (nanoparticles) materials. Uranyl hydrolysis and complex aqueous speciation are the red thread of the review as they represent drivers for structural diversity. The chapter explores covalent bonding with O- and N-donor ligands before highlighting ways of programming targeted coordinationgeometries,compositions,andconnectivitiesintothehybridmate- rials. Purely supramolecular systems, assembled thanks to noncovalent bonds from simple tectons under highconcentrations of anionssuchaschloride, bro- mide,orisothiocyanate,arealsopresented.Finally,luminescencepropertiesare described, particularly with respect to structure/property relationships. The final chapter (Chapter 277) presents a historical insight as well as recent progresses in separation processes of rare earths, with a special focus on Chinese operations. Rare earth ores always contain a blend of several elements, and if some applications rely on mixtures (e.g., the Mischmetal, neodymium/praseodymium/dysprosium mixtures for magnets, or lanthanum/ cerium mixtures for nickel metal hydride batteries or catalysts), many high-technology uses need high-purity individual elements. Separation and purification operations are complex, time consuming, and have negative environmental effects. This points to the importance of developing efficient separation taking into account environmental issues, by making use of “greener” reactants and/or by recycling the chemicals involved. Both funda- mental and applied investigations have to be combined to reach this goal. The chapter reviews the various extractants, methods, and equipment that have been developed for achieving efficient methodologies, progresses being sustainedbyadequatetheoreticalmodeling.Itendsbydescribingtechnologies for the production of very high-purity rare-earth elements and thorium, a by-product of rare-earth extraction. Preface xi CHAPTER 274: PERSISTENT PHOSPHORS Philippe F. Smet, Koen Van den Eeckout, Olivier Q. De Clercq, and Dirk Poelman LumiLab, Department of Solid State Sciences, Ghent University, Ghent, Belgium. E-mail: [email protected] Synthesis Outlook Characterization release capture In vivo absorption emission traps Visibility imaging Mechano- Materials luminescence overview Thermoluminescence Persistent luminescence is the phenomenon whereby a material keeps emittinglightforsecondstohoursaftertheexcitationhasstopped.Thischap- ter describes the history of this class of materials and how the discovery of a new family of very efficient persistent phosphors has given a boost to the development of both new materials and applications. Synthesis conditions and analytical techniques specific to persistent luminescent compounds are described, together with ways to evaluate their performance in terms of human eye perception. A state of the art is presented about the materials— hostsanddopants—currentlyinvestigatedforpersistentluminescence,consis- tently referring to the original literature. Finally, in vivo medical imaging is shown to be a promising but challenging application of long-wavelength per- sistent luminescence and the relation between persistent luminescence and mechanoluminescence are described. xii Preface CHAPTER 275: QUATERNARY R X dPbXdZX 2 3 2 (X5S, Se; Z5Si, Ge, Sn) CHALCOGENIDES Lubomir D. Gulay*, Marek Daszkiewicz†, and Oleg V. Marchuk** *DepartmentofEcologyandProtectionofEnvironment,EasternEuropean University, Lutsk, Ukraine †InstituteofLow-TemperatureandStructureResearch,PolishAcademyof Sciences, Wroclaw, Poland. E-mail: [email protected] **Department of Inorganic and Physical Chemistry, Eastern European National University, Lutsk, Ukraine Complex ternary, quaternary, and multicomponent chalcogenides contain- ingrareearthsareinterestingbecauseofpotentialapplicationsinthefieldsof ionic conductivity and nonlinear optics. The current knowledge about experi- mental investigations of phase diagrams, crystallographic relationships, and magneticpropertiesofquaternaryrare-earthchalcogenidesR X dPbXdZX 2 3 2 (X¼S, Se; Z¼Si, Ge, Sn) is the focus of the chapter. The initial section describes typical preparation of these novel materials in small quantities for studiesoftheirbasicphysicalpropertiesandservesasaguideforthoseinter- estedinpreparinglargerquantitiesinordertoexploretheirpotentialforprac- tical applications. Then the structure types of ternary PbdZdX (X¼S, Se; Z¼Si, Ge, Sn) systems are presented, before the review concentrates on the rare-earth-containing quaternary chalcogenides that are discussed according to their structure type. Description of superstructures and known magnetic properties concludes the chapter. Preface xiii CHAPTER 276: HYBRID MATERIALS OF THE f-ELEMENTS PART II: THE URANYL CATION Robert G. Surbella III and Christopher L. Cahill The George Washington University, Washington, DC, USA. E-mail: [email protected] Thecatalogofuranyl-bearinghybridmaterialshasexpandedconsiderably over the past 10–15 years. Researchers have drawn inspiration from the rich portfolio of structural topologies found in naturally occurring uranyl mineral phases where uranyl oligomerization stemming from hydrolysis is the norm. With these phenomena as guiding principles, our group in particular has pur- sued a program of exploring the relationship between synthetic reaction con- ditions, including ligand geometries and functionalities, with solid-state structure. As the synthetic efforts have flourished, a wide variety of structure types have emerged, yet the ability to fully correlate reaction conditions with resulting topologies remains elusive. As such, this chapter provides an over- view of (whenever possible) synthetic “causes and effects” in the hydrother- mal synthesis of uranyl hybrid materials. It then progresses to more recent developments wherein milder, high anion conditions are utilized to develop themes of assembly via noncovalent interactions between a more restricted suite of uranyl species. xiv Preface CHAPTER 277: PROGRESS IN THE SEPARATION PROCESSES FOR RARE EARTH RESOURCES Zhifeng Zhang1, Qiong Jia2, Wuping Liao1,* 1State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun. E-mail: [email protected] 2College of Chemistry, Jilin University, Changchun, China RE mines Novel extractants Ion exchange Solvent Separation Extraction equipment extraction processes Double salt precipitation Theoretical modeling RE oxides High-purity REs Rare earth elements have widespread applications in materials critical for many high-technology applications, including catalysts, permanent magnets, phosphors, lasers, and rechargeable batteries. Individual rare-earth elements are oftenneeded sothat separation and purification ofrare-earth concentrates are crucial. Importantly, these operations are suffering from environmental problems and viable utilization of the resources. The chapter gives an over- view of the evolution in fundamental research and industrial separation pro- cesses for rare earths. First, the progresses in extractants, novel equipment, alternative technologies, and theoretical modeling are summarized. Industrial hydrometallurgy processesare discussedand evaluatedwith respecttodiffer- ent ores of various origins. The preparation of highly pure rare earths and associated elements such as thorium is then presented. Easily accessible resources and environmentally friendly processes are essential issues to deal with in order to ensure sustainable developments in rare earth metallurgy. Jean-Claude G. Bu¨nzli Vitalij K. Pecharsky Contents of Volumes 1–47 VOLUME1:Metals 1978,1strepr.1982,2ndrepr.1991;ISBN0-444-85020-1 1. Z.B.Goldschmidt,Atomicproperties(freeatom) 1 2. B.J.BeaudryandK.A.GschneidnerJr,Preparationandbasicpropertiesoftherare earthmetals 173 3. S.H.Liu,Electronicstructureofrareearthmetals 233 4. D.C.KoskenmakiandK.A.GschneidnerJr,Cerium 337 5. L.J.Sundstr€om,Lowtemperatureheatcapacityoftherareearthmetals 379 6. K.A.McEwen,Magneticandtransportpropertiesoftherareearths 411 7. S.K.Sinha,Magneticstructuresandinelasticneutronscattering:metals,alloysand compounds 489 8. T.E.Scott,Elasticandmechanicalproperties 591 9. A.Jayaraman,Highpressurestudies:metals,alloysandcompounds 707 10. C.ProbstandJ.Wittig,Superconductivity:metals,alloysandcompounds 749 11. M.B.Maple,L.E.DeLongandB.C.Sales,Kondoeffect:alloysandcompounds 797 12. M.P.Dariel,Diffusioninrareearthmetals 847 Subjectindex 877 VOLUME2:Alloysandintermetallics 1979,1strepr.1982,2ndrepr.1991;ISBN0-444-85021-X 13. A.landelliandA.Palenzona,Crystalchemistryofintermetalliccompounds 1 14. H.R.KirchmayrandC.A.Poldy,Magneticpropertiesofintermetalliccompoundsof rareearthmetals 55 15. A.E.Clark,MagnetostrictiveRFe intermetalliccompounds 231 2 16. J.J.Rhyne,Amorphousmagneticrareearthalloys 259 17. P.Fulde,Crystalfields 295 18. R.G.Barnes,NMR,EPRandM€ossbauereffect:metals,alloysandcompounds 387 19. P.Wachter,Europiumchalcogenides:EuO,EuS,EuSeandEuTe 507 20. A.Jayaraman,Valencechangesincompounds 575 Subjectindex 613 VOLUME3:Non-metalliccompounds–I 1979,1strepr.1984;ISBN0-444-85215-8 21. L.A.HaskinandT.P.Paster,Geochemistryandmineralogyoftherareearths 1 22. J.E.Powell,Separationchemistry 81 23. C.K.Jørgensen,Theoreticalchemistryofrareearths 111 24. W.T.Carnall,Theabsorptionandfluorescencespectraofrareearthionsin solution 171 25. L.C.Thompson,Complexes 209 26. G.G.LibowitzandA.J.Maeland,Hydrides 299 27. L.Eyring,Thebinaryrareearthoxides 337 28. D.J.M.BevanandE.Summerville,Mixedrareearthoxides 401 xv
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