The Analysis of Nuclear Materials and Their Environments PDF
Preview The Analysis of Nuclear Materials and Their Environments
Claude André Degueldre The Analysis of Nuclear Materials and Their Environments The Analysis of Nuclear Materials and Their Environments é Claude Andr Degueldre The Analysis of Nuclear Materials and Their Environments 123 ClaudeAndréDegueldre Engineering Department Lancaster University Lancaster UK and Department ofAnalytical andMineral Chemistry University of Geneva Geneva Switzerland and Nuclear Energy Division PaulScherrer Institute Aargau Switzerland ISBN978-3-319-58004-3 ISBN978-3-319-58006-7 (eBook) DOI 10.1007/978-3-319-58006-7 LibraryofCongressControlNumber:2017939092 ©SpringerInternationalPublishingAG2017 Thisworkissubjecttocopyright.AllrightsarereservedbythePublisher,whetherthewholeorpart of the material is concerned, specifically the rights of translation, reprinting, reuse of illustrations, recitation, broadcasting, reproduction on microfilms or in any other physical way, and transmission orinformationstorageandretrieval,electronicadaptation,computersoftware,orbysimilarordissimilar methodologynowknownorhereafterdeveloped. The use of general descriptive names, registered names, trademarks, service marks, etc. in this publicationdoesnotimply,evenintheabsenceofaspecificstatement,thatsuchnamesareexemptfrom therelevantprotectivelawsandregulationsandthereforefreeforgeneraluse. The publisher, the authors and the editors are safe to assume that the advice and information in this book are believed to be true and accurate at the date of publication. Neither the publisher nor the authorsortheeditorsgiveawarranty,expressorimplied,withrespecttothematerialcontainedhereinor for any errors or omissions that may have been made. The publisher remains neutral with regard to jurisdictionalclaimsinpublishedmapsandinstitutionalaffiliations. Printedonacid-freepaper ThisSpringerimprintispublishedbySpringerNature TheregisteredcompanyisSpringerInternationalPublishingAG Theregisteredcompanyaddressis:Gewerbestrasse11,6330Cham,Switzerland Foreword I am very pleased to see this new book on The Analysis of Nuclear Materials and Their Environments by Claude Degueldre. The challenge of analyzing nuclear materials is that normal procedures are often difficult to use because of the high-radiation field surrounding the material, say with spent nuclear fuel. At the other end of the spectrum, the challenge is to analyze environmental materials in which concentrations of radionuclide are extremely low. In both cases, it is important to determine the solid-state chemistry of the nuclear material and the speciation of the radionuclide in the environment. This is exactly the type of data that are the foundation of safety analyses required by regulators for nuclear facilities. ProfessorDegueldrehaswrittenabookthatsystematicallypresentsandupdates the full range of analytical techniques that can be applied to nuclear materials and radionuclides in the environment. His treatment is comprehensive, dividing the techniquesintotwobroadcategories—thosebywhichamaterialmaybeexamined by passive techniques, such as particle scattering, and those that require an inter- actionoftheenergyoftheprobewiththesample,suchasthosethatcauseelectron excitations. For both cases, the explication of each technique emphasizes an understanding of the interactions and detection methods for the probe energy and solid/liquidinteractionsthatarethebasisforthedifferenttechniques.Bycombining thediscussionofthetechniquesintoasinglevolume,thereadercanalsoappreciate thedifferentlengthscalesatwhicheachprobesamplesthepropertiesofthenuclear material. This allows scientists to match the proper technique to the scientific questionthatisbeingasked.Iappreciatetheemphasisonthedetectionmethods,as detection is often the major challenge of an analytical technique. As the author emphasizes, the way forward with these challenging analytical problems is to combine techniques, taking advantage of the range of particle/wave interactions v vi Foreword with the samples. This book is a welcomed introduction to the panoply of approaches that are available to the modern analyst faced with the challenge of analyzing nuclear materials or radionuclides in the environment. May 2017 Rodney C. Ewing Frank Stanton Professor in Nuclear Security Center for International Security and Cooperation Stanford University Preface Nuclear materials and their environments require analyses before and during their utilizationaswellasafterserviceduringdisposalnotonlyfromthecurrentnuclear units but also from planned or foreseen nuclear installations or systems. Prior analysis, sampling, and sample treatment must be carried out when the analyticaltechniqueisnotappliedinsitu,inanon-invasiveway,orinanin-lineor on-line mode. Theanalysismaybecarriedoutinsitu,forexampleusingaremotesystem,orin anundergroundlaboratoryinthephaseunderconsideration.Theanalysismayalso be done ex situ with transfer of the sample and separation when needed. For all analyses, sample volume, mass or amount, the flux of reagent, the size of the analyzed part of the sample and the acquisition time or time of analysis are key parameters that may affect the detection limit. The information required—such as the chemical or radioisotope activity, the mass orvolumeofthesampledandanalyzeditem, theconcentration asfraction or molarityofdopantsorcontaminantsandthetypeorsizeofstructuresinthestudied phases—hastobedeterminedinamulti-scaleapproachatthenuclearscale,atomic or molecular scale, at the microscopic or macroscopic structural scale, at the bulk scale, at the component or system scale, and/or at the environmental or geo- graphical scale according to the requirements of the study. Identification concerns theactinides,fissionproductsoractivatedproductsasisotopesorelements,butalso their speciation that may not only be done at the molecular scale but also in a broader sense such as at the environmental level. The time scale ranges from the femtosecond, accessible during Free Electron Laser investigations to describe ultra-fast phenomena, through the nanosecond to the mega-second, then to the giga-second or penta-second the timescale of uranium-238 half-life or of the age of the fossil natural geo-reactors. The explored energy range along the analytical methods goes also from the nano-eV (Mössbauer or nuclear magnetic resonance spectroscopy) to the giga-eV (muon-tomography), for example. vii viii Preface Passive and active analytical methods have been revisited in this work, with examples of their utilization in transmission, injection, diffusion or reflection modes.Thesamplingarea,beamsizeandreagentquantitiesareeithermacroscopic, microscopic or nanoscopic in size, while spatial-temporal conditions make exci- tation incidence versus detection directions possible through solid angles, with synchronous detection or with temporal delay. Inthisworktheinvestigatedanalyticaltechniqueshavebeenclassifiedaccording to their interactions, if any, between incident waves, particles or injected reagents and the analyzed sample, and, for their detected or recorded signals. For passive techniques, excitations are absent and phonons, photons, leptons, neutrons or ions are detected or quantified for their energy, flux, activity, quantity or mass. For interactive techniques, irradiations or reagent additions are made with phonons, photons,leptons,neutronsorionswithaknownenergy,flux,activityormass.The irradiation or injection is done locally while the reception may be carried out in a given space at a given angle from the stimuli direction or the incident beam, instantaneously or after a certain delay after irradiation. Thedetectiontoolsarespectroscopy,microscopy,radiography,andtomography. The reaction takes place within or without a specific field such as electrical, magnetic,flowormechanicalacceleration.Thedetectedsignalmaybethesamein natureastheincidentone,withthesameenergy,elasticinteraction,orasignalwith lowerenergyandinelasticinteraction,withparticlesbeingagainphonons,photons, leptons,neutronsorions.Inadditiontotheseanalyticaltoolsortechniques,neutral species such as atoms or molecules may also be used to interrogate the material. Theyaretreated asions fromamassandchargepointofview.Thetechniquesare classifiedaccordingtoincreasingenergyofreagentsorincidentparticlesorwaves. Thecombinationofallexcitationorreagentadditionandproductdetectionsmakes theanalyticpotentialveryrichtoperformtheidentificationofmolecules,elements or isotopes, their quantitative determination, and their spatial speciation. There has been an optimization of techniques and the discovery of new ana- lytical tools over the last century. Some of the techniques are found today to be obsolete, others re-emerge due to new interests; some may be completed by combiningthepotentialofonetechniquewithanother.Inaddition,therehasbeena constant challenge in pushing the use of the analytical techniques toward lower detectionlimits,betterlateralanddepthresolutions,moreextremeapplicationsand more flexible uses. Asfarasthenuclearmaterialsareconcerned,studiesmustreflectthedemanding conditions of temperature, pressure and irradiation under which they are used. These materials act as barriers and their properties are investigated with emphasis on mechanical performances, durability, plasticity and stability when damaged or loadedbydopantsorcontaminants.Thesematerialsrangefromfuelsforthermalor fastreactors,tostructuralmaterials.Fuelsareanalyzedpriortoandafterirradiation, after their reprocessing for recycling and later as waste forms. Macro-properties such as thermodynamic, thermophysical and mechanical as wellas microstructural analysis of these materials have to be analyzed, for example comparing again properties prior to and after irradiation. Preface ix As far as the environments of nuclear materials are concerned, one has to think about the way the analyst and the environmental scientist would collaborate together to produce data that can be used by modelers or by authorities. The challenge is to understand the behavior of actinide elements, fission products and other contaminants in the environment. Biogeochemical pathways have to be described, quantified and understood. Transport of actinides, fission products and other contaminants in fluids such as air or water include particulate or colloidal phases. These analyses must be integrated in the analytical strategy as specific species for modeling their biogeochemical behavior. Data are provided by the analysts for the scientists and the modelers. The problem is to understand the behavior of radionuclides in the systems or the material properties with regard to its integrity. In the environment, contaminant pathways have to be described. The contaminated systems interact with the local environment that may modify radionuclide speciation by physical-chemical pro- cesses. The analytical results must be integrated in the study for modeling their chemical and physical properties. Achallengeforfutureinvestigationswillbetofindanddevelopdirectanalytical probes for full nuclear material characterization at very low defect, dopant or contaminantconcentrationstobettercharacterizethedamages,speciesorstructures and to predict their behavior in homogeneous, heterogeneous or complex nuclear materials and in their environments. Aargau, Switzerland Claude André Degueldre Acknowledgements The author would like to acknowledge several scientists who participated in dis- cussions, providing material or notes. Specifically thanks are due to – F. Aiouache, Lancaster University, UK – R. Bellin, CEA Cadarache, France – S. Caruso, Nagra, Switzerland – M. Döbeli, ETHZ, Switzerland – J. Griffin, Chemistry Department, Lancaster, UK – M. Hertrich, Nagra, Switzerland – M. Joyce, Lancaster University, UK – A. Kerridge, Lancaster University, UK – K. Patel, University of Cambridge, UK – D. Shuh, BNL, USA – S. Stefanovsky, All Bochvar Institut, Moscow, Russia. – N. Toulhoat, CNRS/IN2P3, IPNL, France – M. Tylka, ANL, USA – E. Vance, ANSTO, Australia – M. Veleva, PSI, Switzerland The work has been the fruit of analytical practice over the last 45 years, mainly in Algeria, Belgium, France, Germany, Japan, Switzerland, the UK and USA. The work was however self-financed and its elaboration required intensive personal work.Thedatareportedinthistextbookarenotspecificallythedataoftheauthorof this work. They are taken from the open literature, and their use requires citation. The author of this work is consequently not responsible for their quality. His liability is restricted to the novel form of presentation of the analyses of nuclear materials and their environment. xi
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