Nuclear Energy and the Environment In Nuclear Energy and the Environment; Wai, C., et al.; ACS Symposium Series; American Chemical Society: Washington, DC, 2010. In Nuclear Energy and the Environment; Wai, C., et al.; ACS Symposium Series; American Chemical Society: Washington, DC, 2010. 1046 ACS SYMPOSIUM SERIES Nuclear Energy and the Environment Chien M. Wai, Editor Department of Chemistry University of Idaho Bruce J. Mincher, Editor Aqueous Separations and Radiochemistry Department Idaho National Laboratory Sponsored by the ACS Division of Nuclear Chemistry and Technology and ACS DivisionofIndustrialandEngineeringChemistry AmericanChemicalSociety,Washington,DC In Nuclear Energy and the Environment; Wai, C., et al.; ACS Symposium Series; American Chemical Society: Washington, DC, 2010. LibraryofCongressCataloging-in-PublicationData Nuclearenergyandtheenvironment/[editedby]ChienM.Wai,BruceJ.Mincher; sponsoredbytheACSDivisionofNuclearChemistryandTechnologyandtheACSDivision ofIndustrialandEngineeringChemistry. p.cm.-- (ACSsymposiumseries;1046) Includesbibliographicalreferencesandindex. ISBN978-0-8412-2585-5(alk.paper) 1. Radioactivewastedisposal--Management--Congresses.2. Radioactivewaste repositories--Congresses3. Nuclearfuels--Environmentalaspects--Congresses. I.Wai,ChienM.II.Mincher,BruceJ.III.AmericanChemicalSociety.NuclearChemistry andTechnology.IV.AmericanChemicalSociety.DivisionofIndustrialandEngineering Chemistry. TD812.N832010 621.48’38--dc22 2010036461 ThepaperusedinthispublicationmeetstheminimumrequirementsofAmericanNational Standard for Information Sciences—Permanence of Paper for Printed Library Materials, ANSIZ39.48n1984. Copyright©2010AmericanChemicalSociety DistributedbyOxfordUniversityPress AllRightsReserved. ReprographiccopyingbeyondthatpermittedbySections107or108 oftheU.S.CopyrightActisallowedforinternaluseonly,providedthataper-chapterfeeof $40.25plus$0.75perpageispaidtotheCopyrightClearanceCenter,Inc.,222Rosewood Drive,Danvers,MA01923,USA.Republicationorreproductionforsaleofpagesinthis bookispermittedonlyunderlicensefromACS.Directtheseandotherpermissionrequests toACSCopyrightOffice,PublicationsDivision,115516thStreet,N.W.,Washington,DC 20036. Thecitationoftradenamesand/ornamesofmanufacturersinthispublicationisnottobe construedasanendorsementorasapprovalbyACSofthecommercialproductsorservices referenced herein; nor should the mere reference herein to any drawing, specification, chemicalprocess, orotherdataberegardedasalicenseorasaconveyanceofanyright or permission to the holder, reader, or any other person or corporation, to manufacture, reproduce,use,orsellanypatentedinventionorcopyrightedworkthatmayinanywaybe relatedthereto. Registerednames,trademarks,etc.,usedinthispublication,evenwithout specificindicationthereof,arenottobeconsideredunprotectedbylaw. PRINTEDINTHEUNITEDSTATESOFAMERICA In Nuclear Energy and the Environment; Wai, C., et al.; ACS Symposium Series; American Chemical Society: Washington, DC, 2010. Foreword The ACS Symposium Series was first published in 1974 to provide a mechanism for publishing symposia quickly in book form. The purpose of the series is to publish timely, comprehensive books developed from the ACS sponsoredsymposiabasedoncurrentscientificresearch. Occasionally,booksare developed from symposia sponsored by other organizations when the topic is of keeninteresttothechemistryaudience. Beforeagreeingtopublishabook,theproposedtableofcontentsisreviewed forappropriateandcomprehensivecoverageandforinteresttotheaudience. Some papersmaybeexcludedtobetterfocusthebook;othersmaybeaddedtoprovide comprehensiveness. When appropriate, overview or introductory chapters are added. Draftsofchaptersarepeer-reviewedpriortofinalacceptanceorrejection, andmanuscriptsarepreparedincamera-readyformat. As a rule, only original research papers and original review papers are included in the volumes. Verbatim reproductions of previous published papers arenotaccepted. ACSBooksDepartment In Nuclear Energy and the Environment; Wai, C., et al.; ACS Symposium Series; American Chemical Society: Washington, DC, 2010. Table of Contents Preface Chien M. Wai and Bruce J. Mincher xi Acknowledgement xiii Introduction 1 1 The Nuclear Renaissance: Producing Environmentally Sustainable Nuclear Power Bruce J. Mincher 3-10 Overview 11 2 Separations Research for Advanced Nuclear Fuel Cycles T. A. Todd 13-18 3 Challenges for Actinide Separations in Advanced Nuclear Fuel Cycles K. L. Nash and J. C. Braley 19-38 4 Roadmapping New Cleanup Technologies in the U.S. Department of Energy’s Office of Environmental Management John R. Wiley and Edwin Przybylowicz 39-50 Separations Chemistry 51 5 Green Separation Techniques for Nuclear Waste Management Chien M. Wai 53-63 6 Development of a Unique Process for Recovery of Uranium from Incinerator Ash Sydney S. Koegler 65-78 7 Supercritical Fluid Extraction of Mixed Wastes: PAH, PCB, Uranium and Lanthanum in Solid Matrices Joanna S. Wang, WenYen Chang, HuaKwang Yak, and KongHwa Chiu 79-87 8 Actinide(III) Recovery from High Active Waste Solutions Using Innovative Partitioning Processes Giuseppe Modolo 89-105 9 Combining Octyl(phenyl)-N,N-diisobutyl-carbamoylmethylphosphine Oxide and Bis-(2-ethylhexyl)phosphoric Acid Extractants for Recovering Transuranic Elements from Irradiated Nuclear Fuel Gregg J. Lumetta, Jennifer C. Carter, Artem V. Gelis, and George F. Vandegrift 107-118 10 Development of a Novel GANEX Process Emma Aneheim, Christian Ekberg, Anna Fermvik, and Mark R. S. Foreman 119-130 11 Extraction Chromatographic Separation of Trivalent Minor Actinides Using iHex-BTP/SiO2-P Resin N. Surugaya, Y. Sano, M. Yamamoto, A. Kurosawa, and T. Hiyama 131-139 12 Recent Advances in the Development of the Hybrid Sulfur Process for Hydrogen Production H. R. Colon-Mercado, M. C. Elvington, J. L. Steimke, T. J. Steeper, D. T. Herman, M. B. Gorensek, W. A. Summers, and D. T. Hobbs 141-154 13 Green Process for Uranium Separations Utilizing Molybdenum Trioxide Mohamed Chehbouni, Hamed Al-Busaidi, and Allen W. Apblett 155-167 14 Alpha Spectrometry of Thick Samples for Environmental and Bioassay Monitoring T. M. Semkow, A. J. Khan, D. K. Haines, A. Bari, G. Sibbens, S. Pommé, S. E. Beach, I. AlMahamid, and G. L. Beach 169-177 Radiation Chemistry 179 15 An Overview of Selected Radiation Chemical Reactions Affecting Fuel Cycle Solvent Extraction Bruce J. Mincher 181-192 16 Aqueous Nitric Acid Radiation Effects on Solvent Extraction Process Chemistry Stephen P. Mezyk, Thomas D. Cullen, Gracy Elias, and Bruce J. Mincher 193-203 17 Nitration Mechanisms of Anisole during Gamma Irradiation of Aqueous Nitrite and Nitrate Solutions Gracy Elias, Bruce J. Mincher, Stephen P. Mezyk, Thomas D. Cullen, and Leigh R. Martin 205-214 18 Radiolytic Degradation of Heterocyclic Nitrogen Containing Ligands from Low Dose-Rate Gamma Sources Anna Fermvik, Mikael Nilsson, and Christian Ekberg 215-229 19 Kinetics and Efficiencies of Radiolytic Degradation in Lanthanide/Actinide Separation Ligands - NOPOPO Katy L. Swancutt, Stephen P. Mezyk, Leigh R. Martin, Richard D. Tillotson, Sylvie Pailloux, Manab Chakravarty, and Robert T. Paine 231-242 20 Effects of Aqueous Phase Radiolysis on Lactic Acid Under TALSPEAK Conditions Leigh R. Martin, Bruce J. Mincher, Stephen P. Mezyk, Gracy Elias, and Richard D. Tillotson 243-253 21 DIAMEX Solvent Behavior under Continuous Degradation and Regeneration Operations B. Camès, I. Bisel, P. Baron, C. Hill, D. Rudloff, and B. Saucerotte 255-269 22 Steady-State Radiolysis: Effects of Dissolved Additives J. C. Wren 271-295 Repository Chemistry 297 23 Bridging the Gap in the Chemical Thermodynamic Database for Nuclear Waste Repository: Studies of the Effect of Temperature on Actinide Complexation Linfeng Rao, Guoxin Tian, Yuanxian Xia, Judah I. Friese, PierLuigi Zanonato, and Plinio Di Bernardo 299-318 24 Evaluation of THOR™ Mineralized Waste Forms (Granular and Monolith) for the DOE Advanced Remediation Technologies (ART) Phase 2 Project C. L. Crawford and C. M Jantzen 319-331 25 Effects of Organic Acids on Biotransformation of Acinides Toshihiko Ohnuki, Naofumi Kozai, Takuo Ozaki, Fuminori Sakamoto, Yoshinori Suzuki, and Takahiro Yoshida 333-348 26 The Role of Dissolved Hydrogen on the Corrosion/Dissolution of Spent Nuclear Fuel M. E. Broczkowski, D. Zagidulin, and D. W. Shoesmith 349-380 27 Integrated Repository Science for the Long-Term Prediction of Nuclear Waste Disposal Patricia Paviet-Hartmann and Thomas Hartmann 381-404 Indexes 405 Author Index 407 Subject Index 409-414 Preface A renewed global interest in nuclear power is underway due to concerns about the contribution of combustion of fossil fuels to climate change and the unreliability of the supplyoffossilfuels.Nuclearpoweriscurrentlyanimportantsourceofcarbon-free,safe, anddomesticenergyinmanycountries. However,concernsaboutnuclearwastedisposal and the proliferation of nuclear weapons have hindered its expanded use and continued development. Asworlddemandforenergycontinuestorise,itisrecognizedthatnuclear energy will be required to meet this demand in an environmentally sustainable manner. Responsible management of nuclear wastes, more efficient processes for conversion of uraniumtoenergy,andeffectiveandsecuretechniquesforrecyclingusednuclearfuelare someofthekeyissueswhichmustbeaddressedinordertodevelopsustainablenuclear energytechnologiesforthe21stcentury. Thisbookisbasedonthepaperspresentedatarecentandverysuccessfulsymposium entitled Nuclear Energy and the Environment held at the 238th American Chemical Society (ACS) National Meeting in Washington, DC, August 16-20, 2009. The 3-day ACS symposium was well attended with participants from Canada, France, Germany, Japan,Sweden,Taiwan,andtheUSAdiscussingresearchideasandprogressinseparation of actinides and fission products, green separation techniques, radiation effects, and repositorychemistry.Thisbookstartswithanoverviewofchallengesinactinideseparation chemistryforadvancednuclearfuelcyclesandroadmapsofnewcleanuptechnologiesby theU.S.DepartmentofEnergy. Itisfollowedby3sectionscoveringrecentresearchand developmentinseparationschemistry,radiationchemistry,andrepositorychemistry. The book documents reasons to be optimistic for the future of nuclear power and challenges facingnuclearscientistsandengineerstoday. WeacknowledgesupportfromtheACSNuclearChemistryandTechnologyDivision andtheSeparationScienceandTechnologySubdivisionoftheACSDivisionofIndustrial andEngineeringChemistryforthesymposium. TheACSBooksDepartmentisthanked fortheirencouragementandsupportinthepublicationofthebook. Finally,wethankthe authorsfortheircontributionsandthereviewersfortheirtimeandvaluablecomments. ChienM.Wai DepartmentofChemistry UniversityofIdaho,Moscow,Idaho83844 BruceJ.Mincher AqueousSeparationsandRadiochemistryDepartment IdahoNationalLaboratory,IdahoFalls,Idaho83415 xi In Nuclear Energy and the Environment; Wai, C., et al.; ACS Symposium Series; American Chemical Society: Washington, DC, 2010. Acknowledgement Theeditorsthankthefollowingassociateeditorsfortheirhelpinorganizing thesymposium,editingmanuscripts,andgreatlyimprovingthequalityofthefinal symposiumseriesbook: LinfengRao,DeanR.Peterman,SydneyS.Koegler,and MarshaJ.Lambregts. xiii In Nuclear Energy and the Environment; Wai, C., et al.; ACS Symposium Series; American Chemical Society: Washington, DC, 2010.