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Removal of Actinides from Nuclear Fuelreprocessing

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Removal of Actinides from Nuclear Fuelreprocessing 1 - ARH-SA-217 Qt - 96-09/3 - - /3 Removal of Actinides from Nuclear Fuel Reprocessing Waste Solutions with Bidentate Organophosphorus Extractants Wallace W. Schulz Lyle D. McIsaac August 1975 Prepared for the U.S. Energy Research and Development Administration Under Contract E(45-1)-2130 Atlantic Richfield Hanford Company Richland.Washington 99352 ARA *ASTER /, DISTRICI. 3-10:'1 OF ; Der:1.11·1Et,iT IS I.INLIMITED- DISCLAIMER This report was prepared as an account of work sponsored by an agency of the United States Government. Neither the United States Government nor any agency Thereof, nor any of their employees, makes any warranty, express or implied, or assumes any legal liability or responsibility for the accuracy, completeness, or usefulness of any information, apparatus, product, or process disclosed, or represents that its use would not infringe privately owned rights. Reference herein to any specific commercial product, process, or service by trade name, trademark, manufacturer, or otherwise does not necessarily constitute or imply its endorsement, recommendation, or favoring by the United States Government or any agency thereof. The views and opinions of authors expressed herein do not necessarily state or reflect those of the United States Government or any agency thereof. DISCLAIMER Portions of this document may be illegible in electronic image products. Images are produced from the best available original document. Atlantic Richfield Hanford Company Richland, Washington 99352 A. .' NOTICE THIS REPORT WAS PREPARED AS AN ACCOUNT OF WORK SPONSORED BY THE UNITED STATES GOVERNMENT. NEITHER THE UNITED STATES NOR THE UNITED STATES ENERGY RESEARCH AND DEVELOPMENT ADMINISTRATION, NOR ANY OF THEIR EMPLOYEES, NOR ANYOF THEIR CONTRACTORS, SUBCONTRACTORS, OR THEIR EMPLOYEES, MAKES ANY WARRANTY, EXPRESS OR IMPLIED, OR ASSUMES ANY LEGAL LIABILITY OR RESPONSIBILITY FOR THE ACCURACY, COMPLETENESS, OR USEFULNESS OF ANY IN FORMATION, APPARATUS, PRODUCT OR PROCESS DISCLOSED, OR REPRESENTS THAT ITS USE WOULD NOT INFRINGE PRIVATELY OWNED RIGHTS. (212#K fifs. e 0&61 ED-9300-090.2 (1-75) ARH-SA-217 REMOVAL OF ACTINIDES FROM NUCLEAR FUEL REPROCESSING WASTE SOLUTIONS WITH BIDENTATE ORGANOPHOSPHORUS EXTRACTANTS Wallace W. Schulz NOTICC This report was prepared as an account of work sponsored by the United States Government. Neither • Chemical Technology Laboratory the United States not the United States Eneigy Research and Development Administration, nor any of Research Department their employee, nor any of their contractors. subcontracto/, or their employees, makes any Research and Engineering Division warranty, express or impued, 0, assumes any legal liability or responsibility for the accuracy, completeness . Atlantic Richfield Hanford Company or usefulness of any inforrnation, apparatus, product or process disclosed, or represents that its use would not Richland, Washington infringe privately owned rights. and Lyle D. McIsaac Radiochemistry Section Chemical Research and Engineering Branch Allied Chemical Corporation Idaho Falls, Idaho August 1975 To be presented at the 4th International Transplutonium Element Symposium Baden Baden, West Germany September 13-17, 1975 0 DISTRIBUTION OF. THIS DOCUMENT IS UNLIMITED ii ARH-SA-217 TABLE OF CONTENTS Page iii ABSTRACT . iv LIST OF FIGURES . iv LIST OF TABL,ES . INTRODUCTION . 1 CHARACTERISTICS OF BIDENTATE ORGANOPHOSPHORUS 1 EXTRACTANTS . : . 3 1 3 S Y N T H E S I S. AVAILABILITY AND C O S T. 3 PURIFICATION . , 4 PROPERTIES . 7 Extraction Mechanisms . 7 Equilibrium Distribution Data . 8 12 Solubility in Aqueous Solutions . 14 Radiolytic Behavior . PROPOSED PLANT-SCALE APPLICATIONS OF BIDENTATE EXTRACTANTS . 16 HANFORD PLUTONIUM RECLAMATION FACILITY . 16 IDAHO CHEMICAL PROCESSING PLANT . 21 OTHERS . : . 24 25 SUMMARY AND EVALUATION . 25 ACKNOWLEDGMENTS . : . 26 R E F E R E N C E S. i iii ARH-SA-217 ABSTRACT The neutraZ bidentate organophosphorus reagents DBDECMP (dibutyZ-N,N-diethyZearbamyZmethyZenephosphonate) and its dihezyZ. anaZogue DHDECMP are cand€date eztractants for removaz of actinides from certain acidic waste streams . produced at the U. S..ERDA Sanford and Idaho FaZZs sites. Various chemicaZ and physicat properties ineZuding ava€Za- b€Zity, cost, purification, aZpha radiotybis, and aqueous phase solubility of DBDECMP and DHDECMP are reviewed. A conceptual flowsheet employing a 15% DBDECMP (or DHDECMP)- CCZ 4 extractant for removat (and recovery) of Am and Pu from Hanford's PZutonium RecZamation Facitity acid waste stream (CAW Botution) was suecessfuZZy demonstrated in Zaboratory- scaZe mixer-settZer tests; this extraction scheme can be .used to produce an actinide-free waste. A 30% DBDECMP-xylene fZoesheet is being tested at the Idaho FaZZs site for removeZ of U, Np, Pu, .and Am from Idaho Chemical Processing Plant first-cyete high-ZeveZ raffinate to produce an actinide-free (<10 nCi atpha activity/gram) waste. iV ARH-SA-217 LIST OF FIGURES FIGURE 1 EXTRACTION OF AMERICIUM BY PURIFIED AND TECHNICAL-GRADE DBDECMP FIGURE 2 EQUILIBRIUM DBDECMP EXTRACTION OF Am(111) AND Pu(IV) FROM HN03 SOLUTIONS FIG.URE 3 DBDECMP PROCESS FLOWSHEET FOR RECOVERY OF AMERICIUM AND PLUTONIUM FROM HANFORD CAW SOLUTION FIGURE 4 CONCEPTUAL PROCESS FLOWSHEET FOR REMOVAL OF ACTINIDES FROM ICPP WASTE SOLUTION LIST OF TABLES TABLE I TYPICAL COMPOSITION.OF HANFORD AND ICPP ACTINIDE WASTES TABLE 11 EXTRACTION OF SELECTED METAL IONS BY DBDECMP. AND DHDECMP SOLVENTS. TABLE 111 SOLUBILITY OF DBDECMP· IN VARIOUS AQUEOUS SOLUTIONS TABLE IV ALPHA RADIOLYSIS OF DHDECMP SOLUTIONS r - ARH-SA-217 REMOVAL OF ACTINIDES FROM NUCLEAR FUEL ' REPROCESSING WASTE SOLUTIONS WITH BIDENTATE ORGANOPHOSPHORUS EXTRACTANTS INTRODUCTION The biological hazards and long half-lives of the actinide elements make them of special importance in proper management of. nuclear waste solutions. Potential advantages and simplifications which might accrue from partitioning these wastes into an actinide and a nonactinide fraction have been cited by several· authors.[1-31 Transuranium- contaminated·solid wastes have been defined[1,4] as those contaminated with greater than 10 nei/gram of certain alpha- emitting radionuclides of lon4 half-life and high specific radiotoxicity. Claiborne[2] has noted the desir'ability of ' reducing the long-term (>1000 y) hazard potential of high- level wastes to about 5% of that for pitchblende mineral on the basis of hazard indices. ' Aqueous waste solutionsgenerated in present-day schemes for reprocessing both irradiated and nonirradiated (e.g., Pu scrap· recovery) nuclear fuels contain relatively high doncentrations of nitric acid. From such solutions common monodentate neutral organophosphorus extractants such as TBP (tri-n-butylphosphate) and DBBP (dibutylbutylphospho- nate)-extract Pu(IV), Np(IV), and U(VI) very well but do not exttact trivalent americium and curium. These monodentate reagents will, however, extract Am3+ and Cm 3+ reasonably well from low-acid, highly salted solutions. [Such feed- stock is employed, as described more fully later, in the Hanford DBBP Am-extraction process.] Solvent extraction processes which use HDEHP [bis(2-ethylhexylphosphoric acid)] 2 ARH-SA-217 as the extractant have been devised both in,the United States [5] and in Germany[6] for recovery of americium and curium from nuclear waste solutions previously adjusted to PH's 21. The great advantages of reagents which could be used for solvent extraction of +3 as well as +4 and +6 actinides from strong HN03 solutions were recognized early on. Siddall in the 1960's synthesized various methylene diph6s- 0 0 " 11 phonites [(RO-) 2P-CH 2-P (-OR) 2], carbamylphosphonates 00 [(RO-)2$-C-N(-R)2]11 and carbamylmethylenephosphonates 00 " 11 [ (RO-) 2P-CH 2-C-N(-R) 2] and investigated their ability to extract. Am 3+, Ce 3+, pm 3+, and HNO) from 0.1 to 12M HNO 3 solutions. His:favorable results[7,81 led Siddall to sug- gest such bidentate extractants could be used to remove trivalent ·actinides and lanthanides from high-level Purex process waste; this idea was eventually patented.[91 Work is currently in progress at both the U. S. Energy - Research and Development Administration (ERDA) Hanford and Idaho Falls sites to extend Siddall's pioneering research with bidentate organophosphorus extractants. Our objective is to :develop and demonstrate practical bidentate extraction precesses for plant-scale removal and recovery of americium, plutonium, and other actinides from certain acidic nuclear wastes generated at these sites. This paper summarizes the current status of our research including accomplishments and unsolved problems. · 1 3 ARH-SA-217 CHARACTERISTICS OF BIDENTATE ORGANOPHOSPHORUS EXTRACTANTS SYNTHESIS Methylenediphosphonates, carbamylphosphonates, and carbamylmethylenephosphonates can all be prepared (in 40-60% yield) most conveniently via the Michaelis reaction as illustrated in Equation 1. 0 .: 0 0 0 11 11 11 11 (n-CdH130)2P-Na+Cl-C-N(C2HS)2 + (n-C6H130)2P-C-N(C2H5)2+NaCl (1) The Arbuzov rearrangement (Equation 2) can also. be used to prepare these classes of bidentate extractants. 011 1111 0 0 (n-CGH130)3P+Cl-C-N(C2HS') 2 + (n-C6Hl 30) 2P-C-N(C2HS) 2+(6Hl 3Cl (2) Siddall[9] notes, however, that especially with larger alkoxy substituents the Arbuzov rearrangement takes place with diethylcarbamyl chloride and N,N-dialkylhalodcetamides 0 [(R)2NLC-CH2X] only at temperatures around 200°C. Visible degradation of product occurs at such temperatures. AVAILABILITY AND COST Gram-quantities of purified (99%) dibutyl-N,N-diethyl- carbamylphosphonate
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