Carbide Fuel Development Final Report Period of May 15, 1959 To
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LEGAL NOTICE This report was prepared as an account of Governmeut sponsored work. Neither the United StAtes, noT the Commission, noT any persoIl act1l:l& on behalf of the Commission: A. Makes anywarraDty or representaUoa.expres$ed or Implied. with respect to the accu racy. completeness, or usefulDess of the lnformadoD contained ID this report. or that the use of any information. apparatus. method. or process dts:closed In this report may 001 iDfTiDge privately owned rtgbtB; or UNC-5134 B. Assumes any UablUties wtth respect to the use of. or for damages resultiDg from the use of any informaUon, apparablS. method. or proeesa disclosed 1D this report. Volume I As used ill the above. "person actfDg on behalf of the CommfasJon" tncladea any em ployee or contractor of the CommlBsion. or employee of such contractor. to the extent that such employee or contractor of the Commission, or employee of such contractor prepares, CFSTI PRICES disseminates, or provides access to. any informadcm pursuant to his employment or contract with the Comm.1ssloD. or his employment with such COntraetor~ , ~.c. $~; M~ 15' CARBIDE FUEL DEVELOPMENT FINAL REPORT' PERIOD OF MAY 15. 1959 TO OCTOBER 15, 1965 A. Strasser D. Stahl RELEA·SEll FOR AN'NCU~~CE!~ENT IN NUCLEAR SCIENCE ABSTRACTS L--------I " October 15, 1965 Work Performed under UNC Project 2320 Contract AT(30-1)-2899 and Project IV, Contract AT(30-1)-2303 with the United States Atomic Energy Commission Prime Contractor UNITED NUCLEAR CORPORATION Research and Engineering Center Elmsford, New York Subcontractor THE CARBORUNDUM COMPANY Niagara Falls, New York ,,-r-'i Work Performed by .United Nuclear Corporation The Carborundum Company N. Chu J. Andersen R. Jaroszeski C. McMurtry G. Sofer K. Taylor D. stahl A. Strasser' O. Sullivan 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. I FOREWORD The Carbide Fuel Development Program was sponsored by the USAEC, Division of Reactor Development. The United Nuclear Corporation performed conceptual design, fuel evaluation, and fuel irradiation. Under its prime contract with the AEC, the United Nuclear Corporation, Development Division, "issued a subcontract to The Carborundum Company for fuel fabrication. The authors wish to thank the many people whose talents and diligent work con • tributed to this program. "~ '"'!' ." ,.. ii • TABLE OF CONTENTS 5.2 Structural Characterization ............ 55 5.2.1 Metallography and Microprobe Analyses of Fuel . 55 5.2.2 Effect of Heat Treatment.. .... 59 5.2.3 Effect of Aging on Lattice Parameters. 63 5.3 (UO.95PuO.5)C Specimen Fabrication for Property Measurements .. 67 5.3.1 Powder Preparation. .. .. .. _. 67 5.3.2 Pellet and Other sample Preparation 67 5.4 Fuel-Clad Compatibility. 71 5.4.1 Introduction ....... 71 5.4.2 Tests with UC ...... 71 5.4.3 Tests with (UO.9SPuO.OS)CO.98 ..•. 80 5.5 Coefficient of Thermal Expansion Measurements. 83 5.6 Melting Point Determinations ..... .. 89 5.7 Thermal stability and Vapor Pressure Measurements. 93 5.7.1 Introduction •..... 93 5.7.2 Experimental Equipment. 93 5.7.3 Experimental Data . 95 5.7.4 Discussion of Results .. 97 5.8 Fuel Reprocessing •...... 103 6. REFERENCES AND BmLIOGRAPHY .. 107 TABLES 2.1 Summl.ry of Analytical study Results 4 3.1 Results of the Heat Transfer study .•. 11 3.2 Reactor Characteristics ...... 16 3.3 Isothermal Core Temperature Coefficients of Reactivity. 21 3.4 Fuel Cost Assumptions for EFFBR . .. .. 23 3.5 Total Fuel Cycle Costs for EFFBR ..•..• 25 4.1 Effect of Binder Percentage on Density of UC. 32 4.2 Effect of Particle Size on Density of UC . 32 4.3 Effect of Time and Temperature of Sintering on Density of UC Pellets. ........ .. .. 33 4.4 Effect of Milling Time on Density of UC .... 33 4.5 Effect of Forming Pressure on Unfired and Final UC • Pellet Density. .... .. .... 33 4.6 Fabrication Procedure and Properties of UC Pellets 35 4.7 Effect of Additions of Small Amounts of Nickel on the .- Sintering of UC .. .. 37 iv 4.8 Summary of Experiments on the Preparation of (UPu)C Solid Solutions from UC + Pu2C3 + U. ..... 40 4.9 The Effect of Carbon Content on the Syntheses of (UPU)C Powders. 42 4.10 Results of Additional Experiments to Produce (UO.8PuO.2)CO.95 by Carbon Reduction of the Oxides.. 43 i 4.11 Results of Synthesis Experiments at 1625°C to Produce (UO.8PuO.2)CO.95 '. .......... '" . 45 4.12 Effect of Nickel Addition on the Sintering of UC and (UPU)C 46 4.13 The Effect of Nickel and Carbon Additions on Sintering of (UO.8PuO.2)CO.95 ..... .. .. ..... 48 4.14 Results of Sintering Experiments with (UO.8PuO.2)2C3 51 5.1 Effect of High Temperature Anneal on (UPu)C + 0.1 Ni Pellets.. 61 5.2 Effect of Vacuum Annealing on (UO.8PuO.2)CO.9!i Pellets Previously Sintered in Helium. •. ..... 64 5.3 Effect of Aging on Lattice Parameter of (UO.9SPuO.OS)CO.98 Powder (Camera Method). .. 68 5.4 Effect of Aging on the Lattice Parameter of (UO.8PuO.2)CO.95 Powder (Diffractometer M~thod) ............ 68 5.5 Results of Sintering Experiments with (UO.95PuO.05)CO.98 Pellets. 70 5.6 Results of Sintering Experiments with (UO.95PuO.O!i)CO.98 Bars. 70 5.7 UC Compatibility Test Results .. 72 5.8 (UPu)C CompatibIlity Test Results ..... 72 5.9 Inconel-X- UC Interaction. ........ 75 5.10 Summary of Carbide Thermal Expansion Coefficients. 84 5.11 Coefficient of Expansion of (UO.95PuO.05)CO.98 . 90 5.12 Coefficient of Expansion of (UO.95PuO.05)CO.98 + 0.1 wlo Ni 90 5.13 (UPu)C Melting Point Data. 91 5.14 Data from Vapor Pressure Runs. .. 96 5.15 Calculated Vapor Pressure Data .. 98 5.16 Analyses of Fuel Materials from the Diffusion Cells 99 FIGURES 4.1 Solid Solution Sesquicarbide (Uo. sPuo.2hc3 52 4.2 Reaction Product from (Uo. SPuO• 2)(OC) Synthesis 53 5.1 UC-0.1% Ni - Sintered at 1525°C, 4 hr ..... 58 5.2 UC-0.1% Ni - Sintered at 1525°C, 4 hr, Reheated at 1850°C, 1 hr in Vacuum ................ 58 5.3 (UO.SPuO.2)CO.95 + 0.1% Ni - Sintered at 1550°C, 1 hr .... 62 y 5.4 (UO.SPuO.2)CO.95 + 0.1% Ni - Sintered at 1550°C, 1 hr. Reheated at 1750°C, 3 hr in Helium •. .. 62 5.5 (Uo. sPuO. 2)Co•95 + 0.1 w/0 Ni - As Sintered in Helium at 1550°C, 1/2 hr. .. .. .. ... 65 5.6 (UO.SPuO.2)CO.95 + p.1 w/o Ni - Sintered in Helium and Vacuum Annealed at 1900°C, 1 hr •........ 65 i 5.7 (UO.SPuO.2)CO.95 + 0.1 w/o Ni - Sintered in Helium and Vacuum Annealed at 2200°C. 1/2 hr. .............. 65 5.8 (UO.SPuO.2)CO.95 - As Sintered in Helium at 1925°C, 1 hr .. 66 5.9 (UO.SPuO.2)CO.95 - Sintered in Helium and Vacuum Annealed at 2200°C, 1/2 hr ...... 66 5.10 Compatibility Capsule •..... 73 5.11 Type 304 SS Tested 1000 hr ..•. 76 5.12 ~% Cr-1 Mo Steel Tested 4000 hr •. 76 5.13 UC Tested 1000 hr in Contact with Inconel-X . 77 5.14 Inconel-X, Tested 4000 hr ......... 77 5.15 Niobium Tested 4000 hr ..... .. 79 5.16 Zircaloy-2-UC Interface Tested 4000 hr at 820°C. 81 5.17 Beryllium-UC Interface Tested 4000 hr at 820°C .•. 81 5.18 Type 316 Stainless Steel from Compatibility Test. 82 5.19 2% Cr-1 Mo Steel from Compatibility Test. .... 85 5.20 Niobium from Compatibility Test. ...... 86 5.21 Niobium-1% Zirconium from Compatibility Test 87 5.22 Zircaloy-2 from Compatibility Test. .. 88 5.23 Schematic of Dilatometer. ..•........ 92 5.24 Schematic of Knudsen Vapor Pressure Apparatus. 94 5.25 Vapor Pressure of U and Pu over (UPU)C at 1995°C . 101 5.26 Log of Vapor Pressure of Pu over (UPU)C at 1995°C. 102 5.27 Vapor Pressure of U and Pu over (UPu)C at 1822°C .. 104 vi • 1. INTRODUCTION The Carbide Fuel Development Program was concerned with the technology of the entire UC-PUC fuel cycle. The major goals of the program were to produce (UPU)C* and to obtain data on its irradiation behavior for long burnups and at high power generation rates. In addition, other areas of the fuel cycle were ex plored to discover possible problems. The program was initiated in May 1959 and was completed in October 1965. Fuel made of a combination of UC and PUC has a potential of reducing the fuel cycle cost of existing fast breeder reactors.