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Development of Monitoring Technology for Environmental Radioactivity

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Development of Monitoring Technology for Environmental Radioactivity KAERI/RR-2037/99 KR0000197 Development of Environmental Radiation Protection Technology Development of Monitoring Technology for Environmental Radioactivity 31/40 Please be aware that all of the Missing Pages in this document were originally blank pages KAERI/RR-2037/99 2=1 # a Development of Environmental Radiation Protection Technology Development of Monitoring Technology for Environmental Radioactivity 2000^ : 0| o| I. II- EML ^-A>^ B \f $14. III. o) 4^0. 9Sr Tc-99 )14^H Tc-991- Tc-95m ^^^>* if?!: 7l^^ TBP TBP ^-^^i TEVA ?l^-^ 7] (Quantulus 1220)-!: 44^ *1^^ Pu-241 ^1-Jl £^7l^ 6}-g-«l-^ ^^^ PSA ^^1 Pu-241 a^^l^^: ^1-g-^^ FOM (figure of-merit)7> Pu-241 31# ^fl^l- S^^>^4. FOM° (Ultima gold-AB) ^4^ ^^^^4. S^ ^ 2]^^-€ Pu-241 ^^£ Pu-241 5H ^^^ PERALS® -g-nfl PERALS® PSA 7]^^; 7>*1 ^^]^^-7)]^7l(Quantulus 1220™, Wallac Rn-222 ^ Ra Rn-222 2. on-line «H3-3|i£ £^7l#-ir 7fl#§|-7] $«H ion chromatography£f <SH^% U-A>^^#7|1- ^l-g-^ «j-A}^ ^1#7]1- 7fl^Sl-^4. ion chromatographyS £|M 4^ 14^4^ ^^ #4^ 3. : 7fl#§V7| ^§1] Pu-242 ^«fi^ pH U-232, Th-229 ^ Am-243 Talvitie IV. (Sr-Spec)i 92 % oR1"^ fe^ ^t^: ^.$1^ £lfe Ba, Ca, Y 4. 111 7} %$\ £#*l|3. DC18C6 0.1 Mi tflsfl DNNS 25 mM ^£7} JL 6I *H 90 %°]$£\ ^S^-f- 4i^ > 1 : 5 - 1 ^^4J^A], ^ aflui*l<g<3 (20 - 500 keV) ^A^ ^S 90 % °1&JL 90Y^ 34.2 %, ne)jL 89Sr^r 50.6 % ^1-1^1^^(500 - 1400 keV)iAi^ 7fl#^^^: ^Sr0] 1.7 %, 90Y7} 49.7 %, nelJL 89Sr^l 44.9 % 3£t- .^-^4. Al^^ 600 mL, 93 % ^ S)-^- ^r^ ^ 90 ^- ^1# A] LLD &•& 1.5 dpm/L ^£$14. Spectrum unfolding yov^i ^^> ^^l#^i^fe 60£ ^#A] 90Sr4 89Sr^ LLD & .£. zi-zi- 37.4 mBq/L ^ 32.2 mBq/L ^ 980 TC-95ITH ^tfl5. fl^v£l^4. Tc-95m i^^^:^ 0.5 M K2CO3 ^-f^l 47.7 %, ^^l^i^- 46.3 %, ^ff-^r£] ^-fi 37.2 %^ ^ 4. ^^lS^H 2 M NaOH -§-<^^ ^^#t?r -§-^^ tfl*]-^ TEVA Spec €^ A>-g-t!: ^-f 7l^^l TBP ^#^HH ^7ls|x] ®<&Q Ru ^-f 12.9 13.2 ^^l ^^ PSA ^fe 100^. 4. PSA 100*fHfe ^:47> wflB}-^ ^"^ •y^l^ ^-#4 2.8 %&4. -B-7l^^-^|^4^7> 19 ^l 0.0087 Bq/Al^o]^ pu-239,240i Ai^ 0.0009 Bq/Al£^ ^Afsl^cf. Pu-241 ^£ ^ Pu-241/Pu-239,240 IV Rn-222 PSA %• £ PSA ^ lOO^H 244 ± 4 %, Po-214 ^- 73 ± 2 % fe PSA ^ 100 tfl«l| 200 tfl-gfl 0.14 Bq/L Sl^.^, Po-214 0.06 Bq/LS ^4 ^^8: MDA $4: *r 5 ~ 20 ^€ Rn-222 82 ± 5% 1 PERALS' * L 7 ^r°l 98 ± 1 % 0.7 40% (^§1, NO3", URAEX™ 1.5 mL 100 mL $14. PERALS®!- - 6.5 ^: PERALS 2. on-line ^#-§- ion chromatography^ -^-5. IonPac Csl2A 4 IJi €^ CG12A ^ ^#-§- ^^^ ^S]^]-^JI -g-el^o.^^ MSA (Methanesulfonic acid)* 4 10 ^$\ ^°]£%°) % LAAPD (Large Area Avalanche Photodiode) % ^ 20 Bq - 800Bq ?M 3 #3*1 - ^§H ^*l)^^§: 3)#^ 14 detector bias7> +1850 V ^ ^ 0.5 - 2 cpm ^£ # ^ sasa4. 3. 1.5 ng/l(1.5 ppt)^§£^ ^#§>^^1 (Detection limit)* KU/TEVA- Spec , K, Ca, Mg^)* ^]7-l§|-Jl . U ^ L 100 4. *i^RK§: 2^RV, ^^-Aj|7ll- 950 mA, pH £fe 0.3 M ^a^-^^^i0!^ 0.4 M «a\2.^"l4olS. ^ 0.005 M DTPA B^ -g-^^ ^-t^Pu-2421: ^^t ^-f Pu-2427]- ^tfls. -: 98%) sl84. 7]^ fj-^a.4 ^7}si 84. V. VI Cfl database* migration Sr-90, Tc-99, Pu , Rn-222, Ra-226 7> A] qt^ vn SUMMARY I. Project title Development of Monitoring Technology for Environmental Radioactivitv II. Objective and Importance of the Project Purposes and importance of this project are based on the environmental radiation monitoring and assessment during nuclear facilities operation. As the increasing use of nuclear energy in Korea due to insufficient to natural resources, the public's concern about the nuclear facilities is enhanced. The accurate and reliable determination techniques of the radioactive isotopes in environmental samples are very important to protect public health from the potential hazards of radiation. In order to obtain the confidence of general public to nuclear safety by release of the monitoring results, development of environmental monitoring system and reliable analytical technologies for environmental radionuclides should be established. In the framework of monitoring environmental radioactivity, not only for the emission control of normal nuclear operation but for the accidental release of radionuclides, measurements of alpha- and beta-ray emitting nuclide concentrations in all kinds of environmental samples have to be performed. Because almost all of these radionuclides are hard-to-measure, severely time-consuming and labor-intensive, a demand for a rapid and cost effective analytical procedure and measurement techniques is on the increase. A demand for the measurement of radionuclides requiring a reinforced national IX restriction criteria for the environmental radiation activity should be satisfied also. Establishment of analysis of ultra low level radionuclides technology contributes to the security of national acknowledgement in the radiation monitoring capability as well as in the nuclear safety. III. Scope and Contents of the Project Research for the environmental radionuclides analysis was carried out broadly for the following ; 1. Liquid scitillation counting of alpha/beta emitting radionuclide Isolation and purification of radiostrontium from environmental aqueous sample was performed by using strontium selectively binding resin(Sr-Spec) and strontium selectively permeable liquid membrane. Radioactivity of radiostrontium was measured by liquid scintillation counter coupled with dual counting window and spectrum unfolding method. With combustion apparatus a new determination of Tc-99 in the environmental samples was developed for overcoming demerits of conventional TBP extraction method. The optimum conditions of volatilization and trap solution in the combustion apparatus were investigated. Also, for complete removing Ru isotopes, TEVA column was used in the conventional TBP extraction of Tc-99. An optimized method for determining beta-emitting "* Pu in the presence of alpha-emitting nuclides was developed using a liquid scintillation counting system. Pulse shape analysis level was set using pulse-shape discrimination method and the 241Pu counting channel was adjusted for maximum value of figure of merit using the Pu standard source. The volume of scintillant was determined for the maximum value of counting efficiency. This optimized method has been applied to environmental samples to measure concentration of Pu in soils and mosses. A method for measuring Rn-222 and Ra-226 in aqueous sample using liquid scintillation counting technique has studied. The Rn-222 was extracted easily from the water sample (10 mL) by 12 mL of xylene based organic scintillant. After radioactive equilibrium between Rn-222 and its alpha emitting decay products for three hours, the alpha activity from Rn-222 and its decay products were measured in a scintillation vial using the Wallac 1220™ Quantulus liquid scintillation counter. Ra-226 concentration in aqueous sample was determined, after isolation of Ra-226 from the sample matrix, by extraction the ingrowth of the Rn-222 and its alpha emitting decay products with xylene based organic scintillant. The adaptation of extractive scintillation by URAEX * with a photon-electron rejecting alpha liquid scintillation (PERALSB) spectrometer to the analysis of uranium in aqueous samples was described. The extraction efficiency of the system was evaluated under varing chemical conditions including pH, and sample-cocktail volume ratio. Isotopic information from the PERALS* spectrum of natural uranium was obtained using a curve fitting routine. Comparisons of the result with that obtained from alpha spectrometry method using ion implanted silicon detector showed good agreement, 2. Development of on-line measurement of beta-emitting nuclide system On-line measurement system coupled with ion chromatography and portable liquid scintillation detector was developed. Flow-through type liquid scintillation detector was capable of detection of scintillation light from eluent containing radionuclide with very high sensitivity XI 3. Analysis of long half-life radionuclides using ICP-MS One of the long half-life radionuclides, U and Th was measured by inductively coupled plasma mass spectrometry (ICP-MS). The method of flow-injection preconcentration for the analysis of U and Th in seawater was developed. 4. Development of a new electrodeposition method for alpha spectrometry To determine the optimum conditions for plating plutonium, the effects of electrolyte concentration, chelating reagent, current, pH of electrolyte and the time of plating on the electrodeposition were investigated on the base of the ammonium oxalate-ammonium sulfate electrolyte containing diethyl triamino pentaacetic acid. An optimized electrodeposition procedure was applied to environmental samples as well as the radionuclides such as thorium, uranium and americium. IV. Results from the Research and Development The results of environmental radionuclide analysis are as the follows; 1. Liquid scitillation counting of alpha/beta emitting radionuclide Total strontium recovery obtained from Sr-Spec column was more than 92 % and separational procedure was complete within 2 hour. Interfering nuclide such as Ba, Ca, Y, etc, were completely removed from only one separational procedure. Liquid membrane consisting of 0.1 M DC18C6 and 25 mM of DNNS was capable of selectively permeation of strontium from feed solution Xll to strip solution with more than 90% of strontium selectivity. Within the suitable concentration ratio of Sr to Ca, 1:5 - 1: 50, strontium was selectively separated with great stability. Radiostrontium activity by liquid scintillation counting based on the dual counting window method was shown that the counting efficiency was 90 % for 90Sr, 34.2 % for ^Y and 50.6 % for 89Sr respectively. The low limit of detection(LLD) was 1.5 dpm/L.
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