Simultaneous Separation and Determination of $^{l4}C\;and\;^3H$ in Spent Resins from PWR Nuclear Power Plants

가압경수로형 원전에서 발생된 폐수지의 $^{14}C$ 및 $^3H$ 동시 분리 및 측정

In this work $^{14}C\;and\;^3H$ distribution characteristics of spent resins from nuclear power plants(NPPs), pressurized water reactors(PWRs), was investigated. It was found that the recovery percent of $^{14}C$ by the wet oxidation-acid stripping was $81%{\sim}100%$ for the added activity range of $^{14}C,\;0.72\;Bq{\sim}460\;Bq$, and it was not affected by the kinds of stripping acids, 3N-HCl, $3\;N-HNO_3\;and\;3\;N-H_2SO_4$. And the recovery percent of $^3H$ by distillation using the same apparatus was $81%{\sim}101%$ for the added activity range of $^3H,\;0.60\;Bq{\sim}435\;Bq$. Among the tested stripping acids, 3\;N-HCl, $3\;N-HNO_3\;and\;3\;N-H_2SO_4$, only the trapped $^3H$ solution by distillation in $3\;N-H_2SO_4$ was compatible with the 3H scintillator, Ultimagold XR. Neither of the $^{14}C\;and\;^3H$ trapping solutions from the spent ion exchange resin samples by the wet oxidation-3 $N-H_2SO_4$ stripping contained gamma nuclides. However, some gamma nuclides, $^{60}Co,\;^{134}Cs,\;^{137}Cs\;and\;^{54}Mn$, were found in the trapped $^3H$ solutions of the spent resins by the wet oxidation-3 N-HCl stripping. It was the same for the $^3H$ trapping solutions of the spent resins by Sample Oxidizer(PACKARD MODEL 307). Meanwhile only two nuclides, $^{134}Cs,\;and\;^{134}Cs$, were found in the $^{14}C$ trapping solutions of the spent resins by Sample Oxidizer(PACKARD MODEL 307). It was found that most of the $^{14}C$ in the spent resins existed as inorganic carbon form, more than about 70% of the total $^{14}C$ content. Among the analyzed 30 spent ion exchange resin samples, the average concentration of $^{14}C$ and $^3C$ for the high radioactive samples, 8 samples, was $19000\;Bq/g{\pm}41000\;Bq/g,\;670\;Bq/g{\pm}460\;Bq/g$ and that for the low radioactive samples, 22 samples, was $4.2\;Bq/g{\pm}4.3\;Bq/g,\;6.0\;Bq/g{\pm}5.3\;Bq/g$, respectively. And the average $^{14}C/^3H$ ratio for the high radioactive samples, was higher, 28, than that of low radioactive samples, 0.70. Some linear relationship trend was found between the activity concentrations of $^{14}C\;and\;^3H$.

가압경수로형 원자력발전소의 운영과정에서 발생된 폐수지내 $^{14}C$ 및 $^3H$의 분포특성을 조사하였다. $Na_2^{14}CO_3$ 표준용액을 사용한 $^{14}C$의 회수율 측정결과, 사용한 산의 종류에 관계없이, 3 N-HCl $3\;N-HNO_3,\;3\;N-H_2SO_4$, 주입한 $^{14}C$ 농도 $0.72\;Bq{\sim}460\;Bq$ 범위에서 $81%{\sim}100%$의 회수율을 나타내었다. 같은 장치를 사용하여 HTO 표준용액 증류에 의한 $^3H$의 회수율은 주입한 $^3H$ 농도 $0.60\;Bq{\sim}435\;Bq$ 범위에서 $81%{\sim}101%$ 이었다. 습식산화-산용출법에 의한 폐수지의 $^{14}C$ 및 $^3H$ 동시분리시, $3\;N-H_2SO_4$를 사용했을 때 다른 감마핵종에 의한 방해가 없었으며, $^3H$ 포집액이 섬광제와 잘 혼합되었다. 그러나 3 N-HCl을 사용했을 때 $^3H$ 포집용액에서 $^{60}Co,\;^{134}Cs,\;^{137}Cs$ 및 $^{54}Mn$ 등의 감마핵종이 검출되었다. 또한 Sample Oxidizer에 의한 $^3H$ 포집용액에서도 $^{60}Co,\;^{134}Cs,\;^{137}Cs$ 및 $^{54}Mn$ 등이 검출되었으며, $^{14}C$ 포집용액에서는 $^{134}Cs,\;^{137}Cs$이 검출되었다. 폐수지의 총 $^{14}C$ 함량중 약 70% 이상이 무기 탄소로 확인되었다. 30개 폐수지 시료중 8개 고방사능 폐수지의 $^{14}C$ 및 $^3H$의 평균농도는 각각 $19000\;Bq/g{\pm}41000\;Bq/g,\;670\;Bq/g{\pm}460\;Bq/g$이었으며 22개 저방사능폐수지에서는 각각 $4.2\;Bq/g{\pm}4.3\;Bq/g,\;6.0\;Bq/g{\pm}5.3\;Bq/g$이 검출되었다. 고방사능 폐수지의 평균 $^{14}C/^3H$비는 28로 저방사능 폐수지의 0.70에 비해 높게 나타났으며, $^{14}C$ 및 $^3H$의 농도는 서로 비례하는 경향을 보였다.