Solubilities and Major Species of Selenium and Technetium in the KURT Groundwater Conditions

The long-lived fission products $^{79}Se$ and $^{99}Tc$ have been considered as the major concern nuclides for the disposal of radioactive waste because of their high solubilities and the existence of anionic species in natural water. In this study, the solubilities of $FeSe_2(s)$ and $TcO_2(s)$, known as respective Solubility Limiting Solid Phase (SLSP) of selenium and technetium, were measured in the KURT (KAERI Underground Research Tunnel) groundwater under various pH and redox conditions. And their solubilities and major species were also calculated using geochemical codes under conditions similar to experimental solutions. Experimental results and calculation for $FeSe_2$ show that the solubility of selenium was found to be below $1{\times}10^{-6}mol/L$ under the condition of pH 8~9.5 and Eh=-0.3~-0.4 V while the dominant species was identified as $HSe^-$. For $TcO_2$, the solubility of technetium was found to be $5{\times}10^{-8}{\sim}1{\times}10^{-9}mol/L$ in the solutions of pH 6~9.5 and Eh<-0.1 V, while the dominant species was $TcO(OH)_2$. However, when the Eh of the solution is -0.35 V, $TcO(OH)_3^-$ and $TcO_4^-$ are calculated as the dominant species at pH 10.5~12 and pH>12, respectively.

KURT 지하수 조건에서 셀레늄과 테크네튬의 용해도 및 주요 화학종

장수명 핵분열생성물인 $^{79}Se$와 $^{99}Tc$는 자연수 중에서 용해도가 클 뿐더러 음이온으로 존재하여 방사성폐기물 처분장에서 주요 관심핵종들로 고려되고 있다. 본 연구에서는 KURT 지하수의 다양한 pH와 산화-환원 조건에서 셀레늄과 테크네튬의 Solubility Limiting Solid Phase (SLSP)로 알려진 $FeSe_2$와 $TcO_2$의 용해도를 측정하였다. 또한, 지화학코드를 이용하여 실험과 유사조건에서 이들의 용해도와 주요 화학종을 계산하였다. 실험 및 계산으로부터 pH 8~9.5와 Eh=-0.3~-0.4 V 조건에서 $FeSe_2$의 용해도는 $1{\times}10^{-6}mol/L$이하이며, 주 용해 화학종은 HSe-로 판단된다. $TcO_2(s)$의 경우는 pH 6~9.5와 Eh<-0.1 V 영역에서 용해도와 주 용해 화학종이 각각 $5{\times}10^{-8}{\sim}1{\times}10^{-9}mol/L$와 $TcO(OH)_2$로 나타났지만, Eh=-0.35 V조건에서는 주 용해화학종이 pH가 10.5~12와 12이상에서 각각 $TcO(OH)_3^-$와 $TcO_4^-$로 계산되었다.