자원환경지질 (Economic and Environmental Geology)

  • 제56권6호
  • /
  • Pages.847-870
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  • 2023
  • /
  • 1225-7281(pISSN)
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  • 2288-7962(eISSN)
대한자원환경지질학회 (The Korean Society of Economic and Environmental Geology)
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한국 심부 지하수 환경에서의 방사성 핵종(우라늄, 플루토늄, 팔라듐)의 지화학적 거동 모델링

Geochemical Modeling on Behaviors of Radionuclides (U, Pu, Pd) in Deep Groundwater Environments of South Korea

  • 최재훈 (고려대학교 지구환경과학과) ;
  • 박선주 ((주)어스이엔지) ;
  • 서현수 (고려대학교 지구환경과학과) ;
  • 안현태 (고려대학교 지구환경과학과) ;
  • 이정환 (한국원자력환경공단) ;
  • 박정훈 ((주)어스이엔지) ;
  • 윤성택 (고려대학교 지구환경과학과)
  • Jaehoon Choi (Department of Earth and Environmental Sciences, Korea University) ;
  • SunJu Park (Earth E&G) ;
  • Hyunsoo Seo (Department of Earth and Environmental Sciences, Korea University) ;
  • Hyun Tai Ahn (Department of Earth and Environmental Sciences, Korea University) ;
  • Jeong-Hwan Lee (Korea Radioactive Waste Agency) ;
  • Junghoon Park (Earth E&G) ;
  • Seong-Taek Yun (Department of Earth and Environmental Sciences, Korea University)
  • 투고 : 2023.12.13
  • 심사 : 2023.12.20
  • 발행 : 2023.12.29
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초록

고준위 방사성폐기물을 심지층에 안전하게 처분하기 위해서는 방사성 핵종의 장기적 지구화학 거동에 대한 정확한 예측이 요구된다. 이와 관련하여 본 연구에서는 국내 심부 지하수를 대표하는 다섯가지 지화학 환경 조건에서 지화학 모델링을 수행하여 일부 방사성 핵종의 지화학 거동을 예측하였다. 다섯가지 국내 심부 지하수의 지화학 환경은 다음과 같다: 고 TDS 염지하수(G1), 산성 pH의 CO2가 풍부한 지하수(G2), 고 pH 알칼리성 지하수(G3), 황산염이 풍부한 지하수(G4), 묽은(담수) 지하수(G5). 3~12의 pH 범위와 ±0.2V의 산화-환원전위(Eh) 조건에서 일부 방사성 핵종(우라늄, 플루토늄, 팔라듐)의 국내 심부 지하수 내에서의 용해도와 화학종(존재형태)을 예측하였다. 모델링 결과, 용존 상태의 우라늄은 주로 U(IV)로서 중성~알칼리성의 넓은 pH 환경에서 높은 용해도를 보였으며, Eh가 -0.2V인 환원 환경에서도 알칼리 pH 조건에서 높은 용해도를 보였다. 이러한 높은 용해도는 주로 Ca-U-CO3 착물의 형성에 의한 것으로 예측되는데, 이 착물의 활동도(activity)는 국내 심부 지하수 중 주요 단층대를 따라 산출되는 G2와 화강암반에 위치하는 G3에서 높다. 한편, 플루토늄(Pu)의 용해도는 pH에 따라 달라지며, 특히 중성~알칼리성 조건에서 가장 낮은 용해도가 나타난다. 주요 화학종은 Pu(IV)와 Pu(III)이며, 이들은 주로 흡착을 통해 제거될 것으로 추정된다. 그러나 콜로이드에 의한 이동을 고려하면, 이온강도가 낮은 심부 지하수인 G3와 G5 유형에서 콜로이드 형성 및 이동 촉진에 따라 이동성이 증가할 것으로 예상된다. 팔라듐(Pd)은 환원 환경에서는 황화물 침전 반응으로 인해 낮은 용해도를 나타내며, 산화 환경에서는 주로 금속(수)산화물에의 흡착을 통해 Pd(OH)3-, PdCl3(OH)2-, PdCl42- 및 Pd(CO3)22-와 같은 음이온 착물이 제거될 것으로 판단된다. 본 연구는 한국의 심부 지하수 환경에서 방사성 핵종의 운명과 이동에 대한 이해를 높이고, 고준위 방사성 폐기물의 안전한 처분을 위한 전략 개발에 기여할 것으로 기대된다.

The safe disposal of high-level radioactive waste requires accurate predictions of the long-term geochemical behavior of radionuclides. To achieve this, the present study was conducted to model geochemical behaviors of uranium (U), plutonium (Pu), and palladium (Pd) under different hydrogeochemical conditions that represent deep groundwater in Korea. Geochemical modeling was performed for five types of South Korean deep groundwater environment: high-TDS saline groundwater (G1), low-pH CO2-rich groundwater (G2), high-pH alkaline groundwater (G3), sulfate-rich groundwater (G4), and dilute (fresh) groundwater (G5). Under the pH and Eh (redox potential) ranges of 3 to 12 and ±0.2 V, respectively, the solubility and speciation of U, Pu, and Pd in deep groundwater were predicted. The result reveals that U(IV) exhibits high solubility within the neutral to alkaline pH range, even in reducing environment with Eh down to -0.2 V. Such high solubility of U is primarily attributed to the formation of Ca-U-CO3 complexes, which is important in both G2 located along fault zones and G3 occurring in granitic bedrocks. On the other hand, the solubility of Pu is found to be highly dependent on pH, with the lowest solubility in neutral to alkaline conditions. The predominant species are Pu(IV) and Pu(III) and their removal is predicted to occur by sorption. Considering the migration by colloids, however, the role of colloid formation and migration are expected to promote the Pu mobility, especially in deep groundwater of G3 and G5 which have low ionic strengths. Palladium (Pd) exhibits the low solubility due to the precipitation as sulfides in reducing conditions. In oxidizing condition, anionic complexes such as Pd(OH)3-, PdCl3(OH)2-, PdCl42-, and Pd(CO3)22- would be removed by sorption onto metal (hydro)oxides. This study will improve the understanding of the fate and transport of radionuclides in deep groundwater conditions of South Korea and therefore contributes to develop strategies for safe high-level radioactive waste disposal.

키워드

과제정보

본 논문은 2022년도 정부(산업통상자원부)의 재원으로 "사용후핵연료관리핵심기술개발사업단" 및 한국에너지기술평가원의 지원을 받아 수행된 연구사업의 결과임(과제번호 2021040101003C; 과제명 "사용후핵연료 처분 부지평가기술 및 안전성 입증체계 구축").

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