J. Samper , C. López-Vázquez , B. Pisani , A. Mon , A.C. Samper-Pilar , F.J. Samper-Pilar
{"title":"Global sensitivity analysis of reactive transport modelling for the geochemical evolution of a high-level radioactive waste repository","authors":"J. Samper , C. López-Vázquez , B. Pisani , A. Mon , A.C. Samper-Pilar , F.J. Samper-Pilar","doi":"10.1016/j.apgeochem.2025.106286","DOIUrl":null,"url":null,"abstract":"<div><div>Reactive transport models are used for the performance assessment of high-level radioactive waste repositories (HLW). Quantifying model uncertainty requires the identification of the parameters having the most significant effect on model outputs and the largest impact on prediction uncertainties. Sophisticated sensitivity analysis methods have been developed for numerical models based on the analysis of model results such as the Morris elementary effects and the High Dimensional Model Reduction (HDMR) method proposed by Sobol. VARS (Variogram Analysis of Response Surfaces) is a variance-based method to analyze the structure of a model output. Here we report the application of VARS and HDMR for evaluating the global sensitivities of the predictions of a reactive transport model of the metallic canister and bentonite buffer of a HLW repository in granitic rock. Global sensitivities are analyzed for pH, redox potential and volume of corrosion products at the canister/bentonite interface at t = 1·10<sup>4</sup>, 2.5·10<sup>4</sup> and 5·10<sup>4</sup> years. The input parameters include: the corrosion rate of the metallic canister (CR), the bentonite porewater diffusion coefficient (D<sub>e</sub>), the groundwater flow through the granitic host rock (Q<sub>gra</sub>), the cation exchange selectivity of Fe (K<sub>Fe</sub>) and the solubility of magnetite (Log K). VARS and HDMR results show that the most influential input parameters for pH are CR, Q<sub>gra</sub> and K<sub>Fe</sub>. The sensitivity indexes of pH for parameters CR and K<sub>Fe</sub> increase with time while that of log K of magnetite decreases. The sensitivity index of D<sub>e</sub>, however, remains constant in time. Similar to pH, the most influential parameters for Eh are CR and Q<sub>gra</sub>. The sensitivity indexes of Eh for CR and log K of magnetite decrease with time while that of Q<sub>gra</sub> increases with time. The main interactions between parameters computed with HDMR indexes for pH and Eh at t = 5·10<sup>4</sup> years occur between CR and Q<sub>gra</sub>. Similar to pH and Eh, CR is the most influential parameter for the volume of corrosion products while D<sub>e</sub> is the second most relevant. All the sensitivity indexes for the volume of corrosion products increase with time except for CR. Parameter rankings of Sobol and VARS are nearly identical.</div></div>","PeriodicalId":8064,"journal":{"name":"Applied Geochemistry","volume":"180 ","pages":"Article 106286"},"PeriodicalIF":3.1000,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Applied Geochemistry","FirstCategoryId":"89","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0883292725000095","RegionNum":3,"RegionCategory":"地球科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"GEOCHEMISTRY & GEOPHYSICS","Score":null,"Total":0}
引用次数: 0
Abstract
Reactive transport models are used for the performance assessment of high-level radioactive waste repositories (HLW). Quantifying model uncertainty requires the identification of the parameters having the most significant effect on model outputs and the largest impact on prediction uncertainties. Sophisticated sensitivity analysis methods have been developed for numerical models based on the analysis of model results such as the Morris elementary effects and the High Dimensional Model Reduction (HDMR) method proposed by Sobol. VARS (Variogram Analysis of Response Surfaces) is a variance-based method to analyze the structure of a model output. Here we report the application of VARS and HDMR for evaluating the global sensitivities of the predictions of a reactive transport model of the metallic canister and bentonite buffer of a HLW repository in granitic rock. Global sensitivities are analyzed for pH, redox potential and volume of corrosion products at the canister/bentonite interface at t = 1·104, 2.5·104 and 5·104 years. The input parameters include: the corrosion rate of the metallic canister (CR), the bentonite porewater diffusion coefficient (De), the groundwater flow through the granitic host rock (Qgra), the cation exchange selectivity of Fe (KFe) and the solubility of magnetite (Log K). VARS and HDMR results show that the most influential input parameters for pH are CR, Qgra and KFe. The sensitivity indexes of pH for parameters CR and KFe increase with time while that of log K of magnetite decreases. The sensitivity index of De, however, remains constant in time. Similar to pH, the most influential parameters for Eh are CR and Qgra. The sensitivity indexes of Eh for CR and log K of magnetite decrease with time while that of Qgra increases with time. The main interactions between parameters computed with HDMR indexes for pH and Eh at t = 5·104 years occur between CR and Qgra. Similar to pH and Eh, CR is the most influential parameter for the volume of corrosion products while De is the second most relevant. All the sensitivity indexes for the volume of corrosion products increase with time except for CR. Parameter rankings of Sobol and VARS are nearly identical.
期刊介绍:
Applied Geochemistry is an international journal devoted to publication of original research papers, rapid research communications and selected review papers in geochemistry and urban geochemistry which have some practical application to an aspect of human endeavour, such as the preservation of the environment, health, waste disposal and the search for resources. Papers on applications of inorganic, organic and isotope geochemistry and geochemical processes are therefore welcome provided they meet the main criterion. Spatial and temporal monitoring case studies are only of interest to our international readership if they present new ideas of broad application.
Topics covered include: (1) Environmental geochemistry (including natural and anthropogenic aspects, and protection and remediation strategies); (2) Hydrogeochemistry (surface and groundwater); (3) Medical (urban) geochemistry; (4) The search for energy resources (in particular unconventional oil and gas or emerging metal resources); (5) Energy exploitation (in particular geothermal energy and CCS); (6) Upgrading of energy and mineral resources where there is a direct geochemical application; and (7) Waste disposal, including nuclear waste disposal.