由於多孔介質中的異質性、耦合的輸運機制和多種化學反應過程，導致處置庫中的放射性核素行為非常複雜。放射性物種的行為評估需要對於擴散機理和回填材料的特性進行研究，以防止其洩漏到生物圈中。因此，緩衝材料（如膨潤土）對於吸收放射性核素洩漏和阻止從放射性廢物罐的遷移至關重要。長期以來，人們已經認識到非吸附示踪劑（氚）和反應性示踪劑（銫）在多孔介質中的傳輸行為差異，但尚未完全了解，因此阻礙了對緩衝物質能力的有效評估。本文致力於通過實驗室實驗和作用機理的研究來探索和解釋非吸附性和反應性示踪劑在傳輸行為上的差異。本研究提出一新穎方法（PIPIAM）透過迭代計算並結合解析解方法的新穎參數識別過程，以利用濃度數據獲得膨潤土的目標參數。通過濃度誤差分析比較了PIPIAM和圖形方法的結果。結果表明，在降低濃度誤差方面，PIPIAM優於圖形法。根據實驗觀察和反算結果，本研究提出了與尺度相依的輸運參數，包括幾何因子，擴散係數，延遲因子和分佈係數。根據結果顯示，對於相同厚度的膨潤土樣品，銫的視擴散和有效擴散係數均低於氚，這些差異可以歸因於粘電效應、原子性質和化學反應。在不同厚度的膨潤土樣品的情況下，視擴散和有效擴散係數顯示隨著膨潤土厚度的增加而增加的趨勢，而幾何因子顯示出減少的趨勢。根據實驗數據和反演結果，擴散係數和幾何因子與膨潤土的厚度具有高度相關。因此，提出了對輸運參數的尺度效應來解釋結果，這歸因於膨潤土樣品中孔隙空間的不均勻分佈。示踪劑的尺度效應行為通過回歸分析進行定量。結果可用於改進放射性核素的緩衝液設計。本文有助於闡明與膨潤土中放射性核素行為有關的運輸機制，並為獲取用於核廢料庫安全性評估的運輸參數提供了另一種方法。結果可用於改進放射性核素的緩衝液設計。

Radionuclide behavior in disposal repositories is complex because of the spatial heterogeneity of porous media, coupled flow-transport mechanisms, and multiple chemical reaction processes. The assessment of radioactive species behavior requires research on diffusion mechanism and backfill material characteristic, with the aim to protect the leakage of nuclide to biosphere. Thence, buffer materials such as bentonite are vital for absorbing radionuclide leakage and retarding migration from radioactive waste canisters. Discrepancies in the diffusion behavior of a non-sorbing tracer (HTO) and a reactive tracer (137Cs) in porous media have long been recognized but are not yet fully understood, which hinders effective assessment of the capabilities of buffer materials. This dissertation was dedicated to exploring and explaining the discrepancies in the transport behavior of non-sorbing and reactive tracers through laboratory experiments and an investigation of contributing mechanisms. A novel parameter identification process based on an iterative and analytical method (PIPIAM) is proposed here to obtain the target parameters of bentonite using concentration data. The results of PIPIAM and the graphical method are compared through an error analysis of concentration. The results show that PIPIAM outperforms the graphical method in terms of the error reduction of the concentration. According to the experimental observations and inverse results, for a bentonite sample of the same thickness,137Cs has smaller apparent and less effective diffusion coefficients than those for HTO. These discrepancies can be attributed to the viscoelectric effects, atomic properties, and chemical reactions. In the case of bentonite samples with different thicknesses, the apparent and effective diffusion coefficients show an increasing trend with bentonite thickness, and the geometrical factor shows a decreasing trend. According to the experimental data and inverse results, the diffusion coefficients and geometrical factor are highly related to bentonite thickness. Thus, scale effects on transport parameters were proposed to explain the results, which were attributed to the nonuniform distribution of the pore space in the bentonite sample. The scale effect behavior of tracers was quantified through a regression analysis. The results can be used to improve buffer designs for radionuclides. This study is contributing to clarify the transport mechanisms related to radionuclide behavior in bentonite and the provides alternative method for acquiring transport parameters for the use in safety assessments of nuclear waste repositories. The results can be used to improve buffer designs for radionuclides.

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