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研究生:李俞鋆
論文名稱:硒銫在花崗岩上地下水中的吸附與擴散行為
論文名稱(外文):Sorption and Diffusion of Se and Cs on Granite
指導教授:許俊男許俊男引用關係
指導教授(外文):Chun-Nan Hsu
學位類別:碩士
校院名稱:國立清華大學
系所名稱:原子科學系
學門:工程學門
學類:核子工程學類
論文種類:學術論文
論文出版年:2004
畢業學年度:92
語文別:中文
論文頁數:76
中文關鍵詞:花崗岩地下水吸附擴散
外文關鍵詞:seleniumcesiumgranitegroundwatersorptiondiffusion
相關次數:
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本研究的主要目的是藉由實驗及模式的建立,探討硒和銫在粉碎花崗岩中的擴散行為。由實驗數據的分析結果顯示,可以有效地模擬出放射性核種的擴散模式。本研究包含了批次實驗和管柱實驗,其中所有採用的液相皆為合成地下水及合成海水。在批次實驗中,包含了好、厭氧批次實驗及動力吸、脫附反應。好、厭氧批次實驗主要是觀察在厭氧環境下,其Kd值與在好氧環境下是否有差異,以作為是否進一步探討厭氧中管柱擴散實驗的依據。結果顯示,花崗岩在厭氧的環境下,吸附Cs的能力比在好氧下好,差異也非常明顯。在動力吸、脫附反應裡,主要是在探討其可能的吸附機制。由實驗發現,Cs在花崗岩中的吸附機制為雙位元模式吸附,而Se在花崗岩中的吸附則為單位元模式吸附。在好氧的管柱擴散實驗裡,發現若粉碎花崗岩管柱的直徑和長度比小於5,則不能用以往的濃度累積法來計算其Da及Rf值,而需利用解析解擬合出最適合的破除曲線來找出視擴散係數,進而求出其遲滯因數。在管柱實驗中,發現離子濃度對於擴散情形影響並不大,無論在海水或在地下水中,所求出來的數據都在同一個數級內,且非常地接近。由實驗數據發現,就以本研究中所進行的三種長度而言,視擴散係數及遲滯因數均未受到長度的影響,即無論長度為2公分、4公分或8公分,所得到的數值都差異不大。
To assess the performance of underground radwaste repository, proper evaluation of the fate and transport of radionuclides needs to be established from experimental observation and analysis. The goal of this study is to investigate the sorption and diffusion behaviors of Cs and Se in crushed granite through batch test and column diffusion test. In these tests, synthetic groundwater (GW) and synthetic seawater (SW) were employed as liquid phase. From batch tests, it is observed that the Kd values of Cs on crushed granite in anaerobic condition were higher than those in aerobic condition regardless of GW or SW. Based on the results obtained from batch kinetic sorption/desorption tests, a 1-site and a 2-site kinetic models have been determined to be capable of appropriately describing Cs and Se sorption/desorption under test conditions, respectively. In the column diffusion tests, exact analytical solutions have been used in lieu of the method suggested by Crank(1975), to find the apparent diffusion coefficient (Da), due to the ratio of diameter to length is smaller than 5. The values of Da and Rf for Cs and Se in crushed granite columns are not significantly affected by ion concentrations and column lengths.
目 錄
中文摘要...............................................................................................................................................i
英文摘要..............................................................................................................................................ii
致謝.....................................................................................................................................................iii
目錄.....................................................................................................................................................iv
表目錄.................................................................................................................................................vi
圖目錄................................................................................................................................................vii
第一章 緒論........................................................................................................................................1
1–1 背景介紹......................................................................................................................1
1–2 研究目的......................................................................................................................4
第二章 理論........................................................................................................................................5
2–1 岩石礦物的吸附模式..................................................................................................5
2–2 岩石礦物的擴散理論..................................................................................................7
第三章 方法......................................................................................................................................12
3–1 好氧厭氧批次實驗....................................................................................................12
3–1–1 化學試藥........................................................................................................12
3–1–2 儀器設備........................................................................................................13
3–1–3 實驗材料........................................................................................................13 3–1–4 好氧批次實驗................................................................................................15
3–1–5 厭氧批次實驗................................................................................................15
3–2 動力吸脫附實驗........................................................................................................16
3–2–1 實驗材料........................................................................................................17
3–2–2 動力吸脫附實驗步驟....................................................................................17
3–3 擴散實驗....................................................................................................................17
3–3–1 實驗材料........................................................................................................18
3–3–2 擴散實驗方法................................................................................................18
第四章 結果與討論..........................................................................................................................24
4–1 好氧批次實驗............................................................................................................24
4–1–1 Cs在好氧環境及厭氧環境下的差異...........................................................24
4–1–2 Se在好氧環境及厭氧環境下的差................................................................27
4–2 動力吸脫附實驗........................................................................................................31
4–3 管柱擴散實驗結果....................................................................................................39
4–3–1 地下水環境......................................................................................................39
4–3–2 海水環境..........................................................................................................49
4–3–3 地下水與海水環境下的比較與結果..............................................................57
4–4 批次與管柱的比較....................................................................................................58
第五章 結論......................................................................................................................................61
參考文獻............................................................................................................................................63
附錄一 Cs在好氧及厭氧下批次實驗原始數據...........................................................................65
附錄二 Se在好氧及厭氧下批次實驗原始數據............................................................................67
附錄三 Cs吸附脫附原始數據.......................................................................................................69
附錄四 Se吸附脫附原始數據........................................................................................................73









表目錄
表3-1 合成地下水及合成海水成分表..........................................................................................14
表3-2 各種岩石的基本特性..........................................................................................................14
表4-1 Cs在好氧環境下的各項實驗數據......................................................................................25
表4-2 Cs在厭氧環境下的各項實驗數據......................................................................................25
表4-3 Se在好氧環境下的各項實驗數據......................................................................................28
表4-4 Se在厭氧環境下的各項實驗數據......................................................................................28
表4-5 Cs批次實驗的吸脫附結果..................................................................................................32
表4-6 Se批次實驗的吸脫附結果..................................................................................................32
表4-7 Cs擬合曲線的參數列表......................................................................................................34
表4-8 Se擬合曲線的參數列表......................................................................................................34
表4-9 各核種在地下水環境中數據總整理..................................................................................46
表4-10 各核種在海水環境中數據總整理....................................................................................54
表4-11 批次實驗與擴散實驗的遲滯因數比較............................................................................60











圖目錄
圖1-1 核種從廢料固化體遷移到人類生活圈的路徑示意圖........................................................2
圖1-2 本論文主要研究目的及方向................................................................................................3
圖2-1 一些重要的吸附機制............................................................................................................6
圖2-2 擴散實驗的累積突破曲線圖..............................................................................................11
圖3-1 擴散管柱 (a)構造圖、(b)裝置圖.........................................................................................19
圖3-2 岩石擴散管柱實驗 (a)裝置圖、(b)取樣示意圖.................................................................20
圖3-3 水飽和示意圖......................................................................................................................22
圖4-1 Cs在好氧及厭氧環境下個參數的比較 (a)Kd值、(b)pH、(c)Eh........................................26
圖4-2 Cs在好氧及厭氧環境下個參數的比較 (a)Kd值、(b)pH、(c)Eh........................................29
圖4-3 Cs在地下水中的吸附實驗及其擬合曲線..........................................................................35
圖4-4 Cs在地下水中的脫附實驗及其擬合曲線..........................................................................35
圖4-5 Cs在海水中的吸附實驗及其擬合曲線..............................................................................36
圖4-6 Cs在海水中的脫附實驗及其擬合曲線..............................................................................36
圖4-7 Se在地下水中的吸附實驗及其擬合曲線..........................................................................37
圖4-8 Se在地下水中的脫附實驗及其擬合曲線..........................................................................37
圖4-9 Se在海水中的吸附實驗及其擬合曲線..............................................................................38
圖4-10 Se在海水中的吸附實驗及其擬合曲線............................................................................38
圖4-11 地下水中Cs的突破曲線...................................................................................................40
圖4-12 地下水中的Cs累積曲線...................................................................................................40
圖4-13 地下水中Se的突破曲線...................................................................................................41
圖4-14 地下水中Se的累積曲線...................................................................................................41
圖4-15 地下水中HTO的突破曲線...............................................................................................42
圖4-16 地下水中HTO的累積曲線...............................................................................................42
圖4-17 利用解析解擬合出的視擴散係數 (a)Cs-GW、(b)Se-GW、(c)HTO-GW.........................47

圖4-18 利用濃度累積法算出來的Da值與突破曲線作圖 (a)Cs-GW、(b)Se-GW、
(c)HTO-GW........................................................................................................................48
圖4-19 海水中Cs的突破曲線.......................................................................................................50
圖4-20 海水中Cs的累積曲線.......................................................................................................50
圖4-21 海水中Se的突破曲線.......................................................................................................51
圖4-22 海水中Se的累積曲線.......................................................................................................51
圖4-23 海水中HTO的突破曲線...................................................................................................52
圖4-24 海水中HTO的累積曲線...................................................................................................52
圖4-25 利用濃度累積法算出來的Da值與突破曲線作圖 (a)Cs-SW、(b)Se-SW、
(c)HTO-SW.........................................................................................................................55
圖4-26 利用解析解擬合出的視擴散係數 (a)Cs-SW、(b)Se-SW、(c)HTO-SW...........................56
參考文獻
1. U.S. Energy Research Development Administration, “Alternatives for the of managing wastes from reactors and post-fission operation in the LWR fuel cycle,” Read-76-43,2, Energy Research and Development Administration, Washington, D.C. (1976).
2. 許俊男,「在模擬地下水中沸石和高嶺土對鍶銫核種的吸附機制研究,」國立清華大學原子科學系,行政院國家科學委員會專題研究計畫成果報告(1996)。
3. 張顧齡,「酸鹼度和溫度對鍶銫在膨潤土中吸附與擴散行為之影響,」國立清華大學原子科學系研究所,碩士論文(1997)。
4. W.D. Ehmann, and D.E. Dance, Radiochemistry and Nuclear Methods of Analysis, John Wiley & Sons, U.S. (1991).
5. Y. Tachi, T. Shibutani, H. Sato, M. Yui, ”Sorption and diffusion behavior of selenium in tuff,” Journal of Contaminant Hydrology, 35, 77 (1998).
6. NAGRA, “Sorption Database for Crystalline, Marl and Bentonite for Performance Assessment,” Technical Report 93-06, National Cooperative for the Disposal of Radioactive Waste, Switzerland (1995).
7. A. Muurinen, ”Diffusion of anions and cations in compacted sodium bentonite,” Technical Research Centre of Finaland, VTT Publications 168 (1994).
8. J. Crank, The Mathematics of Diffusion, Claredon Press, Oxford, UK (1975).
9. 陳子雲,「放射性廢料處置主要核種之遷移,」清華大學原子科學系研究所,碩士論文(2001)。
10. M. Ochs, B. Lothenbach, H. Wanner, H. Sato and Mikazu Yui, “An integrated sorption-diffusion model for the calculation of consistent distribution and diffusion coefficients in compacted bentonite,” Journal of Contaminant Hydrology, 47, 283(2001).
11. 劉靜蓉,「鍶銫在潛在母岩與水泥工程障壁中吸附與擴散的基礎研究,」國立清華大學原子科學系研究所,碩士論文(1999)。
12. 王明光譯,土壤環境化學,國立編譯館,台北(1991)。
13. 郭殷銘,「銫在粉碎花崗岩中宿命與傳輸模式之建立,」國立清華大學原子科學系研究所,碩士論文(2002)。
14. 黎華嵊,「銫在粉碎花崗岩與低鹽度人造地下水中傳輸之研究,」國立清華大學原子科學系研究所,碩士論文(2000)。
15. 林哲毅,「從緩衝材料觀點研究放射核種在膨潤土中的吸附與擴散行為,」國立清華大學原子科學系研究所,碩士論文(1997)。
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