臺灣博碩士論文加值系統

　　本研究考慮銫在粉碎花崗岩中之遷移與遲滯。主要目的在探討吾人是否可將批次實驗的結果與所採用的線性、Freundlich、Langmuir或Elovich經驗收附模式直接應用在管柱實驗結果的推估上。在批次實驗中包括了收附與脫附實驗兩部分，目的是探討銫的動力收、脫附反應。而管柱實驗中則包括了擴散(diffusion)實驗及平流(advection)實驗。目的在於用所得的突破曲線(breakthrough curve)探討水流速對收、脫附的影響。批次實驗結果所擬合的收附模式中以Elovich收附模式為最佳，但所擬合的參數值仍然會隨濃度改變而改變。從管柱實驗的結果分析中，吾人認為銫在粉碎花崗岩的收、脫附反應機制可能至少包括兩種速率的反應，而這四種經驗收附模式均無法合適地描述系統內的收附機制。實驗分析結果顯示，在此二公分的管柱中，管柱實驗所求得的參數值與批次實驗求得參數值很接近。

This study investigated the migration and retardation of cesium in crushed granite. The main purpose was to determine whether the sorption model parameters determined from the batch experiment can be applied to estimating the transport result from the column method. Four empirical sorption models, including linear, Freundlich, Langmuir, and Elovich, were taken to fit experimental data. The batch experiment, containing both sorption and desorption experiments, was to study the sorption/desorption kinetics. While the column experiment was taken to examine, through the analysis of breakthrough curves, how flow rate would affect sorption/desorption, and as a result, the retarded migration result. Both advection-dispersion and diffusion column experiments were conducted to achieve the purpose. The Elovich model, among the four sorption models, was determined to best fit the batch experimental result. However, the fitting parameter values varied with cesium concentration. It was also determined, based on the analysis of the column experimental data, that at least two sorption reactions of different rates would contribute to the overall reaction, and none of the four empirical sorption models can adequately describe the system''s sorption/desorption kinetics. Through data analysis, in the 2 cm column, the sorption parameters determined from the column experiment and in the batch experiment are similar.

摘要ii
Abstractiii
致謝iv
目錄v
表目錄vii
圖目錄viii
第一章 緒論1
1-1 背景介紹1
1-2 實驗目的2
第二章 理論3
2-1 收附理論3
2-1-1 線性收附模式3
2-1-2 Freundlich 收附模式4
2-1-3 Langmuir 收附模式4
2-1-4 Elovich 收附模式5
2-2 傳輸理論6
2-2-1 平衡模式6
一、線性平衡模式7
二、Freundlich平衡模式7
三、Langmuir平衡模式7
四、Elovich平衡模式7
2-2-2 動力模式7
一、線性動力模式8
二、Freundlich動力模式8
三、Langmuir動力模式8
四、Elovich動力模式8
2-2-3 擴散理論8
第三章 方法10
3-1 批次實驗10
3-1-1 實驗材料10
一、人造地下水(AGW)10
二、含銫人造地下水(AGW_S)10
三、粉碎花崗岩10
3-1-2 實驗步驟11
一、收附實驗11
二、脫附實驗11
3-2 管柱實驗13
3-2-1 實驗材料13
一、人造地下水(AGW)13
二、含銫人造地下水(AGW_S)13
三、粉碎花崗岩13
3-2-2 擴散實驗13
3-2-3 平流實驗15
第四章 結果19
4-1 實驗前處理19
4-2 批次結果20
4-2-1 批次結果的擬合曲線20
4-2-2 批次實驗與收、脫附模式的相關性22
4-3 管柱結果30
4-3-1 擴散實驗結果30
4-3-2 平流結果的擬合曲線31
4-4 批次與管柱之比較39
第五章 結論40
參考文獻41

 Aharoni, C., N.S. Pasricha and D.L. Sparksm, 1992. "Adsorption and desorption kinetics of cesium in an organic matter rich soil saturated with different cations." Soil Sci., 156: 233-239.
 Artinger, R., B. Kienzler, W. Schubler and J.I. Kim, 1998. "Effects of humic substances on the 241Am migration in a sandy aquifer: column experiments with Gorleben groundwater/sediment systems." J. Contam. Hydrol., 35: 261-275.
 Cornell, R.M., 1993. "Adsorption of cesium on minerals: A review." J. Radioanal. Nucl. Chem., 171: 482-500.
 Crank, J., 1975. The Mathematics Of Diffusion, Oxford University Press, London.
 Ehmann, W.D. and D.E. Dance, 1991. Radiochemistry and Nuclear Methods of Analysis, John Wiley & Sons, U.S.
 Fava, A. and H. Eyring, 1956. "Equilibrium and kinetics of detergent adsoprion - a generalized equilibrium theory." J. Phys. Chem., 60: 890-898.
 Frech, C., W. Simon, S.B. Baderlein, P. Reichert and R.P. Schwarzenbach, 1998. "Nonlinear sorption and nonequilibrium solute transport in aggregated porous media: Experiments, process identification and modeling." J. Contam. Hydro., 31: 373-407.
 Hemond, H.F. and E.J. Fechner, 1994. Chemical Fate And Transport In The Eniveronment, Academic Press, U.K.
 Holtta, P., M. Siitari-Kauppi, A. Lindberg and A. Hautojarvi, 1998. "Na, Ca and Sr retardation on crushed crystalline rock." Radiochim. Acta., 82: 279-285.
 Lide, D.R., Editor-in-Chief, 1992. Hand Book of Chemical and Physics, 73rd ed, Chemical Rubber Company Press, U.S.
 Press, W.H., S.A. Teukolsky, W.T. Vetterling and B.P. Flannery, 1992. Numerical Recipes In FORTRAN : The Art Of Scientific Computing, 2nd ed, Cambridge University Press, New York.
 Saiers, J.E. and G.M. Hornberger, 1996. "Migration of 137Cs through quartz sand: Experimental results and modeling approaches." J. Contam. Hydro., 22:255-270.
 von Gunten, H.R., U.E. Waber, and U. Krahenbuhl, 1988. "The reactor accident at Chenobyl: Apossibility to test colloid-controlled transport of radionuclides in a shallow aquifer." J. Contam. Hydrol., 3: 237-247.
 Yeh, G.-L., G. Iskra, J.M. Zarchara and J.E. Szecsody, 1998. "Development and verifications of a mixed chemical kinetic and equilibrium model." Advances in Environmental Research, 2(1): 24-56.