博碩士論文 90342017 詳細資訊



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姓名 陳文泉(Wen-Chuan Chen)  查詢紙本館藏   畢業系所 土木工程學系
論文名稱 高放射性廢棄物深層地質處置緩衝材料之回脹行為研究
(The study on swelling behavior of buffer material in a deep geological repository)
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摘要(中) 高放射性廢棄物最終處置是核能發電國家關切的環保議題，目前各國都致力於深層地質處置系統的研究發展。本論文以深層地質處置系統中，緩衝材料在處置場近場環境回脹成效為研究軸心，以具潛力的台灣日興土與美國懷俄明州膨潤土（BH膨潤土）為試驗材料，探索膨潤土在深層地質處置場特殊環境下的回脹行為。
試驗結果顯示日興土的主要黏土組成為鈣型鋁蒙脫石，材料成分中含高量鐵化合物，其性質與法國FoCa黏土相近。BH膨潤土則以鈉型蒙脫石為主要組成礦物。熱重分析結果顯示BH膨潤土比日興土具較佳的抗熱性。
高放射性廢棄物處置後，其衰變熱與放射性會持續釋出而影響近場環境，而海水入侵也是瀕海處置場首要分析的重要情節。本研究模擬近場環境對緩衝材料的回脹性質影響，結果發現：
（1）水熱溫度的提昇，將使日興土因熱擾動而使表面吸附水層減少，引發回脹量下降。而BH膨潤土則因滲透壓力增加而回脹量增加。
（2）經高溫熱處理後的膨潤土，其可交換陽離子會移入黏土結構層間或緊密嵌在表面之上，補償結構負電荷，可交換陽離子容量隨之降低，回脹量也因而降低。
（3）膨潤土在NaCl及CaCl2溶液系統中形成不同結構，在NaCl溶液系統中的結構趨向分散狀態，致使回脹行為與擴散雙層理論一致；在CaCl2溶液系統中的膨潤土則形成擬結晶結構，回脹行為無法適用擴散雙層理論。
日興土的自由回脹量約為BH膨潤土的七分之一，藉由添加Na2CO3使其於溶液相中引發離子交換程序，可使日興土改質為鈉型膨潤土，提升其回脹量。由於離子交換的改質程序具遲滯性，故改質土的回脹歷時曲線呈現後期上升的曲線型態。經離子交換程序後的改質日興土，最大回脹量可提升3倍。改質土對輻射衰變熱的耐受性良好，對於200℃乾燥加熱與90℃的水熱環境條件下，都能發揮其回脹潛能。
摘要(英) Bentonites serve as buffer material in an engineered barrier system for isolation of high-level radioactive wastes because of their high swelling potential. In the current proposal for deep geological disposal of the high-level wastes in Taiwan, compacted bentonite is used to contain the metallic waste canisters and separate the waste from the host rock and backfilled materials. Two bentonite samples are used in this study, namely Zhisin clay and BH bentonite. Zhisin clay was identified as a Ca-bentonite, and BH bentonite is a Na-bentonite.
Several near field conditions including decay heat, radioactivity, and groundwater intrusion in a deep geological repository are simulated in this work. Free swelling tests were performed in accordance with the ISRM suggested procedures.
The maximum swelling strain of Zhisin clay decreases with increasing hydrothermal temperature. On the other hand, the maximum swelling strain of BH bentonite increases with increasing hydrothermal temperature. Lattice contraction and osmotic pressure enhancement are judged to be the dominating mechanisms affecting the swelling of Zhisin clay and BH bentonite, respectively.
Thermal treatment of clayey soils was found to result in marked decrease in CEC (cation exchange capacity). Reductions in CEC resulted from thermal treatment caused the swelling of bentonites to decrease.
The maximum swelling strain of bentonites decreases in salt solutions. The amount of reduction in swelling strain is affected by the type of electrolyte and the concentration of solution. The swelling behavior in a NaCl solution conforms to the diffuse double layer theory, so the swelling strain decreases with increasing concentration. Due to the formation of quasi-crystals in the presence of calcium ions, the swelling strains of bentonites in CaCl2 solutions, regardless of the concentration, are much lower.
To enhance the swelling potential of Zhisin clay, a cation exchange process by the addition of Na2CO3 powder is introduced in this research. Experimental results show that Na2CO3-activated Zhisin clay is superior in swelling potential to untreated Zhisin clay. Due to the ion exchange hysteresis, activated bentonite shows a different type of time-swell curve than the traditional sigmoid-shaped curve. The optimal amount of Na2CO3 addition was found to be 1%, and the maximum swelling strain was 3 times as much as that of untreated Zhisin clay. The Na2CO3-activated Zhisin clay exhibits improved resistance to thermal environments and behaves similar to the Na-type bentonites under different hydrothermal temperatures.
關鍵字(中) ★ 緩衝材料
★ 深地層處置
★ 回脹
★ 膨潤土		 關鍵字(英) ★ buffer material
★ deep geological repository
★ swelling behavior
★ bentonit
論文目次 目 錄
摘要............................................................................................................ I
誌謝.......................................................................................................... Ⅵ
目錄.......................................................................................................V III
圖目錄.................................................................................................... XV
表目錄................................................................................................... XXI
第一章 緒論............................................................................................ 1
1.1 研究動機...................................................................................... 1
1.2 研究目的及內容.......................................................................... 2
1.3 論文架構...................................................................................... 4
第二章 文獻回顧（一）：緩衝材料的特性.......................................... 6
2.1 緩衝材料功能需求...................................................................... 6
2.2 膨潤土礦物的結構特性.............................................................. 9
2.2.1 膨潤石、膨潤土、蒙脫石的差異...................................... 9
2.2.2 膨潤土礦物結晶結構.......................................................... 9
2.2.3 膨潤土的微觀結構............................................................ 11
2.2.4 膨潤土水合結構................................................................ 14
2.3 深層處置場近場環境的演化.................................................... 16
2.3.1 近場溫度演化與效應........................................................ 16
2.3.2 輻射場................................................................................ 18
2.3.3 地下水化學........................................................................ 19
2.3.4 近場pH值演化................................................................. 25
2.4 膨潤土活化改質研究................................................................ 26
2.4.1 物理改質方法研究............................................................ 27
2.4.2 酸活化改質方法................................................................ 28
2.4.3 離子交換改質方法............................................................ 30
2.4.4 熱學改質方法.................................................................... 32
2.5 膨潤土基緩衝材料性質探討.................................................... 38
2.5.1 第二相對結構之效應........................................................ 38
2.5.2 第二相對工程性質的效應................................................ 39
第三章 文獻回顧（二）：黏土－水－電解質系統............................ 52
3.1 擴散雙層理論與壓實黏土回脹行為的適用性........................ 52
3.1.1 擴散雙層理論. .................................................................. 52
3.1.2 擴散雙層厚度的影響因子................................................ 54
3.1.3 電雙層理論應用於壓實黏土的挑戰................................ 55
3.2 離子交換理論與特性................................................................ 57
3.2.1 離子交換反應與原理說明................................................ 57
3.2.2 離子交換方程式................................................................ 59
3.2.3 離子交換遲滯性................................................................ 60
3.3 膨潤土的回脹性質.................................................................... 63
3.3.1 緩衝材料的回脹性質要求................................................ 63
3.3.2 回脹型態分類.................................................................... 63
3.3.3 回脹行為............................................................................ 66
3.3.4 水熱溫度對回脹之關係.................................................... 67
3.3.5 電解質溶液對回脹之影響................................................ 69
3.3.6 pH值對回脹之影響.......................................................... 69
第四章 研究規劃.................................................................................. 77
4.1 試驗材料.................................................................................... 77
4.1.1 日興土................................................................................ 77
4.1.2 BH膨潤土.......................................................................... 77
4.1.3 石英砂................................................................................ 78
4.1.4 石墨.................................................................................... 78
4.2 基本物理性質試驗.................................................................... 79
4.3 礦物性質分析方法.................................................................... 80
4.3.1 化學成分分析.................................................................... 80
4.3.2 可交換陽離子量測............................................................ 80
4.3.3 X光繞射分析.................................................................... 81
4.3.4 傅立葉轉換紅外線光譜儀分析........................................ 81
4.3.5 熱重分析............................................................................ 82
4.3.6 電子顯微鏡觀察................................................................ 83
4.3.7 膨潤土pH值與Eh值量測............................................... 83
4.3.8 氣體層析儀........................................................................ 84
4.4 回脹試驗.................................................................................... 85
4.4.1 回脹試驗方法選擇............................................................ 85
4.4.2 回脹試體製作.................................................................... 85
4.4.3 單向度回脹試驗................................................................ 86
4.5 模擬近場環境之試驗方法........................................................ 88
4.5.1 衰變熱效應........................................................................ 88
4.5.2 輻射效應............................................................................ 88
4.5.3 地下水化學效應................................................................ 89
4.5.4 pH值效應.......................................................................... 89
4.6 日興土活化改質方法................................................................ 92
4.6.1 物理方法............................................................................ 92
4.6.2 酸活化方法........................................................................ 92
4.6.3 離子交換法........................................................................ 92
第五章 膨潤土物理化學性質.............................................................. 96
5.1 基本物理性質分析.................................................................... 96
5.1.1 比重分析............................................................................ 96
5.1.2 粒徑分析............................................................................ 97
5.1.3 阿太堡限度試驗................................................................ 97
5.2 材料性質分析............................................................................ 98
5.2.1 化學組成分析.................................................................... 98
5.2.2 可交換陽離子容量分析.................................................... 98
5.2.3 X光繞射分析.................................................................... 99
5.2.4 紅外光光譜分析................................................................ 99
5.2.5 熱重分析.......................................................................... 100
5.2.6 電子顯微鏡觀察.............................................................. 101
第六章 模擬近場環境之回脹行為探討............................................ 108
6.1 回脹歷時曲線型態.................................................................. 108
6.2 雙曲線模式推估最大回脹量探討.......................................... 110
6.3 日興土與BH膨潤土回脹行為差異性探討........................... 113
6.3.1 黏土含量因素.................................................................. 113
6.3.2 非回脹性礦物效應.......................................................... 114
6.3.3 結構負電荷因素.............................................................. 115
6.3.4 可交換陽離子因素.......................................................... 116
6.4 熱處理對自由回脹行為之效應.............................................. 119
6.4.1 乾燥加熱後試體的回脹行為.......................................... 119
6.4.2 乾燥加熱膨潤土的材料性質.......................................... 123
6.5 水熱溫度對自由回脹行為的影響.......................................... 126
6.6 輻射對自由回脹行為的影響.................................................. 129
6.7 地下水化學對自由回脹的影響.............................................. 131
6.7.1 陽離子效應...................................................................... 131
6.7.2 陰離子效應...................................................................... 134
6.8 pH值對自由回脹的影響........................................................ 139
6.8.1 膨潤土的pH值調節能力............................................... 139
6.8.2 膨潤土在酸性溶液的回脹行為...................................... 141
6.8.3 膨潤土在鹼性溶液的回脹行為...................................... 143
6.9 小結..........................................................................................145
第七章 日興土活化改質研究............................................................ 190
7.1 物理改質法.............................................................................. 191
7.2 酸活化改質法.......................................................................... 193
7.2.1 酸活化改質試驗.............................................................. 193
7.2.2 酸活化機制探討.............................................................. 194
7.3 Na2CO3離子交換程序法........................................................ 197
7.3.1 回脹歷時曲線型態分析.................................................. 197
7.3.2 Na2CO3添加量之效應.................................................... 200
7.3.3 陳化時間之影響.............................................................. 202
7.4 Na2CO3改質日興土的穩定性評估........................................ 204
7.4.1 乾燥加熱.......................................................................... 204
7.4.2 水熱環境.......................................................................... 204
7.5 小結......................................................................................... 206
第八章 BH膨潤土複合材料之回脹行為.......................................... 229
8.1 複合材料的回脹行為研究回顧.............................................. 230
8.1.1 微分模式分析.................................................................. 230
8.1.2 有效黏土乾密度概念...................................................... 231
8.2 石英砂細度對回脹行為之效應............................................. 234
8.3 添加鈍性材料對回脹行為之影響.......................................... 236
第九章 結論與建議............................................................................ 244
9.1 結論......................................................................................... 244
9.2 建議......................................................................................... 247
參考文獻................................................................................................ 249
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指導教授 黃偉慶(Wei-Hsing Huang) 審核日期 2005-1-10
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