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研究生:黃才榜
研究生(外文):Tsai-Bang Huang
論文名稱:氫氧氯化鈣與模來石、燃煤飛灰高溫反應之研究
論文名稱(外文):Reaction of CaClOH with Mullite and Coal Fly Ash at High Temperatures
指導教授:施信民施信民引用關係
指導教授(外文):Shin-Min Shih
口試委員:張慶源何春松劉瓊芳
口試日期:2011-07-28
學位類別:碩士
校院名稱:國立臺灣大學
系所名稱:化學工程學研究所
學門:工程學門
學類:化學工程學類
論文種類:學術論文
論文出版年:2011
畢業學年度:99
語文別:中文
論文頁數:138
中文關鍵詞:焚化飛灰氫氧氯化鈣模來石燃煤飛灰氯鹽
外文關鍵詞:incineration fly ashCaClOHmullitecoal fly ashchloride
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  • 被引用被引用:1
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  都市固體廢棄物焚化所產生之飛灰含有高含量的氯鹽及微量的重金屬與毒性有機物。氯鹽中的氫氧氯化鈣(CaClOH)會造成飛灰高溫熱處理時產生結塊、粘壁等問題。本研究探討將CaClOH與模來石或燃煤飛灰反應,以分解CaClOH並固定氯的可行性。
  CaClOH暴露於環境中會吸水潮解。CaClOH/mullite或CaClOH/coal fly ash混合物於高溫反應後會生成wadalite和calcium silicate chloride固體產物以及HCl和H2O氣體產物。反應後試樣水洗後有Friedel''s salt (Ca2Al(OH)6Cl‧2H2O)生成。CaClOH/mullite試樣在莫耳比為2時有最高之非水溶性固體氯含量分率,最高分率隨反應溫度、圓片試樣厚度、進料氣體含水量增加而上升。CaClOH/coal fly ash於高溫反應所生成之非水溶性固體氯含量分率隨反應溫度升高、重量配比減小而上升,且不受coal fly ash種類影響。CaClOH/coal fly ash粉末試樣於相同反應條件下使用coal fly ash所得之非水溶性固體氯含量分率較使用mullite者為高。CaClOH/mullite莫耳比越高(≧2)的粉末試樣,反應後其黏結及黏壁的現象越嚴重。CaClOH/coal fly ash粉末試樣反應後皆有輕微的黏結及黏壁現象。沒有CaO存在下,700℃時CaCl2並不會與mullite反應。


  Fly ash generated from MSW incinerator contains high contents of alkali chlorides and trace amounts of heavy metals and toxic organic chlorides. Calcium hydroxychloride (CaClOH), one of the alkali chlorides, can cause solidification of fly ash in the heat treatment at high temperatures. This work is to study the feasibility of decomposition of CaClOH and fixation of chlorine by reacting CaClOH with mullite or coal fly ash at high temperatures.
  CaClOH deliquesced when exposed to air. CaClOH reacted with mullite and coal fly ash at high temperatures (700-800℃) to form wadalite (Ca6Al5Si2O16Cl3), calcium silicate chloride (Ca3SiO4Cl2), HCl, and H2O. Friedel''s salt (Ca2Al(OH)6Cl‧2H2O) was found after the reacted sample was washed with water. The distribution of total chlorine in water-soluble salts, water-insoluble salts, and gas phase were mearsured. The highest mole fraction of total chlorine in water-insoluble salts was achieved at a CaClOH/mullite mole ratio of 2; the highest fraction increased with increasing reaction temperature, increasing thickness of disc sample, and increasing water vapor content of the swept gas. When CaClOH reacted with coal fly ash, the mole fraction of total chlorine in water-insoluble salts increased with increasing temperature and with decreasing CaClOH/coal fly ash weight ratio; the source of coal fly ash did not affect the reaction. Under the same reaction conditions, coal fly ash resulted in higher mole fraction of total chlorine in water-insoluble salts than millite. Reacted powder samples of CaClOH/mullite sintered when the mole ratios ≧ 2; all those of CaClOH/coal fly ash slightly sintered. CaCl2 alone did not react with mullite at 700℃.


目錄 I
摘要 III
Abstract IV
符號說明 VI
圖表索引 VII
第一章 緒論 1
1-1 研究緣起 1
1-2 研究目標 3
第二章 文獻回顧 4
2-1 焚化飛灰的介紹 4
2-1-1 都市垃圾焚化飛灰的來源 4
2-1-2 焚化飛灰的成分 6
2-1-3 焚化飛灰中氯鹽成份分析 9
2-1-4焚化飛灰中重金屬、毒性氯化有機物來源及其危害 9
2-2 氫氧氯化鈣生成之研究 12
2-3 氫氧氯化鈣及相關物質之熱力學性質 13
2-4 氫氧氯化鈣與添加物反應之研究 17
2-4-1 氫氧氯化鈣與添加物高溫反應之研究 17
2-4-2 模來石之研究 23
2-4-2-1 模來石之製備 24
2-4-3 燃煤飛灰 24
2-4-4 Wadalite之研究 25
2-4-4-1 Wadalite的結構分析 25
2-4-4-2 Wadalite之生成 26
2-4-5 Calcium silicate chloride之研究 27
第三章 實驗與分析方法 29
3-1 試藥來源 29
3-2 試樣製備 30
3-2-1 CaClOH製備 32
3-2-2 CaClOH/mullite及CaClOH/coal fly ash試樣製備 32
3-3 CaClOH室溫下穩定性實驗 35
3-4 CaClOH/mullite及CaClOH/coal fly ash高溫反應實驗 35
3-4-1 反應實驗設備 35
3-4-2 反應實驗步驟 37
3-4-3 反應實驗條件 38
3-5 試樣分析 38
3-5-1 重量測定 38
3-5-2 BET比表面積及孔隙體積分佈測定 39
3-5-3 粒徑分析 39
3-5-4 真實密度測定 39
3-5-5 X光繞射分析(XRD) 40
3-5-6 電子顯微鏡分析(SEM) 40
3-5-7 EDTA滴定 40
3-5-8 熱重分析與熱差分析(TG-DTA) 41
3-5-9 反應後試樣生成物分析 43
3-5-10 離子層析(IC) 43
3-5-11 固體氯含量分佈分析 45
3-5-12 實驗誤差 48
第四章 結果與討論 49
4-1 CaClOH室溫下穩定性實驗 49
4-2 CaClOH與模來石之反應 54
4-2-1 反應產物 54
4-2-2 反應時間對CaClOH與模來石反應之影響 67
4-2-3 CaClOH/模來石莫耳比對反應之影響 70
4-2-4 試樣加壓成型對CaClOH與模來石反應之影響 74
4-2-5 煅燒溫度對CaClOH與模來石反應之影響 84
4-2-5-1 粉末試樣 84
4-2-5-2 圓片試樣 93
4-2-6 進料氣體對CaClOH與模來石反應之影響 98
4-2-7水蒸氣對CaClOH與模來石反應之影響 104
4-3 CaClOH與coal fly ash之反應 110
4-3-1 煅燒溫度對CaClOH與coal fly ash反應之影響 110
4-4 CaClOH/mullite與CaClOH/coal fly ash粉末試樣反應結果之比較 122
4-5 CaClOH/mullite與CaClOH/coal fly ash反應後試樣外觀觀測 127
4-6 CaCl2與模來石之反應性 127
第五章 結論 132
參考文獻 134

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