台灣地區的垃圾係以焚化為主要的處理方式，焚化處理雖具有減容、減量、衛生之效果，但仍產生一定比例的灰渣，其中飛灰內含重金屬等有害物質，易溶出而超過有害廢棄物認定標準，因此被判定為有害廢棄物，需經適當處理降低其毒性後始可進掩埋場。由於新掩埋場開發愈形不易，且固化體的長期重金屬穩定性仍有疑慮，因此追求有效的飛灰無害化及資源化技術之開發，已成為刻不容緩的議題。
本研究引進機械化學反應(Mechanochemical Reaction)之觀念，藉由機械能促使飛灰中的重金屬特性改變，達到穩定不易溶出的效果。本研究以採高能球磨以減少所需的研磨時間，首先找出最佳的濕式高能球磨操作條件，再探討重金屬鉛穩定機制。此外，機械化學研磨後由於粒徑減小，大幅度提高表面積，有助於吸濕性能，故嘗試再利用為製備調濕陶瓷材料的原料，搭配含大量鋁矽酸鹽的高嶺土，提高燒結性。另一方面，利用飛灰富含鈣基的特性，與高嶺土進行調配，並藉由機械研磨達成軟化學合成反應，製成鈣長石基陶瓷產品。
由實驗結果發現，濕式高能球磨研磨8小時即可達到傳統濕式球磨研磨96小時對鉛的穩定效率。而鉛在飛灰之高pH值下與氯離子反應生成Pb7O6Cl2的沉澱，經研磨處理後會形成較穩定的PbO2及Pb2O3。由數學關係式求得鉛穩定因子權重，發現研磨灰穩定能力最高，達92.44 %，鉛氯鹽沉澱穩定效果最低且為負值，且在試驗中會影響其他作用的穩定性。
機械化學研磨8小時的水萃飛灰與高嶺土調配後可製成良好調濕性能的調濕陶瓷材料，吸濕量為日本調濕建材性能評價委員會之等級3，放濕率並可達到70 %標準。而研究中也發現鈣鋁石(Mayenite，Ca12Al14O33【C12A7】)之繞射峰強度與吸放濕量成正比，而鈣鋁黃長石(Gehlenite，Ca2Al2SiO7【C2AS】)之繞射峰強度則成反比，鈣鋁石的生成有助於長時間研磨的燒結體之吸放濕。
機械研磨飛灰-高嶺土不僅將粉體粒徑減小，且使粉體達到無晶序化(amorphization)，粉體的無晶序化和燒結後鈣長石相對含量具正相關；而以焚化飛灰作為合成鈣長石的鈣源，經研磨粉體燒製後，可觀察到眾多短柱狀的鈣長石結晶，成功製備出鈣長石基陶瓷材料，並將燒製的溫度從1,300 ℃降至950 ℃，經燒製後的產品，重金屬溶出已經非常低，產品已無害化。

In Taiwan, incineration had become the major method to treat the municipal solid waste. Incineration has the advantages of good volume and mess reduction efficiency and healthy, but the residual fly ash was classified as hazardous waste since it contained much heavy metals, which could not pass the TCLP test, and should be solidified before landfilling. Nevertheless, the landfill site is difficult to be installed, and the long-term stability of the heavy metals of the solidified matrix was doubted by the publics. Therefore, to develop new detoxification and recovery technologies for fly ash are urgently.
This study introduced the concept of mechanochemical reactions, which provided mechanical energy to promote the characteristics change of the heavy metals in the fly ash to reach the aim of stability. In this study, the high energy ball milling was used to reduce the milling time. The optimum operation conditions for wet milling were studied, and then to explore the stabilization mechanism of lead. Furthermore, milled fly ash powder was blended with aluminum silicate rich kaolin, and sintered to produce humidity-controlling ceramic as the ecological building material. On the other hand, the soft mechanochemical synthesis mechanism was applied in the anorthite-based ceramic production with fly ash blended with kaolin, due to the rich calcium-based property of fly ash.
 The results showed that, 8 hours milling can reach the effect of 96 hours traditional wet ball milling for lead stabilization. Lead in the high pH could react with chloride ions to generate Pb7O6Cl2 precipitation, after milling, the much stable species PbO2 and Pb2O3 will produced. The results of the mathematical relationship analysis for weight factors of lead stabilization showed that, the highest weight factors is milled ash, 92.44 %; but the lowest is lead chloride salt which weight factor, which is negative, and it will affect the other stability effects. 
The humidity-controlling ceramic produced from mixed powder milled 8 hours and then sintered at 1,000 oC performed 70 % moisture absorption ability, which can meet the grade 3 standard in Japan. It was found that the intensity of the diffraction peaks of mayenite (Ca12Al14O33, C12A7) of sintered sample is proportional to the amount of moisture absorption and desorption, while calcium aluminum (Ca2Al2SiO7, C2AS) is inversely proportional. Therefore, the mayenite generated in sintered specimen is helpful to moisture absorption and desorption.	
Mechanical milling of the fly ash with kaolin not only decreases particle size, but also transforms the crystals into amorphization. Furthermore, the amorphization of the powder and relative content of anorthite after sintering process have a positive correlation. Using fly ash as a calcium source to synthesize anorthite by milling and sintering could observe many short columnar crystals of anorthite. The process of milling and sintering can successfully prepare anorthite-based ceramic materials and could decrease the sintering temperature from 1,300 oC to 950 oC. The leaching of heavy metals of the product is very low and it has been harmlessly.

目錄
第一章	前言	1
1.1	研究緣起	1
1.2	研究目的及內容	4
第二章	文獻回顧	6
2.1	垃圾焚化飛灰介紹	6
2.1.1	垃圾焚化灰渣的來源及產量	6
2.1.2	焚化灰渣種類及特性	8
2.1.3	反應灰之特性	11
2.1.4	焚化飛灰常見處理/處置方法	25
2.1.5	飛灰資源化再利用技術	29
2.2	機械化學作用介紹	29
2.2.1	機械化學的過程	30
2.2.1	機械化學的原理	33
2.2.2	機械化學的效應	36
2.2.3	各種參數對機械化學製程的影響	47
2.2.4	機械化學在環境工程上的應用	48
2.3	調濕材料的介紹	51
2.3.1	調濕材料的原理	52
2.3.2	調濕材料孔隙特性	54
2.3.3	多孔陶瓷材料的成孔之製備方法	57
2.3.4	調濕建材調濕性能之評估標準	58
2.4	鈣長石的合成	60
2.4.1	鈣長石的介紹	60
2.4.2	鈣長石的用途	61
2.4.3	鈣長石的合成	62
第三章	研究方法及步驟	65
3.1	研究方法	65
3.2	研究步驟	69
3.2.1	濕式高能球磨對鉛穩定機制之探討	69
3.2.2	穩定後研磨灰製備調濕陶瓷材料之可行性	80
3.2.3	機械化學法促進飛灰合成鈣長石陶瓷	86
3.3	分析方法	92
第四章	結果與討論	96
4.1	原料特性之結果與討論	96
4.1.1	垃圾焚化飛灰之基本特性	96
4.1.2	高嶺土之基本特性分析	103
4.2	濕式高能球磨對鉛穩定機制之探討	105
4.2.1	最佳重金屬鉛穩定效率	105
4.2.2	高能濕式球磨穩定重金屬之機制探討	114
4.3	穩定後研磨灰製備調濕陶瓷材料之可行性	130
4.3.1	水萃飛灰量對製備調濕陶瓷之影響	130
4.3.2	不同研磨時間之研磨灰對製備調濕陶瓷之影響	143
4.1	研磨製備水萃飛灰-高嶺土無晶序化粉體對合成鈣長石之影響	154
4.1.1	飛灰作為鈣長石的鈣源之可行性	154
4.1.2	不同研磨時間對粉體特性的影響	155
4.1.3	研磨粉體製備鈣長石之影響	162
第五章	結論	169
參考文獻	173


 
圖目錄
圖3 - 1 研究架構圖	68
圖3 - 2 機械化學法穩定重金屬鉛機制探討之流程圖	69
圖3 - 3 處理程序及酸萃試驗之輸入和輸出	71
圖3 - 4 各試驗加入的物質	75
圖3 - 5 研磨灰製備調濕陶瓷材料可行性之流程圖	80
圖3 - 6 可調控恆溫恆濕實驗設備圖	85
圖3 - 7 機械化學法促進水萃飛灰-合成鈣長石陶瓷之流程圖	86
圖3 - 8 鈣長石合成燒製條件	90
圖4 - 1 飛灰及水萃飛灰之外觀	97
圖4 - 2 飛灰及水萃飛灰之粒徑分佈圖	97
圖4 - 3 飛灰之SEM圖	98
圖4 - 4 水萃飛灰之SEM圖	99
圖4 - 5 飛灰的物種分析	101
圖4 - 6 高嶺土之粒徑分佈	103
圖4 - 7 高嶺土的物種分析	104
圖4 - 8 不同磨球配比與研磨時間之(a) 研磨液 (b) 研磨灰酸萃液之Pb含量及百分比	107
圖4 - 9 不同研磨時間的研磨灰之XRD分析	107
圖4 - 10 不同鉛濃度的攪拌灰之XRD	109
圖4 - 11 不同鉛液濃度攪拌處理 (a) 攪拌液 (b) 攪拌灰酸萃液之Pb含量及Pb殘留百分比	110
圖4 - 12 不同鉛液濃度攪拌處理之鉛穩定效率	110
圖4 - 13 不同攪拌和研磨時間之(a) 研磨液 (b) 研磨灰酸萃液之Pb含量及百分比	112
圖4 - 14 不同鉛液濃度、磨球配比、攪拌或研磨時間之重金屬Pb的處理穩定效率	113
圖4 - 15 試驗A1及A2的處理灰之XRD分析	116
圖4 - 16 試驗A1及A2的處理灰之SEM分析	117
圖4 - 17 試驗B1及B2的處理灰之XRD分析	118
圖4 - 18 試驗B1及B2的處理灰之粒徑分佈	118
圖4 - 19 試驗B1及B2的處理灰之SEM分析	119
圖4 - 20試驗C1及C2的處理灰之XRD分析	120
圖4 - 21 試驗C1及C2的處理灰之SEM分析	121
圖4 - 22 試驗D1及E1的處理灰之XRD分析	122
圖4 - 23 試驗D1及E1的處理灰之SEM分析	122
圖4 - 24 鉛於處理程序中的穩定作用	123
圖4 - 25 (a) A1 (b) A2試驗中各鉛穩定作用所占比例	129
圖4 - 26 不同水萃飛灰添加量之動態濕度應答分析	132
圖4 - 27不同水萃飛灰添加量之吸放濕速率	132
圖4 - 28 不同水萃飛灰添加量之調濕性能	133
圖4 - 29 不同水萃飛灰添加量之燒失量及體積變化率	135
圖4 - 30 不同飛灰量之體積變化率、燒失量、吸濕量、放濕量變化	135
圖4 - 31 C2S的多晶轉變	137
圖4 - 32 不同水萃飛灰量燒後之XRD	137
圖4 - 33 不同水萃飛灰添加比例之成分三相圖	138
圖4 - 34 不同水萃飛灰量燒製後之微觀	141
圖4 - 35不同水萃飛灰量燒製後之結晶情況	142
圖4 - 36不同研磨時間試體燒後之動態濕度應答分析	145
圖4 - 37不同研磨時間燒後之吸放濕速率	145
圖4 - 38不同研磨時間燒後之調濕性能	146
圖4 - 39不同研磨時間試體之燒失量及體積變化率	147
圖4 - 40不同研磨時間燒後試體之XRD	149
圖4 - 41 不同研磨時間燒後試體其鈣鋁石與鈣鋁黃長石最主要繞射峰之強度變化	149
圖4 - 42 研磨0 、1、5 、8、10小時試體燒後之微觀	151
圖4 - 43研磨0 、1、5、8、10小時試體燒後之結晶情況	152
圖4 - 44 不同鈣源試燒後試體之XRD圖	154
圖4 - 45 KWFA不同研磨時間的粉體之粒徑分佈	155
圖4 - 46 KWFA不同研磨時間的粉體之平均粒徑變化	156
圖4 - 47 KWFA不同研磨時間的粉體之SEM變化	158
圖4 - 48 KWFA不同研磨時間的粉體之XRD變化	159
圖4 - 49 KWFA經不同研磨時間的粉體之X射線繞射峰之強度及無晶序化程度	159
圖4 - 50 KWFA經不同研磨時間的粉體之熱分析	161
圖4 - 51不同研磨時間的粉體進行燒製900~1,300 ℃後之XRD	164
圖4 - 52 KWFA不同研磨時間的燒結體之相對鈣長石量	165
圖4 - 53 KWFA不同研磨時間經1200 oC燒製的燒結體之SEM	167
 
表目錄

表4 - 1 飛灰基本物理特性分析	97
表4 - 2 飛灰主要組成元素分析	100
表4 - 3 飛灰重金屬含量	102
表4 - 4 飛灰之TCLP	102
表4 - 5 高嶺土主要組成元素分析	104
表4 - 6 各試驗之液體及固體鉛含量與處理、酸萃殘留率及穩定效率	114
表4 - 7 鉛穩定因子權重	127
表4 - 8 K(001)和K(002)對不同溫度燒結後之鈣長石相對含量之相關性	166
表4 - 9 KWFA研磨5小時燒製1,200 oC的燒結體之TCLP	168

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