都市垃圾焚化飛灰經過水萃處理程序之後，可去除大量的溶解性的鹽類，對
於後續再利用之產品的穩定性有相當顯著之成效。而水萃後的飛灰經由機械研磨
處理程序後，顯示出相當低的重金屬溶出效果，證明具有穩定重金屬的效果。而
研磨後的水萃反應灰(研磨灰)在取代部分市售水泥製成水泥漿體後，顯示具有卜
作嵐性質。本研究利用機械研磨使焚化飛灰的物理與化學性質同時轉變，降低重
金屬移動性，搭配鹼活化促進無機膠體的產生，掺配於市售水泥，達到無害化及
資源化之目標。
實驗以水、不同濃度之磷酸(0.002 M、0.2 M PO4
3-)、不同濃度之氫氧化鈉(1M、
5M)為鹼液，研磨時間設定為0.5、1、24、96 小時，水泥漿體養護時間為0.35、
0.38、0.45、0.55，漿體養護時間為1、3、7、28 天。以ICP、粒徑分析儀、比表
面積儀、壓汞分析儀、X 光繞射儀、核磁共振儀等進行分析。
焚化飛灰經研磨96 小時後發生無晶序化，使重金屬溶出降至接近儀器偵測極
限。加入研磨飛灰的水泥漿體其膠體孔隙與毛細孔隙含量比純水泥漿體高出許
多，形成的漿體較緻密，以NMR 分析後發現C-S-H 聚合度提升，抗壓強度與市
售水泥相比顯著提升，由此可證明長時間研磨的焚化飛灰有助於加強水化反應與
促進卜作嵐反應的進行。
當以0.2 M 磷酸研磨液進行研磨時，研磨時間小於1 小時即產生許多磷酸鈣
結晶 (HAp, TCP, TTCP)，然而可解離的磷酸鈣化合物及過多的PO4
3-殘留，將消
耗水泥中的氫氧化鈣，經96 小時研磨後，降低水泥強度的效果大於研磨提升水泥
強度的效果，導致漿體抗壓強度較市售水泥漿體為低。以0.002 M 磷酸進行時，
由於研磨灰中產生大量的TTCP，遇水解離成HAp 與氫氧化鈣，然而長時間研磨
所產生的卜作嵐反應造成7 天與28 天抗壓強度仍大於OPC。
以不同偏高嶺土調配比進行研磨活化時(1 M 氫氧化鈉、24 小時)，發現鹼液
濃度的不足，未能將矽酸鹽溶出。研磨活化所產生的化合物可進行離子交換反應，
達到穩定重金屬的效果。然而當鹼液濃度提高時(5 M 氫氧化鈉)，則變成由活化膠
體與重金屬離子進行接合，由於鍵結強度較弱，研磨造成溶出僅略為增加，此外，
高濃度氫氧化鈉則會對水化反應造成負面的影響。
利用5 M 氫氧化鈉搭配煆燒淨水污泥進行研磨活化，水萃反應灰調配量較高
時，會產生穩定的氯離子結晶，調配量較低時，則產生膠體型態以物理穩定機制
結合氯離子，加入水泥漿體卻使得穩定性較差，可知活化粉形成結構較弱的膠體
反而不利於水泥早期反應結合氯離子。以水為研磨液時，產生許多類似Friedel’s
salt 結構，因而有顯著的化學穩定性能，在7 天齡期中水泥漿體即有相當優良的
氯離子穩定效果。以無機膠體形態掺配於水泥中，其氯離子的穩定型態和反應過
程和傳統水泥大不相同。

This study used mechanical milling to change physical and chemical properties of
municipal solid waste incinerator (MSWI) fly ash. The mobility of heavy metals would be
reduced by mechanical milling and the amount of inorganic gelwould be also promoted by
alkali activation of the MSWI fly ash. After mechanical milling and alkali activation
processes, the MSWI fly ash can achieve the aim of detoxification and recovery, and can
be a good substitute of Type I ordinary Portland cement (OPC).
The crystal structure of MSWI fly ash was destroyed and became the amorphous
phase after milling 96 h. At the same time, the leaching concentration of the heavy metals
of milled fly ash could be decreased below the detection limit. The paste which partial
substituted the OPC by the milled fly ash would increase the amount of gel pores and
middle-size pores, and led the paste to become denser than OPC paste. The results of the
nuclear magnetic resonance Spectrometer (NMR) test indicated that the milled fly ash
can not only increase the amount of C-S-H gel which is caused by the higher hydration
reaction, but also can accelerate the pozzolanic reaction. Based on these results, the
compressive strength of the paste could rise up in all of the curing times.
By 0.2 M PO4
3- of milling solution and 1 h milling time, the calcium phosphate of
hydroxyapatite (HAp), tricalcium phosphate (TCP) and tetracalcium phosphate (TTCP)
would be produced. However, the dissolution of calcium phosphate compounds and
excessive PO4
3- remained in the milled ash, which made the calcium hydroxide of paste be
consumed. This result indicate that the milled fly ash by PO4
3- caused the negative impact
of the compressive strength of the milled fly ash paste greater than the positive impact,
and led the compressive strength lower than the OPC paste.
The milled fly ash with 0.002 M PO4
3- would produce a lot of TTCP when it partial
substituted OPC paste, which the TTCP would react with water to produce HAp and
calcium hydroxide. In addition, the effect of the pozzolanic reaction premature generated
by 96 h of milling time still appears and the compressive strength of the milled fly ash
paste after 7 days and 28 days of curing also higher than the OPC paste.
The effect of metakaolin and washed fly ash on a different mixing ratio by
mechanical milling activation (1 M NaOH , 24 h) was evaluated. The results show 1 M
NaOH of milling solution was lack of alkali concentration, thus it could not dissolute the
silicate of metakaolin. The compounds produced by metakaolin after mechanical milling
activation could conduct an ions exchange of heavy metal and achieve the stabilization of
heavy metal. When the alkali concentration increased to 5 M, heavy metal would bond
with the activated gel. Due to the bonding strength is weak, so the leaching concentration
of heavy metal was slightly increased. In addition, the high concentration of sodium
hydroxide would cause significant negative influence on the hydration reaction.
The milling activation was conducted in 5M of NaOH with the water treatment plant
sludge after calcination. The results show that the stabilized chloride crystallization would
be increased when the amount of the extracted fly ash was increased. Nevertheless, when
the amount of the extracted fly ash was decreased, the type of the bound with chloride ion
was the physical stability mechanism, which would lead to poor stability of the paste.
From above statement, the milled activated fly ash would form a gel of weak structure for
binding with chloride ion and was not conducive to stabilize chloride for the paste in the
early curing time. When the water was the milling solution, it would generate many
similar Friedel’s salt structure which caused the effect of observably chemical stability.
The excellent of the effect of stabilize chloride ion for the paste would be appeared after 7
days of curing. The stabilization and reaction mechanism of chloride ion in the inorganic
gel is difference with traditional cement evidently.

第一章	前言	1
1-1	研究緣起	1
1-2	研究架構	3
第二章	文獻回顧	5
2-1	焚化飛灰之介紹	5
2-1-1	焚化飛灰基本特性	5
2-1-1-1	物理組成	5
2-1-1-2	化學組成	6
2-1-2	焚化飛灰一般常見處理/處置方法	8
2-1-3	資源再生利用技術	11
2-2	機械力化學反應之介紹	13
2-2-1	機械合金技術之介紹	13
2-2-1-1	機械合金原理	14
2-2-1-2	機械合金之發展	16
2-2-2	機械化學反應之介紹	18
2-2-2-1	機械化學反應產生之原理	18
2-2-2-2	機械化學反應運作之過程	20
2-2-3	機械化學反應之應用	21
2-2-3-1	利用機械化學法製作高活性無晶序粉體	22
2-2-3-2	利用機械化學法提高水泥化學活性	22
2-2-3-3	機械化學於環境工程上的應用	24
2-3	水泥水化反應與化學反應原理	26
2-3-1	水泥熟料礦物的水化	26
2-3-1-1	C3S之水化	  30
2-3-1-2	C2S之水化	  32
2-3-1-3	C3A之水化	  33
2-3-1-4	C4AF之水化	37
2-3-2	波特蘭水泥之凝結與硬化過程	37
2-3-2-1	凝結與硬化對結構的改變	41
2-3-2-2	水化程度與強度之關係	48
2-3-2-3	卜作嵐反應	52
2-3-3	水泥與氯離子的反應	53
2-3-3-1	水泥結合氯離子之反應機制	54
2-3-3-2	氯離子穩定能力之影響因子	59
2-4	磷酸穩定重金屬	64
2-4-1	添加磷酸穩定重金屬之原理	64
2-4-2	磷酸與鈣離子之反應	65
2-5	無機聚合材料	67
2-5-1	無機聚合材料之聚合原理	67
2-5-2	無機聚合材料之發展與應用	70
2-5-2-1	原料－以含鈣化合物為主	70
2-5-2-2	C-S-H無機膠體的結構特性	72
2-5-2-3	C-S-H無機膠體成型的影響	73
2-5-2-4	無機聚合物於廢棄物資源再利用和處理的應用	73
第三章	研究方法	75
3-1	研究內容	75
3-2	實驗內容與步驟	78
3-2-1	焚化飛灰經由機械化學穩定處理對水泥漿體之影響	78
3-2-2	焚化飛灰以磷酸搭配研磨對重金屬穩定與水泥漿體之影響	83
3-2-3	利用研磨搭配鹼活化改質焚化飛灰提升水化膠體	88
3-2-4	改質焚化飛灰提升水化膠體對氯離子結合情況之探討	92
3-3	分析方法與檢測項目	96
3-3-1	焚化飛灰經由機械化學穩定處理對水泥漿體之影響	96
3-3-2	焚化飛灰以磷酸搭配研磨對重金屬穩定與水泥漿體之影響	103
3-3-3	利用研磨搭配鹼活化改質焚化飛灰提升水化膠體	106
3-3-4	改質焚化飛灰提升水化膠體對氯離子結合情況之探討	109
第四章	結果與討論	116
4-1	焚化飛灰基本物化性質	116
4-2	焚化飛灰經由機械化學穩定處理對水泥漿體之影響	120
4-2-1	研磨96小時對水萃灰粉體性質所造成之變化	        120
4-2-2	研磨灰取代市售水泥對水泥漿體微結構之影響	126
4-2-3	研磨灰取代市售水泥對水泥漿體工程性之影響	134
4-2-4	小結	137
4-3	焚化飛灰以磷酸搭配研磨對重金屬穩定與水泥漿體之影響	138
4-3-1	短時間研磨與長時間研磨對研磨水萃反應灰所造成的差異	138
4-3-2	以磷酸為研磨液對研磨水萃反應灰所造成的影響	143
4-3-3	經磷酸研磨後的研磨水萃反應灰取代部分市售水泥對水泥漿體造成之影響
                148
4-3-4	小結	160
4-4	利用研磨搭配鹼活化改質焚化飛灰提升水化膠體	161
4-4-1	不同偏高嶺土調配百分比所產製的活化粉之分析	161
4-4-2	不同鹼液濃度對研磨活化粉之影響	168
4-4-3	活化粉掺配於水泥漿體後對水泥漿體之影響	171
4-4-4	小結	176
4-5	改質焚化飛灰提升水化膠體對氯離子結合情況之探討	177
4-5-1	不同煆燒淨水污泥調配百分比對氯離子移動性之探討	177
4-5-2	不同鹼液濃度對研磨活化過程中氯鹽分佈之情況	185
4-5-3	小結	189
第五章	結論與建議	190
5-1	結論	190
5-2	建議	193
參考文獻                 195
圖目錄
Fig. 1- 1 本研究之架構圖	4
Fig. 2- 1焚化飛灰在兩種分散劑之下所測得的顆粒分佈圖	6
Fig. 2- 2焚化飛灰水洗前SEM圖	10
Fig. 2- 3焚化飛灰水洗後SEM圖	11
Fig. 2- 4機械合金法之原理	16
Fig. 2- 5機械合金的粉末粒徑與球磨時間之曲線圖	16
Fig. 2- 6於不同Ca(OH)2和Al2O3濃度之下的結晶產物	35
Fig. 2- 7水化初期(在初始的數小時或數天)的反應情況	38
Fig. 2- 8波特蘭水泥於不同水化時間之下的放熱速率曲線	41
Fig. 2- 9波特蘭水泥於水化過程中各種水化物的相對含量	42
Fig. 2- 10以CaO-SiO2-H2O系統圖描述水泥在25 oC之下之水化產物	45
Fig. 2- 11波特蘭水泥水化過程中，漿體溶液的pH值變化與C-S-H型態之關係圖	46
Fig. 2- 12純水泥熟料礦物之養護齡期對強度發展之趨勢	50
Fig. 2- 13以壓汞分析儀進行水泥漿體的孔隙特性分析	51
Fig. 2- 14 CaO-CaCl2-H2O三元系統相圖	57
Fig. 3- 1 本研究之研究流程圖	77
Fig. 3- 2「焚化飛灰經由機械化學穩定處理對水泥漿體之影響」之實驗流程圖	82
Fig. 3- 3 「焚化飛灰以磷酸搭配研磨對重金屬穩定與水泥漿體之影響」之實驗流程圖	87
Fig. 3- 4 「利用研磨搭配鹼活化改質焚化飛灰提升水化膠體」之實驗流程圖	91
Fig. 3- 5 「改質焚化飛灰提升水化膠體對氯離子結合情況之探討」之實驗流程圖	95
Fig. 3- 6 氯離子分佈關係圖	114
Fig. 3- 7 以活化粉取代市售水泥所製成之水泥漿體的氯離子分佈關係	115
Fig. 4- 1水萃灰(EA)與96小時研磨灰(MEA)與市售水泥(OPC)之粒徑分布圖	122
Fig. 4- 2經研磨處理前與研磨處理後的顯微結構(a)水萃灰、(b)96小時研磨灰	123
Fig. 4- 3水萃灰(EA)與96小時研磨灰(MEA)的XRD分析結果	124
Fig. 4- 4 OPC-EA 10%、OPC-MEA 10%、OPC三種水泥漿體 (W/B=0.38) 於 (a)養護28天、(b)養護7天之下的XRD分析結果	129
Fig. 4- 5 OPC-EA 10%、OPC-MEA 10%、OPC三種水泥漿體 (W/B=0.38) 於養護28天之29Si MAS-NMR分析結果	131
Fig. 4- 6 OPC-EA 10%、OPC-MEA 5%、OPC-EA 5%、OPC四種水泥漿體(W/B=0.38) 於養護28天之MIP分析結果	132
Fig. 4- 7 OPC-EA 10%、OPC-MEA 5%、OPC-EA 5%、OPC四種水泥漿體(W/B=0.38) 於養護28天內部膠體孔隙(<10 nm)與中毛細孔隙(10-100 nm)含量變化情況	133
Fig. 4- 8 OPC-EA 10%、OPC-MEA 5%、OPC三種取代比例之水泥漿體在不同養護時間、三種水膠比(a) 0.38、(b) 0.45、(c) 0.55之抗壓強度分析	136
Fig. 4- 9 以水為研磨液，水萃反應灰於不同研磨時間之下的粉體粒徑分布圖 (a)：體積分佈；(b)：累計體積分佈	140
Fig. 4- 10 以不同磷酸濃度為研磨液，於不同研磨時間下的研磨水萃反應灰之鉛的溶出率	144
Fig. 4- 11 以不同磷酸濃度為研磨液，研磨1小時後之XRD圖	146
Fig. 4- 12 不同磷酸研磨液濃度於研磨時間0.5小時、1小時、96小時之研磨水萃反應灰，取代10%市售水泥後製作水泥漿體，(a)：養護齡期為7天、(b)：養護齡期為28天之抗壓強度變化	149
Fig. 4- 13 不同磷酸研磨液濃度於研磨時間96小時研磨水萃反應灰，取代10%市售水泥之28天水泥漿體的TG/DTA分析((a)：TG圖、(b)：DTA圖)	150
Fig. 4- 14 不同原料配比進行研磨活化之活化粉XRD分析	166
Fig. 4- 15 不同原料配比進行研磨活化的活化粉之TCLP溶出液鉛濃度與粉體鉛溶出率	167
Fig. 4- 16 在高嶺土調配比50%之下，不同鹼液濃度所產製的活化粉之XRD分析	170
Fig. 4- 17 不同原料配比進行研磨活化的活化粉取代10%市售水泥製成漿體養護28天之抗壓強度	173
Fig. 4- 18 不同調配比活化粉取代10%市售水泥製成漿體養護28天之膠體含量分析	174
Fig. 4- 19以不同鹼液濃度活化後之活化粉取代10%市售水泥製成漿體養護28天之抗壓強度	175
Fig. 4- 20 不同煆燒淨水污泥調配百分比之氯離子分佈情況	181
Fig. 4- 21 不同煆燒淨水污泥調配百分比之活化粉XRD分析	182
Fig. 4- 22 不同煆燒淨水污泥調配百分比之活化粉FTIR分析	184
Fig. 4- 23 (a)70S/30A-5、(b) 70S/30A-1、(C) 70S-30A-0的氯離子分佈情況	187
Fig. 4- 24 不同鹼液濃度之活化粉XRD分析	188

 
表目錄
Table 2- 1機械合金的特色	17
Table 2- 2機械合金發展的重要里程碑	18
Table 2- 3本文所使用之水泥化學符號簡稱	28
Table 2- 4波特蘭水泥主要成分及說明	28
Table 2- 5各類型波特蘭水之各項要求	29
Table 2- 6 C3S各個反應階段的反應情況之描述	31
Table 2- 7幾種主要鋁酸鈣水化物整理	34
Table 2- 8波特蘭水泥中C3A與CaSO4水化反應之後產物	37
Table 2- 9常見的幾種水化物的反應熱	42
Table 2- 10常見Tobermorite之種類	47
Table 2- 11C-S-H漿體的各種結構的命名	48
Table 2- 12浸泡於鈉離子濃度550 mmol/L溶液中，白水泥與CaCl2結合之情況	62
Table 2- 13不同鈣/磷比之下所形成的磷酸鈣鹽之種類	66
Table 3- 1本階段之水泥漿體製作取代配比	81
Table 3- 2本階段各項樣品與實驗條件之對照表	85
Table 3- 3 本階段各項樣品與實驗條件之對照表(a)不同調配百分比、(b)不同氫氧化鈉濃度	90
Table 3- 4 本階段各項樣品與實驗條件之對照表(a)不同調配百分比、(b)不同氫氧化鈉濃度	94
Table 3- 5 矽酸鹽四面體之聚合單體之結構	102
Table 3- 6 固態物質中常見的IR訊號	108
Table 4- 1 近3年鍋爐灰(BA)、反應灰(RA)、水萃反應灰(ERA)、市售水泥之一般元素分析	118
Table 4- 2 近3年鍋爐灰(BA)、反應灰(RA)、水萃反應灰(ERA)、市售水泥(OPC)之重金屬成份分析	118
Table 4- 3 近3年鍋爐灰(BA)、反應灰(RA)、水萃反應灰(ERA)之TCLP試驗結果	119
Table 4- 4 鍋爐灰(BA)、反應灰(RA)、水萃反應灰(ERA)之物理性質分析	119
Table 4- 5不同研磨時間之下的研磨灰的比表面積	124
Table 4- 6水萃灰、攪拌灰、研磨灰、市售水泥之重金屬成份	125
Table 4- 7攪拌灰、研磨灰TCLP結果	125
Table 4- 8 OPC-EA 10%、OPC-MEA 10%、OPC三種水泥漿體 (W/B=0.38) 於養護7天和28天的XRD分析中氫氧化鈣特徵峰半高寬積分結果	130
Table 4- 9不同取代條件之下，4種水膠比對漿體凝結時間之變化	137
Table 4- 10 以不同磷酸濃度為研磨液、不同研磨時間之下研磨水萃反應灰之TCLP結果	142
Table 4- 11 以XRD分析不同磷酸濃度為研磨液與不同研磨時間之研磨水萃反應灰中所含的主要結晶成分	147
Table 4- 12 不同磷酸研磨液濃度於研磨時間96 小時之研磨水萃反應灰，取代10%市售水泥之7天、28天水泥漿體內部氫氧化鈣的含量及其變化計算值	155
Table 4- 13不同原料配比進行研磨活化的活化粉之活化度	166
Table 4- 14 在高嶺土調配比50%之下，不同鹼液濃度所產製的活化粉之TCLP結果	170
Table 4- 15 結合氯離子和自由氯離子佔原料的百分比	181
Table 4- 16 不同煆燒淨水污泥調配百分比取代市售水泥之水泥漿體的氯離子分佈及相對抗壓強度分析	184
Table 4- 17 不同鹼液濃度之活化粉取代市售水泥之水泥漿體的氯離子分佈及相對抗壓強度分析	188

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