污泥及含氯灰渣燒製環保水泥之研究

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張博荏(Po-jen Chang) 查詢紙本館藏

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論文名稱

污泥及含氯灰渣燒製環保水泥之研究
(Production of eco-cement by using sludge and incinerator ash)

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摘要(中)

本研究將以焚化灰渣、大理石污泥、下水污泥進行環保水泥之燒製，尤其對高氯含量之灰渣，除預先除氯外，亦考慮在燒製過程嘗試使其形成氯鋁酸鈣固定與熟料中，而成為環保水泥之一部分，以解決氯鹽之干擾。
原料前處理研磨後，利用水泥配料係數計算配比之環保水泥生料，再以實驗室高溫爐燒結處理，燒成兩系列六組不同配比之環保水泥熟料，進行各項物化特性分析以及工程性質與水化反應行為之探討。實驗結果如下：實驗燒製之兩系列六組環保水泥熟料，其游離石灰量皆小於1，且製程燒失量介於25% -30%間，符合實廠窯燒水泥之品管規範。其重金屬溶出濃度均符合法規標準值，後續資源化利用作為土木工程材料深具潛力。研究中所燒製各組環保水泥熟料與波特蘭水泥成份類似，其單礦物組成除了含有C3S、C2S、C3A及C4AF，還有環保水泥特有的C11A7CaCl2等晶相物種。OEC系列環保水
泥漿體部分初終凝時間與OPC比較有略微的提早的現象，但差異並不大且也符合規範；REC系列環保水泥漿體部分初終凝時間明顯的提前許多。環保水泥漿體抗壓部分跟初終凝有正向的關係，在OEC系列環保水泥漿體與OPC強度發展類似，而REC系列環保水泥漿體則有早強的現象發生，這也是含氯環保水泥的特性。由XRD之物種分析得知，環保水泥漿體主要產物為CH、C-S-H膠體，並無明顯差異。此外，環保水泥漿體會產生部分之Mg(OH)2，這是利用大理石污泥取代石灰石的原因。由FTIR分析結果顯示，隨齡期發展均可發現，環保水泥漿體矽酸鈣水化產物C-S-H膠體則具有強的Si-O伸縮振動頻帶；碳酸鹽物種為C-O鍵結；此外，CH為-OH伸縮振動頻帶。由核磁共振(NMR)
技術以29Si為核種進行分析結果顯示，環保水泥漿體之水化產物Q0 峰會隨齡期增加逐漸轉移至Q1與Q2峰，且水化程度與聚矽陰離子皆有隨齡期而增加之趨勢。

摘要(英)

The high chlorine content in the incinerator ash has limited the use of it as part of the raw material for producing ecocement. It is possible, however, to
calcine chlorine-containing raw meal into calcium chloroaluminate, one cement hydrate mineral, which can not only fix the chlorine in it but also function just
like the other cement clinker minerals. This study investigated the feasibility of producing ecocement, using chlorine-containing incinerator ash, marble sludge,
and sewage sludge as raw materials, and the hydration characteristics of the resulting cement clinkers.
In the design of the raw materials incorporated the tested wastes, a computational model was established on the basis of cement modulus to formulate possible range of the compositions of raw meals with tested chlorine contents in the raw materials verifying from 1.5-37.8 %(w/w). The calcination of raw materials into cement clinker minerals were examined and the hydration characteristics of the resultant ecocements and the engineering properties of their pastes were studied including the compressive strength, speciation and the degree of hydration, as compared to those of ASTM type I ordinary Portland cement
(OPC).In this study, the amount of free CaO decreased to less than 1 %(w/w) and the LOI for all tested meals met the eco-cement criteria. In conclusion, the formation of major cement clinker minerals such as C3S, C2S, C3A, C4AF and C11A7CaCl2 were confirmed in all the eco clinkers.
Ecocement produced with was washed incinerator ash, marble sludge, and sewage sludge as raw meal (referred to as ordinary ecocement, OEC) showed both the initial and the final setting times were slightly shortened or similar to
those of OPC. However, ecocement produced using chlorine-containing incinerator ash, marble sludge, and sewage sludge as raw meal (referred to as chlorine-containing ecocement, REC) exhibited both the initial and the final
setting times were significantly shortened with the increasing chlorine content in the RECs.
On the other hand, the compressive strength development of OEC samples showed slightly decreased as compared to that of OPC samples, whereas the REC samples showed a reversed trend. The development of compressive strength
outperformed those of OPC samples during the early 28 days, showing the contribution by the hydration of the C11A7CaCl2 which characterizes the rapid setting and strength development of the REC samples.
The results of XRD analysis confirmed that OPC, OEC and REC showed common hydration products of CH and CSH gel, the OEC and REC exhibited the presence of hydration product, (Mg(OH)2), which were supposed contributed by
the use of marble sludge in the raw meals.
The FTIR analysis of the OEC and REC pastes cured at 90 days containes three wavenumbers: the first wavenumber was mainly due to the Si-O bonds of calcium silicate hydrates (CSH); the second wavelength represents the C-O
bonds of the calcium carbonate (CaCO3); and the third wavelength the decomposition of calcium hydroxide (Ca(OH)2). The results indicate the hydration products of the tested OEC and REC samples. The hydration products of both OEC and REC pastes, as analyzed by 29Si
NMR techniques showed that Q0 peak decreased and O1 peake increased with increasing curing age. And the hydration degree and length of the linear polysilicate anions, as estimated on the basis of the Q0 and Q1 peaks, showed the
increasing trend with increasing age.

關鍵字(中)

★ 灰渣
★ 氯鹽
★ 氯鋁酸鈣
★ 環保水泥

關鍵字(英)

★ eco-cement
★ calcium chloroaluminate
★ chlorides
★ incinerator ash

論文目次

第一章前言1
1-1 研究緣起1
1-2 研究目的2
第二章文獻回顧3
2-1 都市垃圾焚化灰渣來源及特性3
2-1-1 都市垃圾焚化灰渣來源及產量3
2-1-2 灰渣特性5
2-1-2-1 飛灰之物化性質6
2-1-2-2 洗滌灰之物化性質8
2-2 大理石污泥來源及特性9
2-2-1 大理石污泥來源及產量9
2-2-2 大理石污泥之物化性質12
2-3 下水污泥來源及特性13
2-3-1 下水污泥來源及產量13
2-3-2 下水污泥之物化性質14
2-4 水泥之製程16
2-4-1 水泥原料及生產過程16
2-4-2 水泥配料係數19
2-4-3 水泥燒製反應與影響因子24
2-4-4 水泥品保規範27
2-5 水泥之物化特性與微觀結構30
2-5-1 水泥水化反應機制30
2-5-2 水泥MgO 系統34
2-5-3 水泥漿體微觀結構36
2-6 環保水泥39
2-6-1 環保水泥概要39
2-6-1 環保水泥物化特性44
2-6-3 環保水泥之水化特性47
2-6-4 不純物對水泥燒製之影響48
第三章實驗材料與方法52
3-1 實驗流程52
3-2 實驗材料56
3-3 實驗配置57
3-3-1 實驗燒製條件之配置57
3-3-2 各組環保水泥之配比設計59
3-3-3 環保水泥漿體試驗條件配置60
3-4 實驗設備與方法60
3-4-1 實驗設備與方法60
3-4-2 分析方法63
第四章結果與討論77
4-1 水泥生料基本性質分析77
4-1-1 水泥生料之物化特性77
4-1-2 水泥生料之物種型態82
4-1-3 水泥生料之重金屬總量與TCLP試驗85
4-2 生料配比與燒製方法86
4-2-1 生料配比設計結果86
4-2-2 生料燒制條件89
4-3 水泥熟料之基本性質分析91
4-3-1 熟料之物化性質91
4-3-2 熟料之物種型態92
4-3-2-1 XRD 物種分析92
4-3-2-2FTIR 化學鍵結分析95
4-3-3 熟料之重金屬總量與TCLP 試驗96
4-3-4 環保水泥熟料之SEM 結構分析97
4-4 水泥規範品管檢驗分析99
4-4-1 化學成份規定99
4-4-1-1 化學組成99
4-1-1-2 燒失量100
4-1-1-3 游離石灰量(f-CaO)100
4-4-2 物理性質規定102
4-4-2-1 細度102
4-4-2-2 抗壓強度102
4-4-2-3 凝結時間102
4-4-2-4 製程燒失量103
4-5 環保水泥漿體之巨觀分析104
4-5-1 凝結行為104
4-5-2 抗壓強度發展105
4-6 環保水泥漿體水化產物之分析108
4-6-1 環保水泥漿體XRD 分析108
4-6-2 環保水泥漿體DTA/TGA 分析114
4-6-3 環保水泥漿體FTIR 分析122
4-7 環保水泥漿體孔隙結構分析125
4-8 環保水泥漿體NMR 分析131
4-8-1 環保水泥漿體特徵峰變化131
4-8-2 環保水泥漿體水化程度變化與聚矽陰離子長度變化140
4-9 環保水泥漿體之SEM 觀察142
4-10 綜合討論147
第五章結論與建議149
5-1 結論149
5-2 建議152
參考文獻153

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指導教授

王鯤生(Kuen-sheng Wang)

審核日期

2009-10-18

推文