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姓名	蕭毓撰(Yu-Chuan Hsiao)  查詢紙本館藏	畢業系所	環境工程研究所
論文名稱	加速碳酸鹽反應對都市垃圾焚化灰渣捕捉二氧化碳之可行性評估研究 (Feasibility of Carbon Dioxide Capture by using Accelerated Carbonation of Municipal Solid Waste Incineration (MSWI) Residues)
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摘要(中)	本研究應用自行開發之半乾式旋轉窯加速碳酸鹽反應系統，探討都市垃圾焚化飛灰及底渣無害化及捕捉二氧化碳之可行性，研究分別針對二氧化碳的捕捉效率、加速碳酸鹽反應前後焚化飛灰之重金屬溶出特性、酸中和能力，以及後續水泥穩定化作業之水泥添加量之影響等進行評估。加速碳酸鹽反應系統控制條件，主要包括模擬焚化廢氣組成之二氧化碳(10 %)、二氧化硫(15及30 ppm)及反應系統的濕度(20 %及30 %)。研究結果顯示不論是焚化底渣或飛灰，控制前述之反應條件，反應均可在8小時左右，達成加速碳酸鹽礦化反應之效果(pH<9)。反應系統濕度對焚化灰渣捕捉二氧化碳效率的評估結果顯示，反應濕度較高(30 %)易造成阻塞灰渣孔隙，不利於二氧化碳於孔隙間的氣體流通性，致使二氧化碳捕捉量較反應濕度20 %為低，其中焚化飛灰及底渣對二氧化碳捕捉量分別從29.66 g/kg及77.73 g/kg降低至27.46 g/kg及66.37 g/kg。此外，焚化底渣對二氧化碳的捕捉量均較焚化飛灰為高，此係焚化底渣在反應系統之填充比較低，亦即孔隙率較高，因此，二氧化碳擴散性與底渣接觸反應的效果較佳。二氧化硫對二氧化碳捕捉量的競爭影響結果顯示，在廢氣含有較高濃度之二氧化硫(30 ppm)條件下，焚化飛灰或底渣之鈣含量將與二氧化硫反應並消耗，致使二氧化碳的捕捉量明顯降低。以10 %二氧化碳及反應濕度20 %的反應條件而言，當二氧化硫濃度從0 ppm增加至30 ppm時，焚化飛灰及底渣捕捉二氧化碳量，分別從29.66 g/kg及77.73 g/kg降低至23.79 g/kg及64.17 g/kg。 經加速碳酸鹽反應後飛灰及底渣之環境安全性評估結果顯示，反應後之焚化飛灰及底渣，其試驗重金屬之溶出濃度，均可符合法規管制標準，其中焚化飛灰中重金屬鉛之溶出濃度，可由反應前之4.12 mg/l降低至反應後之0.16 mg/l以下，足見加速碳酸鹽反應對飛灰中重金屬鉛之溶出，具有穩定化之效果。加速碳酸鹽反應對焚化飛灰水泥穩定化作業，水泥使用減量之評估結果顯示，在達到飛灰穩定化物相同之抗壓強度標準之條件下，經碳酸鹽反應後之飛灰，其水泥使用量約可減少20 %。整體而言，本研究已成功開發一套具有加速碳酸鹽礦化的反應系統，不僅驗證焚化飛灰及底渣均具捕捉二氧化碳之應用潛力外，同時亦可有效減少飛灰穩定化作業的水泥使用量，達成資源減量、飛灰無害化及二氧化碳捕捉的多重效果。
摘要(英)	The accelerated carbonation system combined with semi-dry rotary kiln was developed and investigated the feasibility of the carbon dioxide capture and non-hazardous treatment of municipal solid waste incineration (MSWI) fly ash and bottom ash. The carbon dioxide capture efficiency, the tested metals leaching characteristics and acid neutralization capacity of MSWI fly ash and bottom ash after accelerated carbonation reaction, , and reduction in cement usage by stabilization were discussed, respectively. The experimental results showed that pH value of MSWI fly ash and bottom ash could significantly decrease from 12 to 9 and below by accelerated carbonation during 8 hours reaction time. It is implied MSWI fly ash and bottom ash have matched criteria of carbonation reaction. In the case of moisture content effect on carbon dioxide capture efficiency, the carbon dioxide was captured by MSWI fly ash and bottom ash were decreased from 29.66 g/kg and 77.73 g/kg to 27.46 g/kg and 66.37 g/kg with moisture content increasing from 20 % to 30 %, respectively. This is because higher moisture content of ash could tend to block the pores of fly ash resulted in decreasing diffusion of carbon dioxide. On the other hand, due to the filling ratio of MSWI bottom ash in carbonation system was lower than that of fly ash, it can have a higher porosity and good diffusion of carbon dioxide resulted in MSWI bottom ash exhibits good carbon dioxide capture efficiency than that of MSWI fly ash. The presence of sulfur dioxide (SO2) could occur a competitive reaction during accelerated carbonation process. The experimental results indicated carbon dioxide was captured by MSWI fly ash and bottom ash were decreased from 29.66 g/kg and 77.73 g/kg to 23.79 g/kg and 64.17 g/kg with sulfur dioxide concentration increasing from 0 ppm to 30 ppm, respectively. That is, the sulfur dioxide could competitively react and consume the calcium content of fly ash and/or bottom ash resulted in decreasing carbon dioxide capture efficiency. Based on the analysis results of environmental safety of MSWI fly ash and bottom ash by accelerated carbonation, the all tested heavy metals of carbonated fly ash and bottom ash were in compliance with current Taiwan EPA regulation thresholds. In the case of variation in Pb TCLP concentration of fly ash, it was significantly decreased from 4.12 mg/l to 0.16 mg/l and below after accelerated carbonation reaction. It could conclude that the accelerated carbonation has good potential for enhancing in Pb stabilization of MSWI fly ash. According to the results of compressive strength of stabilization product using fly ash before and after carbonation treatment, it was shown that the cement usage amounts for MSWI fly ash stabilization after carbonation could approximately reduce 20 % under controlled at the similar requirement of compressive strength of stabilization product. In summary, this research has been successfully developed and proven the performances of accelerated carbonation reaction system combined with semi-dry rotary kiln. It could have good potential for carbon dioxide sequestration, but also could reduce the cement usage amounts in MSWI fly ash stabilization. The multiple purposes of resources reduction, harmless of MSWI fly ash, and carbon dioxide sequestration by accelerated carbonation have been conducted in this research.
關鍵字(中)	★ 焚化飛灰 ★ 焚化底渣 ★ 加速碳酸鹽反應 ★ 二氧化碳捕捉	關鍵字(英)	★ MSWI fly ash ★ MSWI bottom ash ★ accelerated carbonation ★ carbon dioxide capture
論文目次	摘要 i Abstract iii 誌謝 v 目錄 vii 圖目錄 xi 表目錄 xiii 第一章 前言 1 第二章 文獻回顧 5 2-1 焚化飛灰及底渣處理再利用現況 5 2-1-1 國內外焚化飛灰和底渣處理及再利用現況 5 2-1-2 國內外焚化飛灰及底渣重金屬溶出及總量濃度 8 2-2 碳酸鹽礦化反應之影響參數 10 2-2-1 碳酸鹽礦化反應之原理 10 2-2-2 廢棄物特性對碳酸鹽反應影響 13 2-2-3 二氧化碳濃度對碳酸鹽反應影響 15 2-2-4 溫/濕度對碳酸鹽反應影響 17 2-3 碳酸鹽礦化反應之技術 19 2-3-1 自然碳酸鹽礦化 20 2-3-2 加速碳酸鹽礦化 21 2-4 碳酸鹽礦化反應後對於焚化飛灰及底渣影響 22 2-4-1 碳酸鹽礦化反應後對於基本性質影響 22 2-4-2 碳酸鹽礦化反應後對於重金屬溶出影響 24 2-4-3 碳酸鹽礦化反應後對於二氧化碳捕捉影響 27 2-5二氧化硫對於碳酸鹽礦化反應之競爭作用 28 第三章 研究材料與方法 31 3-1 研究材料 31 3-2 研究方法及實驗條件 33 3-2-1 加速碳酸鹽礦化反應試驗條件 34 3-2-2 加速碳酸鹽礦化反應設備 36 3-2-3 水泥穩定化及其減量評估之試驗條件 38 3-3 分析項目與方法 39 3-3-1 分析儀器 39 3-3-2 分析方法 41 第四章 結果與討論 47 4-1 研究材料基本性質分析 47 4-1-1 焚化飛灰及底渣基本性質分析結果 47 4-1-2 焚化飛灰及底渣戴奧辛特性 61 4-2 碳酸鹽礦化後焚化飛灰及底渣性質分析結果 75 4-2-1 碳酸鹽礦化反應後焚化飛灰之基本特性變化 75 4-2-2 碳酸鹽礦化反應後焚化底渣之基本特性之變化 82 4-3 碳酸鹽礦化反應對焚化灰渣二氧化碳捕捉之評估 90 4-3-1 碳酸鹽礦化反應後焚化飛灰二氧化碳捕捉之評估 92 4-3-2 碳酸鹽礦化反應後焚化底渣二氧化碳捕捉之評估 93 4-3-3 焚化飛灰及底渣二氧化碳捕捉率及氧化鈣化轉換率結果 95 4-3-4 碳酸鹽礦化反應指標及速率 101 4-4 碳酸鹽礦化焚化飛灰及底渣環境安全性評估 112 4-4-1 碳酸鹽礦化後對焚化飛灰及底渣重金屬穩定性評估 112 4-4-2 酸中和能力及不同pH之金屬溶出情況 117 4-5 碳酸鹽礦化對焚化飛灰及底渣戴奧辛影響 124 4-5-1 碳酸鹽礦化後對戴奧辛影響 125 4-5-2 碳酸鹽礦化後對PCDD/Fs質量與毒性當量濃度之物種分布 127 4-6 碳酸鹽反應後焚化飛灰水泥穩定化評估 136 4-6-1 水泥添加比例對抗壓強度影響 137 4-6-2 含水率對抗壓強度影響 138 4-6-3 碳酸鹽礦化反應對於水泥穩定化程序減量評估 140 4-6-4 碳酸鹽礦化後對焚化飛灰水泥穩定化重金屬溶出影響 141 4-7 半乾式旋轉窯加速碳酸鹽礦化系統評估 144 第五章 結論與建議 147 5-1 結論 147 5-2建議 148 參考文獻 151
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指導教授	江康鈺(Kung-Yuh Chiang)	審核日期	2018-1-26
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