本研究首先針對台灣地區都市垃圾焚化爐煙道排氣中含汞污染物之濃度進行量測，並結合廢棄物資源回收再生利用之觀念，利用廢輪胎熱裂解產物碳黑製備粉狀活性碳，並進行加硫改質，最後以自製之粉狀活性碳進行氣相氯化汞之管柱吸附實驗，俾做為都市垃圾焚化爐操作之重要參考。
都市垃圾焚化爐煙道排氣中含汞污染物之現場採樣與分析結果顯示，四座都市垃圾焚化爐排氣中粒狀物、含汞污染物及其他重金屬之排放濃度均合乎法規排放標準。除含汞污染物外，其他重金屬皆可達到90%以上的去除效率。A、B、C及D四廠之含汞污染物去除效率分別為83.71%及81.51%、96.22%及87.18%，顯示於煙道中噴入活性碳確實有助於含汞污染物之去除，而氧化態含汞污染物較元素態含汞污染物更容易被去除。
就廢輪胎熱裂解產物製備活性碳之影響因素而言，廢輪胎之熱裂解溫度約為400~500℃，殘餘固體之生成百分比約介於35%~37%之間；而氣體與胎油之生成則呈相互消長之現象。就熱裂解溫度而言，提高熱裂解溫度有助於碳黑孔隙的發展。此外，隨著注水速率與活化時間的增加，活性碳產率呈現逐漸減少之趨勢，但有助於活性碳孔隙的發展。而活性碳加硫改質之實驗結果顯示，加硫改質會造成活性碳比表面積的大幅減少，因此在進行加硫改質時，必須考量活性碳含硫量與比表面積之平衡。
本研究進一步以自行製備之粉狀活性碳進行氣相氯化汞管柱吸附實驗，其實驗結果顯示，在室溫（25℃）吸附條件下，活性碳之比表面積愈高者，其所需之飽和吸附時間較長，吸附效果較佳，吸附量亦隨著活性碳的比表面積增加而增加。在室溫之吸附條件下，硫化改質會降低活性碳的比表面積，導致活性碳吸附效率之降低；而比較兩種比表面積相近之活性碳，以含硫量高者吸附效果較佳，顯示增加活性碳中的含硫量對於吸附氣相氯化汞仍有所助益。在較高吸附溫度（150℃）下，活性碳之吸附容量隨著活性碳含硫量之增加而提昇。在室溫吸附條件下，活性碳吸附氣相氯化汞係以物理吸附為主，而在較高的操作溫度下，則以化學吸附較為重要。此外，在室溫之吸附條件下，自製之粉狀活性碳與焚化爐實際使用之商用粉狀活性碳之氯化汞吸附能力極為相似，而於150℃之吸附條件下，其吸附容量高於商用粉狀活性碳，此結果顯示本研究自行製備之粉狀活性碳亦可達到實廠使用活性碳的吸附水準。

The objective of this study was to remove mercury vapor from municipal waste incinerator (MWI) by the adsorption of powder activated carbon (PAC) prepared from the pyrolysis of waste tire. The study focused on the measurement of mercury concentration in flue gas emitted from municipal waste incinerator, the preparation of PAC from the pyrolysis of the waste tire and impregnated with sulfur, and the adsorption capacity of mercury by the self-made PAC.
The measurement of heavy metals in flue gas emitted from four typical MWIs was conducted in this study. Experimental results obtained from the measurement of mercury from flue gas indicated that the removal efficiency of mercury ranged from 83.71%~96.22%for the tested MWIs. This study revealed that the injection of PAC in flue gas would enhance the removal efficiency of mercury. Besides, oxided mercury (Hg2+) can be removed much more easily than elemental mercury (Hg0).
Experimental results obtained from the pyrolysis of waste tires indicated that the pyrolysis temperature of waste tire was approximately 400~500℃, and the percentage of carbon residue is 35~37%. With higher temperature and water feed rate and longer activation time, the specific surface area and total pore volume of PAC increased while the average pore radius decreased. The highest specific surface area of PAC obtained in this study was 996 m2/g. In addition, experimental results obtained from sulfur impregnation process indicated that the specific surface area of PAC decreased dramatically as sulfur was added to PAC.
Experiment results obtained from the adsorption capacity of HgCl2 on PAC by column test indicated that PAC with higher specific surface area could adsorb more HgCl2 at room temperature (25℃). The adsorption capacity of sulfur impregnated PAC decreased at 25℃ was due to the decrease of specific surface area of PAC. However, results from the comparison of two PAC with similar specific surface area indicated that the PAC with higher sulfur content had higher adsorption capacity. It suggested that the addition of sulfur to PAC could enhance the adsorption of HgCl2 at 25℃. Experimental results obtained from column tests at 150℃ showed that the adsorption capacity of PAC increased as sulfur content of PAC increased. These results suggested that the adsorption mechanism of HgCl2 by PAC was mainly physical adsorption at lower temperature and it was chemisorption at higher temperature. Besides, the self-made PAC demonstrated the similar adsorption capacity of HgCl2 with commercial PAC used in MWIs.

謝誌
摘要
英文摘要
目錄
表目錄
圖目錄
第一章 前言
1-1 研究緣起
1-2 研究目的
1-3 研究流程
第二章 文獻回顧
2-1 汞之物化特性及影響
2-1-1汞之物理化學特性
2-1-2汞對人體健康之影響
2-2 都市垃圾焚化爐排氣中含汞污染物之來源及種類
2-2-1含汞污染物之來源
2-2-2含汞污染物之物種型態
2-3 都市焚化爐排氣中含汞污染物之控制技術及去除機制
2-3-1含汞污染物之補集機制與控制技術
2-3-2活性碳噴入設備
2-4 活性碳之種類、特性與應用
2-4-1活性碳之種類
2-4-2活性碳之特性
2-4-3活性碳在污染防治之應用
2-5 活性碳之製備方式
2-5-1物理活化
2-5-2化學活化
2-6 廢輪胎之組成與特性
2-7 廢輪胎之環境問題與處理技術
2-7-1國內外廢輪胎之環境問題
2-7-2國內外廢輪胎之處理技術
2-8 熱裂解原理、應用與特性
2-8-1熱裂解之原理
2-8-2影響熱裂解之操作條件
2-8-3廢輪胎熱裂解之產物成份
2-9 活性碳改質對吸附汞蒸氣的影響
第三章 研究方法
3-1 實驗設計與流程
3-2 都市垃圾焚化爐排氣中含汞污染物之現場煙囪量測
3-2-1實驗設備
3-2-2採樣流程
3-2-2-1煙道採樣方法
3-2-2-2煙道採樣前準備工作
3-2-2-3煙道採樣步驟
3-2-3樣品前處理與分析
3-2-3-1樣品前處理
3-2-3-2樣品分析
3-3 粉狀活性碳之製備與氣相氯化汞管柱吸附實驗
3-3-1實驗設計與流程
3-3-2實驗設備
3-3-2-1廢輪胎熱裂解系統
3-3-2-2活性碳製備系統
3-3-2-3活性碳硫化改質系統
3-3-2-4氣相氯化汞管柱吸附系統
3-3-2-5分析系統
3-3-3實驗方法
3-3-3-1廢輪胎熱裂解及碳黑活化反應
3-3-3-2活性碳硫化改質
3-3-3-3氣相氯化汞管柱吸附實驗
3-3-4分析方法
3-4 品保與品管
3-4-1煙道採樣之品保品管
3-4-1-1採樣前準備工作
3-4-1-2現場採樣品管查核
3-4-2實驗室分析品保品管
3-4-2-1實驗室可信度要素
3-4-2-2數據品保工作項目及執行方式
第四章 結果與討論
4-1 都市垃圾焚化爐煙道採樣工作
4-1-1煙道廢氣主要組成之分析
4-1-2都市垃圾焚化爐排氣中粒狀物濃度
4-1-3都市垃圾焚化爐煙道排氣中重金屬濃度
4-1-3-1煙道排氣中含汞污染物及重金屬之濃度
4-1-3-2煙道氣中氧化態與元素態含汞污染物之分佈
4-2 操作條件對廢輪胎熱裂解及碳黑活化之影響
4-2-1加熱溫度對廢輪胎熱裂解之影響
4-2-1-1產物生成百分比
4-2-1-2固態產物碳黑之元素分析
4-2-1-3固態產物碳黑微孔隙分析
4-2-2活化操作條件對活性碳物理性質之影響
4-2-2-1注水速率對碳黑活化之影響
4-2-2-2活化時間對碳黑活化之影響
4-3 粉狀活性碳之硫化改質
4-3-1改質含硫量對活性碳比表面積之影響
4-3-2硫份增加量對活性碳比表面積之影響
4-4 氣相氯化汞管柱吸附測試結果
4-4-1活性碳之比表面積對吸附氣相氯化汞之影響
4-4-2活性碳含硫量對吸附氣相氯化汞之影響
4-4-3自製與實廠使用粉狀活性碳之比較
第五章 結論與建議
5-1 結論
5-2 建議
參考文獻
附錄 A 採樣儀器校正紀錄
附錄 B 汞之檢量線
附錄 C ICP-MS校正曲線
附錄 D 元素分析圖例
附錄 E 蠕動幫浦校正曲線
附錄 F 實驗結果一覽表

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