以觸媒催化分解戴奧辛於實廠與小型模廠之研究

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葉智偉(Chi-Wei Yeh) 查詢紙本館藏

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論文名稱

以觸媒催化分解戴奧辛於實廠與小型模廠之研究
(Evaluation of PCDD/F Decomposition over SCR Catalyst and Activated Carbon-Supported Catalysts)

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摘要(中)

SCR早期應用在NOx之去除，後來才應用在戴奧辛之去除，利用觸媒技術對戴奧辛破壞分解已成為現今控制戴奧辛排放之主要技術。本研究分成實廠與模廠測試部份進行探討，實廠部份針對國內現有ＳＣＲ場址，對戴奧辛之排放控制採樣與調查，模廠測試部份將採用觸媒(Cu/C、Fe/C、Cu-Fe/C)進行測試，探討觸媒於不同操作條件對戴奧辛催化分解能力。
實廠部分初步結果顯示金屬冶煉廠SCR對氣相戴奧辛的去除率66%，對PCDD與PCDF之去除率分別約為67.3%與 65.4%。在垃圾焚化廠方面，該廠SCR對氣相戴奧辛的去除率約為96.9%，對PCDD與PCDF之去除率分別為96.0%與 95.8%。垃圾焚化廠蜂巢狀V2O5/WO3/TiO2觸媒表面積(870 m2/m3)遠大於金屬冶煉廠平板狀V2O5/WO3/TiO2觸媒表面積(320 m2/m3) ，所以造成煙道氣流中戴奧辛與觸媒接觸頻率較高而予以催化分解，導致垃圾焚化廠對氣相戴奧辛有較佳之去除效率。
模廠部份在金屬冶煉廠煙道氣測試結果顯示，在不同溫度下(150℃、200℃、250℃)就觸媒對戴奧辛去除效率而言，三種觸媒(Cu/C、Fe/C與Cu-Fe/C)對戴奧辛的去除效率約達95 ﹪以上。就觸媒對戴奧辛破壞效率而言，在150℃時三種觸媒對戴奧辛之破壞效率約為20~30﹪，然而隨溫度的升高，Fe/C與Cu-Fe/C觸媒對戴奧辛之破壞效率越好，當在250℃時，Fe/C觸媒對戴奧辛之破壞效率高達78 ﹪。在垃圾焚化廠煙道氣測試方面，在不同溫度下(150℃、200℃、250℃)就觸媒對戴奧辛去除效率而言，二種觸媒(Cu/C與Fe/C)對戴奧辛的去除效率約達90 ﹪以上。就觸媒對戴奧辛破壞效率而言，在150℃時觸媒之破壞效率約為30~40 ﹪，然而隨溫度的升高，Fe/C觸媒在200℃時對戴奧辛之破壞效率達66 ﹪，當在250℃時對戴奧辛之破壞效率降為57 ﹪。
在金屬冶煉廠煙道氣測試時使用Cu/C觸媒於200℃與250℃時與Cu-Fe/C觸媒於250℃時，觸媒上皆有戴奧辛生成現象產生，在進流組成不同之垃圾焚化廠煙道氣測試，Cu/C觸媒於250℃時，觸媒上有戴奧辛生成現象產生，顯示觸媒上含有Cu催化金屬和Fe催化金屬相較之下，含有Cu催化金屬利於戴奧辛之再生成發生，然而在200℃時於金屬冶煉廠煙道氣測試，Cu-Fe/C觸媒中也含有Cu催化金屬，但並未見明顯生成，可能和Cu催化金屬含量多寡及操作溫度有關。

摘要(英)

SCR was mainly applied to removal of NOx as initially developed and now it has been used to abate dioxin emissions as well. Presently, abatement of dioxin using catalysis has become the mainstream technology. This study can be divided into two parts including field tests and pilot-scale system tests. The former focuses on sampling and investigating the control of dioxin emissions for existing SCR devices. The latter utilized several kinds of activated carbon-supported catalysts (Cu/C, Fe/C and Cu-Fe/C) to evaluate the feasibility of removing dioxins.
Regarding the tests conducted in field, the results showed that removal efficiency of gas-phase dioxin achieved with SCR at metal smelting factory was 66% while that of PCDD and PCDF were 67.6% and 65.4%, respectively. For the MSWI, the SCR could remove 95% of gas-phase dioxin, in which 96% of PCDD and 97% of PCDF were removed. The surface area of the honeycomb-type V2O5/WO3/TiO2 catalyst (870m2/m3) adopted by MSWI is much higher than that of plate-type V2O5/WO3/TiO2 catalyst (320 m2/m3) utilized by metal smelting factory, resulting in the higher removal efficiency obtained in MSWI.
The source of pilot-scale system sampling in metal smelting factory conducted the removal efficiencies achieved by utilizing Cu/C, Fe/C and Cu-Fe/C catalysts were as high as 95%. As for source of pilot-scale system sampling in the MSWI, the removal efficiencies achieved with Cu/C and Fe/C catalysts were more than 90%.
In the metal smelting factory, the destruction efficiencies of three catalysts at 150℃ were about 20-30%. However, the destruction efficiencies obtained with Fe/C and Cu-Fe/C catalysts increased with increasing temperature. At 250℃, the destruction efficiency achieved with Fe/C catalyst was 78%. In the MSWI, the destruction efficiencies obtained with activated carbon-supported catalysts (Cu/C and Fe/C) were 30-40% when the temperature was kept at 150℃. For the Fe/C catalyst, the obtained destruction efficiency at 200℃ was 66%; however, once the temperature is increased to 250℃, the destruction efficiency was reduced to 57%.
For the results of metal smelting factory, dioxin were generated through catalysis when the temperature of the Cu/C catalyst was 200℃ or 250℃ and that of the Cu-Fe/C catalyst was 250℃. In the MSWI, dioxin were generated through catalysis while the temperature of the Cu/C catalyst was 250℃. Compared with the results obtained with Cu/C and Fe/C catalysts in the metal smelting factory, it can be concluded that dioxin would be more easily produced when Cu/C catalyst is applied. Although the Cu-Fe/C contained Cu as well, no dioxin was generated at 200℃, which might be relevant to the Cu content and operating temperature.

關鍵字(中)

★ SCR 觸媒
★ 活性碳載體觸媒
★ 戴奧辛
★ 催化分解

關鍵字(英)

★ dioxin
★ active carbon-supported catalyst
★ catalysis
★ SCR catalyst

論文目次

目錄
摘要 i
Abstract iii
第一章前言 1
1.1 研究緣起 1
1.2 研究目的與範疇 2
第二章文獻回顧 1
2.1 戴奧辛類化合物之基本特性 1
2.1.1 戴奧辛類化合物之結構 1
2.1.2 戴奧辛類化合物之物化特性 2
2.1.3 戴奧辛類化合物之毒性當量 4
2.2 戴奧辛類化合物對人體健康之影響 6
2.3 戴奧辛之生成機制 7
2.4 戴奧辛之控制技術 9
2.5 觸媒之特性 11
2.5.1觸媒機制與原理 11
2.5.2傳統觸媒的種類與組成 12
2.5.2.1 活性相金屬物質 13
2.5.2.2 觸媒載體 13
2.5.3 活性碳擔體觸媒之應用 15
2.6 選擇性觸媒還原之使用與控制 16
2.6.1選擇性觸媒還原法原理 16
2.6.2 以SCR控制技術去除煙道氣中戴奧辛 17
2.6.3影響SCR觸媒催化分解戴奧辛之因素 18
2.7實廠使用觸媒催化分解戴奧辛之相關研究 28
第三章研究方法 32
3.1研究流程設計 32
3.2 採樣程序 33
3.2.1 採樣對象選擇 33
3.2.2 煙道採樣程序 33
3.2.3 觸媒上樣品取樣程序 33
3.2.4 碳基觸媒(Cu/C、Fe/C、Cu-Fe/C)製備介紹 34
3.3 實驗藥品與試劑 41
3.3.1 實驗藥品 41
3.3.2 實驗溶劑 42
3.4 實驗材料與設備 42
3.4.1 實驗材料 42
3.4.2 實驗設備 43
3.5 採樣方法 44
3.5.1 樣品瓶之清洗程序 44
3.5.2 煙道採樣設備 45
3.6 戴奧辛分析方法 52
3.6.1 戴奧辛樣品前處理 52
3.7 HRMS分析儀器條件 56
第四章結果與討論 58
4.1金屬冶煉廠與垃圾焚化廠SCR觸媒催化分解戴奧辛 58
4.1.1 金屬冶煉廠與垃圾焚化廠之戴奧辛濃度與物種分佈 58
4.1.2 金屬冶煉廠與垃圾焚化廠SCR對戴奧辛之去除效率 59
4.2 Pilot-Scale觸媒反應系統對戴奧辛之催化分解之探討 67
4.2.1觸媒選用及基本性質說明 67
4.2.2 Pilot-Scale 觸媒反應系統操作參數與採樣位置說明 68
4.2.3 Pilot-Scale觸媒系統對戴奧辛催化分解之濃度與物種分佈 71
4.3 Pilot-Scale觸媒系統對戴奧辛之去除與破壞效率評估 83
4.3.1 Pilot-Scale觸媒系統溫度效應對戴奧辛催化反應之影響 83
4.3.2 Pilot-Scale觸媒系統進流組成不同對戴奧辛催化反應之影響 86
第五章結論與建議 94
5.1 結論 94
5.1.1 實廠部份 94
5.1.2 小型模廠廠部份 95
5.2 建議 96
參考文獻 97

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指導教授

張木彬(Moo-Been Chang)

審核日期

2005-7-28

推文