| 研究生: |
黃媺瓊 Huang, Mei-Chiung |
|---|---|
| 論文名稱: |
碳表面植入氮官能基以增進NH3還原NO時之觸媒效應 Nitrogen-Containing Carbons from Phenol-Formaldehyde Resins and Their Catalytic Activity in NO Reduction with NH3 |
| 指導教授: |
鄧熙聖
Teng, Hsisheng |
| 學位類別: |
碩士 Master |
| 系所名稱: |
工學院 - 化學工程學系 Department of Chemical Engineering |
| 論文出版年: | 2002 |
| 畢業學年度: | 90 |
| 語文別: | 中文 |
| 論文頁數: | 69 |
| 中文關鍵詞: | 氮官能基 、碳觸媒 、酚醛樹脂 、選擇性觸媒還原反應 |
| 外文關鍵詞: | selective catalytic reduction., nitrogen functional group, carbon catalyst, phenol-formaldehyde |
| 相關次數: | 點閱:68 下載:2 |
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本研究主要探討碳觸媒表面之氮官能基對NH3選擇性觸媒還原NO的影響。研究中碳觸媒的製備程序是以合成酚醛樹酯為基材,並於交聯過程摻入含氮之化合物,製得表面含有氮官能基之碳觸媒。實驗中以添加Urea及m-phenylenediamine (MPDA)的方式製得所須之碳觸媒,並且進行觸媒之成份分析及觸媒活性偵測,而添加MPDA的觸媒含氮量隨之提高且觸媒活性有增加的趨勢。
由添加Urea的碳觸媒之表面結構分析得知其有較高的表面積,但由於元素分析得此觸媒並不含氮成份,因此改變製程添加m-phenylenediamine (MPDA)於酚醛樹脂製得含氮碳觸媒。
添加MPDA的製程由實驗得知此樹脂及碳觸媒之化學成份及其活性。而氮的添加對於碳觸媒在NH3還原NO時之觸媒活性有促進的效應,此外由XPS分析得知氮含量對於碳觸媒之活性有密切的關係,且反應主要發生於較大的孔洞。而觸媒活性反應中,對於低溫(< 140℃)系統下反應受吸附作用影響活性隨溫度提高而降低;高溫系統下,反應受吸附氣體與觸媒之親合性影響活性隨溫度提高而增加。本研究發現氮的添加有促進NO的吸附,並且增進吸附氣體與觸媒間的交互作用,因此提高了觸媒於NH3還原NO之反應活性。
Activated carbons with nitrogen functional group will make use of selective catalytic reduction (SCR). Carbons with well-controlled nitrogen contents were prepared from phenol-formaldehyde resins impregnated with different amounts of urea and m-phenylenediamine. The performance of these carbon catalysts for selective catalytic reduction (SCR) of nitric oxide by ammonia were investigated. The chemical compositions of the resin precursors and the resulting carbons well characterized using various analytical techniques. Elemental analysis of the chars from the urea-impregnated resins showed very little presence of nitrogen. For impregnating m-phenylenediamine there are nitrogen functional group in phenol-formaldehyde resins, and in this research we discussed the carbons with m-phenylenediamine in selective catalytic reduction (SCR). The heteroatoms, N and O, in the carbons were found to be more populated in small pores. The catalytic activity of the carbons in NO reduction of NH3 increased because of the nitrogen impregnation. The activity showed a close correlation with the nitrogen content obtained with X-ray photoelectron spectroscopy, indicating that the reaction mainly occurred in larger pores. In the low temperature regime (< 140°C), the reaction was dominated by the adsorption, which rendered a negative apparent energy, while surface interactions controlled the reaction at higher temperatures. The impregnated nitrogen atoms were found to promote the adsorption of NO, as well as to accelerate the interactions between the adsorbed species.
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