臺灣博碩士論文加值系統

選擇性觸媒還原法SCR (Selective catalytic reduction)為廣泛應用處理氮氧化物之技術，而傳統用於脫硝之釩類觸媒因其具毒性且操作溫度較高(較耗能)，近年研究多趨向發展中低溫觸媒。因此，本研究將嘗試以Mn20Fe10/TiO2觸媒同步處理模擬之廢氣，以了解廢氣組成對本實驗室所開發觸媒之脫硝效率之影響。
本研究針對脫硝系統模擬之煙道廢氣，探討不同廢氣組成(水氣、CO、SO2)的影響。結果顯示，中溫範圍內無論有無水氣存在，200 ℃之效率較250 ℃略佳，但當系統中同時具水氣和SO2時情況恰好逆轉，以250 ℃為佳。僅有CO和NO存在時(無NH3)雖可提供部分脫硝和CO轉換率，但以觸媒適用性而言效果仍不如NH3-SCR佳，無法完全取代NH3。SO2一直以來都是NH3-SCR脫硝觸媒中的毒化因子，因其反應性佳，易與NH3或觸媒金屬反應成硫酸銨鹽或金屬硫化物，毒化觸媒降低其使用壽命。此外，研究發現水氣與CO的存在對SCR脫硝來說有一體兩面的功用: 雖多了這些物種會競爭反應活性位置而使脫硝性能下降，但長時間下來此抑制也些許減緩了觸媒受SO2的毒化作用，而部分扮演了保護觸媒的角色。
結合上述結果，所製備之Mn20Fe10/TiO2觸媒經模擬廢氣條件測試，可成功應用處理氮氧化物，於空間流速10,000 h-1、反應溫度250 ℃、有15%水氣、8,000 ppm CO與20 ppm低濃度SO2之條件下，可在36 hr長時間下維持90%以上的脫硝效能。

Selective catalytic reduction (SCR) is a commonly used technique for NO reduction. The toxicity and higher operating temperature (higher energy consumption for reheating waste gas to optimal temperature) of traditional vanadium SCR catalyst restrict its application. Therefore, there has been an increasing interest in developing mid-to-low temperature SCR catalysts in recent years. This study attempts to treat simulated waste gas with Mn20Fe10/TiO2 catalyst to explore the influence of different waste gas compositions on NO abatement.
The aim of this study is to investigate the impact of different simulated waste flue gas composition (moisture, CO, SO2) to NO removal efficiency. The result shows that the NO conversion at 200 ℃ is better than at 250 ℃ no matter with/without moisture. In contrast, the NO conversion is better at 250 ℃ when moisture and SO2 exist simultaneously. When CO and NO co-exist in the system (without NH3), it can provide NO and CO conversion to some extent. However, CO is not as good as NH3 on deNO efficiency. NH3-SCR catalyst is prone to react with SO2, which poisons the catalysts due to its great chemical reactivity with NH3 and the metal on catalysts forming ammonium and metal salts. In addition, the role of moisture and CO have both positive and negative effects to SCR efficiency. The presence of moisture and CO might act as competitors to catalyst active sites and regard the NO removal; nevertheless, they also play a role in protecting catalyst by slowing down the SO2 poisoning effect. In conclusion, the Mn20Fe10/TiO2 catalyst can sustain over 90% deNO efficiency for 36 hrs under the conditions of 250 ℃, 10,000 h-1 space velocity, 15% moisture, 8,000 ppm CO and 20 ppm SO2.

摘要 i
Abstract ii
誌謝 iii
目錄 vi
圖目錄 x
表目錄 xii
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 4
2.1鋼鐵工業與燒結 4
2.1.1鋼鐵工業與生產流程 4
2.1.2燒結理論 6
2.1.3影響燒結過程的因素 8
2.1.4鋼鐵燒結流程與環境影響 8
2.2氮氧化物(NOx) 10
2.2.1 NOx來源、傳輸與生成機制 11
2.2.2 NOx危害 12
2.2.3 NOx減量處理技術 13
2.3選擇性觸媒還原法(SCR, selective catalytic reduction) 14
2.3.1 SCR原理 14
2.3.2氨洩漏(ammonia slip) 16
2.3.3 SCR反應機制 18
2.3.4影響SCR反應效率之因素: 觸媒自身特性 19
2.3.4.1觸媒結晶性(crystallinity) 19
2.3.4.2觸媒金屬分散性(dispersion) 20
2.3.4.3觸媒比表面積與孔洞體積 21
2.3.4.4觸媒表面酸度(surface acidity) 22
2.3.5影響SCR反應效率之因素: 觸媒反應環境 23
2.3.5.1反應氧含量 23
2.3.5.2空間流速 24
2.3.5.3反應溫度 24
2.3.5.4 NH3/NO注入比 25
2.3.5.5觸媒毒化 26
2.4 SCR觸媒 26
2.4.1 SCR觸媒歷史演進 26
2.4.1.1傳統SCR觸媒 27
2.4.1.2中低溫SCR觸媒 28
2.4.2 SCR觸媒活性金屬 29
2.4.2.1添加Mn金屬 30
2.4.2.2添加Fe金屬 31
2.4.2.3添加Mn和Fe金屬 32
2.4.3 SCR觸媒擔體 38
2.4.3.1擔體功用 38
2.4.3.2 TiO2擔體 39
2.4.3.3擔體與觸媒毒化的關係 40
2.5廢氣中其他物種對脫硝效率之影響 41
2.5.1煙塵(dust)和微粒 41
2.5.2水氣 42
2.5.3 SO2 46
2.5.4 水氣與SO2影響 49
2.6 SO2毒化觸媒解決之道 54
2.6.1觸媒使用前-SO2減量或調整觸媒材料 54
2.6.2觸媒使用後-觸媒再生 55
第三章、實驗方法與步驟 59
3.1研究步驟與流程 59
3.2實驗藥品及儀器設備 61
3.2.1實驗藥品及材料 61
3.2.2實驗氣體 61
3.2.3實驗儀器設備 62
3.3實驗方法 63
3.3.1觸媒製備 63
3.3.2觸媒效率測試 64
3.3.2.1脫硝實驗系統 64
3.3.2.2水氣管線流路與計算說明 67
3.3.3氣體分析 69
3.3.4觸媒特性分析 70
第四章、結果與討論 77
4.1觸媒基本物化特性分析 77
4.1.1 ICP金屬元素含量分析 77
4.1.2氮氣吸脫附分析 78
4.1.3 NH3-TPD觸媒表面酸基分析 78
4.1.4 TGA熱重損失分析 80
4.2燒結廢氣組成對脫硝效率之交互影響討論: 無SO2 80
4.2.1水氣含量對脫硝效率的影響 80
4.2.2水氣與還原劑(NH3、CO)對脫硝效率的影響 84
4.2.2.1 NO、CO觸媒催化氧化還原關係 86
4.2.2.2有無水氣影響 87
4.2.2.3還原劑(NH3、CO)影響 88
4.2.2.4溫度影響 89
4.3燒結廢氣組成對脫硝效率之交互影響討論: 有SO2 90
4.3.1水氣與SO2對脫硝效率的影響 90
4.3.2有SO2時水氣含量對脫硝效率的影響與相關性分析 94
4.3.2.1有SO2時水氣含量對脫硝效率的影響 94
4.3.2.2脫硝效率影響之相關性分析 95
4.3.2.3比表面積影響之相關性分析 96
4.3.2.4 NH3-TPD分析影響之相關性分析 98
4.3.2.5 TGA分析影響之相關性分析 104
4.3.2.6觸媒脫硝效率、物化特性與含水量之相關性關係綜合討論 108
4.3.3 SO2毒化下水氣與還原劑(NH3、CO)對脫硝效率的影響 109
4.3.3.1水氣影響 111
4.3.3.2還原劑影響(NH3、CO) 112
4.3.3.3溫度影響 114
4.4模擬燒結廢氣之長效測試 115
4.4.1 SO2濃度影響 115
4.4.2空間流速(GHSV)影響 116
4.4.3溫度影響 118
4.4.4溫度、水氣與SO2綜合影響 119
4.4.5模擬完整廢氣長效測試 120
4.5廢氣成分對SCR脫硝之影響 121
第五章、結論與建議 125
5.1 結論 125
5.2 建議 126
第六章、附錄 128
6.1觸媒脫硝相關資料 128
6.2使用後觸媒相關特性分析資料 144
參考文獻 150

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