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dc.description.abstract本研究使用流體化觸媒反應器控制廢氣中的一氧化氮(NO)、二氧化硫(SO2)及粒狀污染物,主要以燃煤電廠廢氣組成作一系列探討。探討內容主要包括:(1)氧化銅觸媒(CuO/AC)的改質與選擇,使用不同溶劑對擔體作預處理,並使用含浸法製備所需觸媒;(2)探討流體化觸媒反應器對個別汙染物(NO、SO2及飛灰)的控制;及(3)探討流體化觸媒反應器同時控制 NO或SO2和飛灰之研究。 實驗結果顯示,用硝酸(AC-N)及硫酸(AC-S)預處理活性碳擔體,可以增加酚基和羧酸基的含量,可以提升觸媒活性相的分散性及控制CuO晶相大小(20~100 nm)。此外,改質CuO觸媒的活性依前處理的擔體依序排列如下:AC-N>AC-S>AC。此外,當增加觸媒表面酚基和羧酸基的含量時,可以增加觸媒對還原劑NH3的吸附能力,這行為可以提升觸媒對NO的轉換效率。當使用流體化觸媒反應器對個別汙染物控制時,對NO、SO2及飛灰的去除效率分別為57%、84%及74%。然而,當曝入在飛灰濃度約為1000 mg m-3模擬氣體時,NO及SO2的去除效率則會降低9~17%,當操作時間增加時,觸媒表面活性相會被覆蓋,進而導致觸媒物理性的失活現象。 添加4及40 μm的SiO2及Al2O3顆粒時,對流體化觸媒反應器同時控制NO、SO2及顆粒的影響顯示出增加飛灰濃度會抑制觸媒的活性。且經由氮吸附儀(BET)及表結構分析(SEM)可以證實4 μm的SiO2顆粒會造成觸媒中孔(meso-)及巨孔(marco-)孔洞的堵塞;而Al2O3顆粒則會濾除於床質內,較少堵塞於觸媒表面。此外,當增加水汽濃度時,會增加飛灰過濾的效率;但煙道中的水汽及飛灰會抑制觸媒對酸性氣體的活性,進而導致去除效率的降低。由粒徑分析(PSD)的結果指出,當水汽濃度增加時,出口粒徑會以大顆粒為主:且BET分析指出,觸媒表面堵塞現象因增加水汽含量而減少。顯示水汽濃度濃度增加有利於小顆粒凝聚及成大顆粒,因此增加粒狀物的去除效率。zh_TW
dc.description.abstractIn this study, a fluidized-bed catalytic reactor was applied for the removals of NO, SO2 and fly ash in a simulated condition of coal-fired power plant flue gas. The objectives of this study are included three parts. First, the modified and selected of catalyst, AC supports were modified by different solutions and impregnated with Cu, and analyzed their properties. Second, the removals of single pollutant such as NO, SO2, and fly ash by fluidized-bed catalytic reactor was studied. Finally, the activity of the catalyst for simultaneous removals of NO, SO2, and fly ash was investigated. Experimental results indicated that AC supports pretreated by HNO3 (AC-N) and H2SO4 (AC-S) increased the amounts of phenol and carboxylic acid groups, and further increased the dispersion and decreased the crystallite sizes of Cu active phases (20~100 nm). The activities of the CuO/AC catalysts on different pretreated AC supports follow the sequence of AC-N > AC-S > AC. The removal efficiency of NO can be improved by the adsorption capacity of NH3 when both phenol and carboxylic acid groups increased on the surface of the catalysts. The removal efficiencies of apart from NO, SO2 and fly ash are about 57%, 84% and 74%, respectively. However, the removal efficiencies of NO and SO2 were decreased to 9-17% after exposure to a concentration 1000 mg m-3 of fly ash. When the operating time was increased, the surface of the catalyst was covered by these fly ashes and resulted in the deactivation of the catalyst. For an average size of 4 (fine) and 40 (coarse) μm SiO2 and Al2O3 the activities of catalysts for simultaneous removals of NO, SO2, and particles were inhibited with increasing concentration of fly ash. The results of BET and SEM analyses verified meso- and macro-pore volume of the catalyst were obstructed by 4 μm SiO2. However, Al2O3 may become a part of catalyst bed material, and less likely to plug the catalyst surface. The removal efficiency of fly ash was increased with the increased in H2O content, but the activities of catalysts for simultaneous removals of SO2 and particles were inhibited. As the H2O content increased, the particle size distribution (PSD) of fine particles shifted to the coarse particles. The results of BET analyses show the particles obstruction phenomenon of the catalyst volume was lessened with increased H2O content. The aggregation phenomenon of fine particles shifted to the coarse particles may cause increase H2O content content in fluidized-bed catalytic reactor.en_US
dc.description.tableofcontents摘要 I ABSTRACT II 目錄 III 圖目錄 VII 表目錄 X 第一章 前言 1 1-1 研究缘起與目的 1 1-2 研究動機與目的 2 1-3 研究架構與內容 3 第二章 文獻回顧 5 2-1 燃煤火力電廠的控制對策 5 2-2 觸媒催化之特性 14 2-2-1觸媒催化對NO催化之原理與反應機制 14 2-2-2影響觸媒催化去除效率之因素 16 2-2-3觸媒催化NO及SO2及抗毒化之相關研究 22 2-2-4使用碳或含碳物質對酸性氣體之控制與除酸機制 25 2-3 粒狀污染物控制之研究 29 2-3-1 煙道中粒狀物生成特性 29 2-3-2 粒狀污染物的控制 32 2-3-3 顆粒床過濾系統 33 2-3-3-1 顆粒床收集機制 33 2-3-3-2 流體化床過濾作用 39 2-3-4 流體化床基本性質 40 2-3-4-1 最小流體化速度 40 2-3-4-2床質膨脹現象 41 2-3-4-3 床質粒徑分布 41 2-3-4-4 氣泡的性質 42 2-3-4-5 多元介質的影響 42 2-3-4-6 床質的磨損與淘失 43 3-3-5 流體化床控制飛灰及氣狀汙染物之研究 44 2-4 文獻總結與研究方向 48 第三章 實驗方法及研究設備 49 3-1 觸媒製備 49 3-2觸媒特性分析 52 3-3 觸媒反應系統 56 3-4流體化觸媒床操作條件 60 3-5床質的淘失實驗 64 3-6氣狀物及粒狀物採樣分析 67 第四章 酸預處理對碳擔體及觸媒之物化特性影響 69 4-1前言 69 4-2結果與討論 70 4-2-1 改質擔體及觸媒表面微顯型態分析 70 4-2-2 改質擔體及觸媒的XRD分析結果 74 4-2-3 改質擔體及觸媒的熱穩定性分析結果 76 4-2-4 改質擔體及觸媒的比表面積與孔洞結構之分析結果 79 4-2-5 改質擔體及觸媒的表面含氧官能基之分析結果 80 4-2-6 改質觸媒的活性測試結果 87 4-3 結論 88 第五章 流體化觸媒反應器分別控制氮氧化物及硫氧化物及粉塵之研究 89 5-1 前言 89 5-2 流體化觸媒反應系統分別控制SO2、NO及粉塵之操作條件 90 5-3流體化觸媒反應系統分別控制粉塵、SO2及NO效率之評估 91 5-3-1流體化觸媒反應系統控制粉塵效率之評估 91 5-3-2 流體化觸媒反應系統控制SO2之去除效率評估 93 5-3-3 流體化觸媒反應系統控制NO之去除效率評估 95 5-4 小結 97 第六章 流體化觸媒反應器同時控制硫氧化物及粉塵研究 98 6-1 前言 98 6-2同時控制SO2及粉塵的研究之操作條件 99 6-3結果與討論 100 6-3-1 粉塵對流體化觸媒反應器控制飛灰及SO2之研究 100 6-3-2粉塵及水汽成分對流體化觸媒反應器同時控制SO2及粉塵的影響 105 6-3-2-1 不同粉塵與水汽進料參數對控制飛灰的影響 105 6-3-2-2 不同粉塵與水汽參數對控制SO2的影響 111 6-4小結 120 第七章 流體化觸媒反應器同時控制氮氧化物及粉塵之研究 121 7-1 前言 121 7-2同時控制NO及粉塵的研究之操作條件 122 7-3結果與討論 123 7-3-1 粉塵對流體化觸媒反應器控制飛灰及NO之研究 123 7-3-2不同粉塵參數對流體化觸媒反應器同時控制NO及粉塵的影響 125 7-4 小結 137 第八章 流體化觸媒反應器同時控制氮氧化物硫氧化物及粉塵之研究 138 8-1 前言 138 8-2同時控制NO、SO2及粉塵的研究之操作條件 139 8-3結果與討論 140 8-3-1 不同操作條件下流體化觸媒反應器同時控制NO、SO2飛灰及之研究 140 8-3-2流體化觸媒反應器同時控制NO、SO2及粉塵的時間動態變化 142 8-3-3同時控制NO、SO2及粉塵的觸媒表面形態圖 144 8-3-4反應前後煙道廢氣中的飛灰PSD圖譜 145 8-3-5反應前後觸媒的XRD分析圖譜 147 8-4小結 151 第九章 結論與建議 152 9-1 結論 153 9-2 未來研究建議 154 參考文獻 156zh_TW
dc.subjectFluidized-bed catalytic reactoren_US
dc.subjectSimultaneous removalen_US
dc.subjectFly ashen_US
dc.subjectAcid gasesen_US
dc.subjectParticle size distributionen_US
dc.subjectModified catalysten_US
dc.titleDynamic variation and influence factors on the simultaneous removal of NO, SO2 and fly ash using a fluidized-bed catalytic reactoren_US
dc.typeThesis and Dissertationzh_TW
item.openairetypeThesis and Dissertation-
item.fulltextno fulltext-
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