鈣鈦礦型觸媒之製備與其應用於分解NO之探討

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陳玫君(Mei-chun Chen) 查詢紙本館藏

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論文名稱

鈣鈦礦型觸媒之製備與其應用於分解NO之探討
(Perovskite-type oxides prepared as the catalyst for NO decomposition)

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摘要(中)

本研究以檸檬酸溶膠凝膠法（sol-gel）製備La2NiO4、LaSrNiO4、La0.7Ce0.3SrNiO4等Pervskite oxide型觸媒，並觀察三者分解NO效能之差異。此外，亦利用非熱電漿放電技術，針對鍛燒後之La0.7Ce0.3SrNiO4觸媒進行N2或Air電漿處理，以瞭解電漿處理對於觸媒效能之影響，並針對電漿處理前後的觸媒進行相關物性分析。實驗結果顯示，La0.7Ce0.3SrNiO4觸媒具最佳NO分解率。操作參數方面，固定NO濃度1000ppm、反應溫度600－900℃、空間流速8000h-1。在無氧、900℃的條件下、，以氮氣作為載氣之NO分解率高於氬氣，所得結果分別為99.90％和49.89％；在900℃、氧氣濃度1%時，以氮氣和氬氣作為載氣之NO分解率略為下降，分別為99.12%和44.97%，表示觸媒在此含氧量下活性抑制的情形輕微，但提高含氧量至3%及6%時，NO分解率低於40%。非熱電漿改質觸媒方面，其操作參數為：氣體流量1000sccm、空間流速1241 h-1、施加電壓16.5kV、放電頻率100Hz、氣體種類為N2及Air。未經電漿改質的La0.7Ce0.3SrNiO4觸媒在900℃、氧氣濃度0%和1%時之NO分解率雖高於經電漿處理之觸媒，但提高氧氣濃度後，發現經電漿改質後的觸媒之NO分解率並未像電漿改質的觸媒急速下降，N2電漿及Air電漿觸媒在氧氣濃度3%及6%時之NO分解率分別為36.45%、17.81%及28.55%、12.27%；未經電漿改質觸媒在氧氣濃度在3%及6%時之NO分解率分別為24.66%及6.54%，顯示在較高含氧量下，電漿改質後之觸媒對氧氣有較高之容忍力。

摘要(英)

Perovskite-type oxides including La2NiO4, LaSrNiO4, and La0.7Ce0.3SrNiO4 were prepared by the citric acid complexation and used as catalysts for direct decomposition of NO. Moreover, non-thermal plasma technology was applied after calcinations of La0.7Ce0.3SrNiO4. In this study, i.e., citric acid complexation (without plasma treatment), N2-plasma-treated, and air-plasma-treated catalysts were tested for NO decomposition to understand the effect of plasma treatment on the catalytic performance. The catalysts before and after plasma treatment were characterized, respectively, to discern the effects. The activities of La2NiO4, LaSrNiO4, and La0.7Ce0.3SrNiO4 for NO decomposition were tested and the results indicate that in the same experimental parameters, La0.7Ce0.3SrNiO4 catalyst is of the highest NO decomposition with Ar, with the efficiency up to 49.89%. The inlet NO concentration was controlled at 1000 ppm, and the reaction temperature ranged from 600℃ to 900 ℃, while the space velocity was fixed at 8,000h-1. The influences of oxygen content and water vapor content on NO decomposition were also explored. In the absence of O2, NO decomposition achieved is much higher as N2 is used as carrier gas compared with Ar. With 1% oxygen content in the gas stream, NO decomposition decreased slightly to 99.12% and 44.97%, respectively, as N2 and Ar are used as the carrier gases. The results indicate that the activation of catalyst was slightly suppressed with 1% O2 content. On the other hand, NO decomposition decreases rapidly as the oxygen content is increased to 3% and 6%.
Non-thermal plasma is applied to modify the performance of perovskite-type oxides catalyst. The operating parameters are as following：gas flow rate is 1000 sccm, space velocity is 1241 h-1, the applied voltage is 16.5kV, and the discharge frequency is 100 Hz with either nitrogen or air as carieer gas. At 900℃, NO decomposition achieved with La0.7Ce0.3SrNiO4 catalyst before plasma treatment as N2 is used as carrier gas is much higher than that the catalyst after plasma treatment in the presence of 0% or 1% O2, however, as the oxygen content is increased to 3% and 6%, the La0.7Ce0.3SrNiO4 catalyst before plasma treatment activity is significantly decreased to 24.66% and 6.54%, respectively, as N2 is used as the carrier gas. The results lower than the La0.7Ce0.3SrNiO4 catalyst after plasma treatment with N2 as the carrier gas. As the oxygen content is increased to 3% and 6%, the N2-plasma-treatment catalyst activity is 36.45% and 17.81%, respectively, and air-plasma-treatment catalyst activity is 28.55% and 12.27%, respectively. The results indicate that the the catalysts after plasma treatment possess strong tolerance in the presence of 3% and 6% oxygen content.

關鍵字(中)

★ Pervskite oxides 型觸媒
★ NO分解
★ 電漿處理觸媒
★ 非熱電漿

關鍵字(英)

★ non-thermal plasma
★ plasma treatment catalyst
★ perovskite-type oxides catalyst
★ NO decomposition

論文目次

摘要.......................................................I
Abstract.................................................VII
表目錄.....................................................X
第一章前言................................................1
1-1 研究緣起...............................................1
1-2 研究目的與內容.........................................2
第二章文獻回顧............................................3
2-1 氮氧化物的特性、來源與危害.............................3
2-1-1 氮氧化物的基本特性...................................3
2-1-2 氮氧化物的來源.......................................5
2-1-3 氮氧化物對健康與環境造成的衝擊.......................5
2-2 氮氧化物生成機制.......................................8
2-3 氮氧化物控制技術.......................................9
2-3-1 燃燒前處理（Pre－Combustion Ttreatment）.............9
2-3-2 燃燒程序修正（Combustion Modification）.............10
2-3-3 燃燒後處理（Post－Combustion Removal）..............10
2-3-3-1 溼式法（Flue Gas Denitrification, FGDN）..........12
2-3-3-2 乾式法............................................12
2-4 Perovskite oxide型觸媒催化分解氮氧化物................19
2-4-1 Perovskite oxide型觸媒簡介..........................19
2-4-2 Perovskite oxide型觸媒製備方法......................21
2-4-3 部分取代A-site陽離子的影響..........................22
2-4-4 活性位的結構與反應機制..............................25
2-5 電漿..................................................32
2-5-1 電漿生成原理........................................32
2-5-2 電漿產生方式........................................36
2-5-3 電漿放電對於觸媒表面物化特性之影響..................40
第三章研究方法與設備.....................................43
3-1 研究流程與架構........................................43
3-2 觸媒製備..............................................44
3-2-1 傳統檸檬酸法........................................44
3-2-2 空氣電漿處理與氮氣電漿處理..........................46
3-3 實驗設備..............................................49
3-3-1 氣體供應與試藥......................................51
3-3-2 實驗參數控制系統....................................51
3-3-3 反應器..............................................53
3-3-4 電力供應設備........................................54
3-3-5 反應物與產物分析設備................................55
3-4 研究方法..............................................55
3-4-1 NO分解實驗..........................................55
3-4-2 數據計算............................................57
3.5 儀器原理及操作條件....................................57
第四章結果與討論.........................................61
4-1 以氬氣為載氣對NO分解效率之影響........................61
4-2 以氮氣為載氣對NO分解效率之影響........................63
4-2-1 氧氣含量對NO分解效率之影響..........................66
4-2-2 水氣含量對NO分解效率之影響..........................67
4-3 觸媒之基本特性分析結果................................71
4-3-1 BET氮氣吸脫附測試...................................71
4-3-2 LV-SEM分析..........................................72
4-3-3 SEM-EDS觸媒元素組成.................................73
4-3-4 XRD晶相分析.........................................74
4-3-5 O2-TPD..............................................77
4-4 介電質放電實驗........................................79
4-4-1 電漿處理後之觸媒對NO分解效率之影響..................79
4-4-2 氧氣含量對NO分解效率之影響..........................80
4-5 電漿處理後之觸媒基本特性分析結果......................82
4-5-1 BET氮氣吸脫附測試...................................82
4-5-2 LV-SEM分析..........................................83
4-5-3 XRD晶相分析.........................................84
4-5-4 O2-TPD..............................................87
第五章結論與建議.........................................88
5-1 結論..................................................88
5-2 建議..................................................89
參考文獻..................................................90

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指導教授

張木彬(Moo-been Chang)

審核日期

2012-8-25

推文