由於礫石兼具有高蓄熱與廉價的特性，本研究以蓄熱式石材作為載體，以銅、錳、鈷活性金屬，分別製作不同金屬配比與不同金屬負載量之金屬觸媒，來處理揮發性有機氣體之異丙醇。並從觸媒焚化處理之轉化效率來探討出最佳之觸媒，並深入探討各種操作參數對於該觸媒之活性表現，以及長時間衰敗測試對於觸媒活性變化之觀察，並找出描述異丙醇觸媒氧化之反應動力模式。

觸媒篩選呈現結果為金屬配比10 %與金屬配比6：4之銅鈷觸媒表現最佳，在異丙醇進流濃度1500 ppm、空間流速13500 hr-1、焚化溫度350 ℃時轉化率可達95 %，乃自製觸媒21組裡處理效率最佳的觸媒，並選擇此組觸媒進行操作參數之實驗。

操作參數實驗結果呈現為焚化溫度、進流氧氣濃度、進流異丙醇濃度升高，則轉化率也相對提高；反之空間流速之增大，則轉化率則相對降低；另外在長時間之衰敗測試下其仍具有較佳的穩定性，並輔助以掃描式電子顯微鏡(SEM)、表面元素分析(EDS)、元素分析儀(EA)、X-ray觀察其衰敗前後之變化情形，由觀察結果顯示出長期衰敗測試無明顯之觸媒破損之現象以及積碳之情形發生。

觸媒反應動力模式中Power-rate Law模式較為適用，觸媒焚化反應回歸結果為近一階反應。

In general, the characteristics of stone are two: high regenerative thermal activity and low cost. In this study, isopropyl alcohol (IPA) was oxidized by metallic catalysts with stones as carriers. To discover the best removal efficiency of isopropyl alcohol, different catalysts with different ratios of metal (these metals were copper, manganese, and cobalt) and different loading (loading meant the ratio of the weight of metal to the weight of stone) were made. Moreover, others parameters such as different inlet concentration of IPA, inlet concentration of oxygen, space velocity, reaction temperature, and long-term test were also discussed. Finally, two kinetic models were introduced to prove the catalytic oxidation mechanism of IPA.

The experimental results showed that the most effective catalyst is copper-cobalt catalyst, which ratio of metals is 6: 4 and loading is 10%. With this kind of catalyst, the optimal operational parameters could be easily found, and they were as follows: the inlet concentration of IPA was 1500 ppm, space velocity was 13500 hr-1, and reaction temperature was 350℃. It was noticed that the conversion of IPA was all up to 95% in these conditions.

In conclusion, the experimental results also indicated that conversion was increased with reaction temperature, inlet concentration of IPA and inlet concentration of oxygen increasing. On the contrary, the conversion was decreased as space velocity was increased. Besides, after long-term test of catalyst, the results showed that the performance of the catalyst acted still fairly well in oxidation. To realize the physical properties of catalysts, some analytic instruments such as SEM, EDS, EA, XRD were used. These analytic results could also tell us the difference between fresh and aged catalysts.

Two kinetic models, Power rate law Model and Mars-Van Krevelen Model, were used to fit the kinetic mechanism of the decomposition of IPA. The fitting result was that Power rate law Model was rather suitable to describe the catalytic decomposition of IPA in the operational conditions in this work, and the reaction order was nearly first order.

中文摘要..............................................................................................................I
英文摘要.............................................................................................................Ⅱ
目錄....................................................................................................................Ⅲ
表目錄................................................................................................................Ⅶ
圖目錄................................................................................................................Ⅸ

第一章 緒論...................................................................................................1
1-1 前言..........................................................................................................1
1-2 研究目的..................................................................................................2
1-3 研究內容..................................................................................................3

第二章 文獻回顧............................................................................................5
2-1 VOCs之簡介............................................................................................5
2-1-1 異丙醇之介紹................................................................................7
2-2 VOCs之控制技術介紹............................................................................9
2-3 金屬觸媒之特性.....................................................................................13
2-4 影響VOCs觸媒焚化效能之操作參數.................................................16
2-4-1 VOCs的種類與濃度.................................................................16
2-4-2 焚化溫度....................................................................................18
2-4-3 空間速度......................................................................................20
2-4-4 氧氣濃度....................................................................................22
2-4-5 載體之特性與選擇....................................................................23
2-4-6 觸媒種類與負載量比................................................................25
2-4-7 觸媒活性的衰退........................................................................26
2-5 觸媒焚化理論與動力式探討...............................................................28
2-5-1 觸媒焚化VOC之反應機制.......................................................28
2-5-2 反應動力式的探討....................................................................30

第三章 研究方法與實驗設備.......................................................................39
3-1 研究方法................................................................................................39
3-1-1 實驗規劃....................................................................................48
3-1-2 實驗步驟與方法........................................................................49
3-1-3 檢量線製作..................................................................................50
3-1-4 載體物性測試..............................................................................52
3-2 觸媒的製備.............................................................................................54
3-3 實驗設備與藥品.....................................................................................55
3-3-1 實驗系統裝置............................................................................55
3-3-2 試藥與氣體................................................................................59
3-3-3 主要儀器與條件........................................................................59

第四章 結果與討論.......................................................................................65
4-1 觸媒活性篩選..........................................................................................65
4-1-1 3%、5%、10%負載量的純銅觸媒比較..................................66
4-1-2 3%、5%、10%金屬負載量的銅錳觸媒比較..........................72
4-1-3 3%、5%、10%負載量的銅鈷觸媒比較..................................77
4-1-4 銅鈷觸媒、銅錳觸媒之比較....................................................82
4-2 觸媒製作成本之推估.............................................................................92
4-3 觸媒焚化異丙醇操作參數探討.............................................................93
4-3-1 觸媒焚化產物測試...................................................................94
4-3-2 空白測試...................................................................................96
4-3-3 進流濃度之效應.......................................................................98
4-3-4 空間流速之效應.....................................................................100
4-3-5 進流氧氣含量之效應.............................................................102
4-4 觸媒長期活性衰退的探討..................................................................104
4-4-1 觸媒衰退現象.........................................................................104
4-4-2 掃描式電子顯微鏡分析(SEM) .............................................106
4-4-3 表面分析(EDS) ......................................................................108
4-4-4 元素分析(EA) ........................................................................111
4-4-5 BET比表面積分析................................................................113
4-5 操作參數對反應速率之影響..............................................................113
4-5-1 Power-rate law.........................................................................114
4-5-2 Mars-Van Krevenlene Model...................................................119
4-6 操作參數對反應速率之影響..............................................................123
4-6-1 進流濃度對反應速率之效應.................................................123
4-6-2 不同反應溫度對反應速率之影響.........................................125
4-6-3 氧濃度對反應速率之影響.....................................................127
第五章 結論與建議......................................................................................130
5-1 結論.......................................................................................................130
5-2 建議.......................................................................................................132

參考文獻........................................................................................................133

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