臺灣博碩士論文加值系統

本研究係利用固定床 (fixed-bed) 反應器進行沸石吸附劑 (NaY、V/NaY 及PtO2/NaY) 應用於去除揮發性有機氣體 (乙醇) 之吸附性能及再生之結構研究。並藉由同步輻射之粉末X光繞射及X光吸收光譜分析吸附劑結構。由貫流曲線 (Breakthrough curve) 估算吸附容量 (adsorption capacity) 結果顯示PtO2/NaY＞NaY＞V2O5/NaY。造成此結果之因素可由吸附劑結構研究得以瞭解。由EXAFS結果顯示氧化釩在沸石中呈現孤立結構，因佔據沸石之吸附活性位，導致吸附能力降低。相反地，由FT-IR結果顯示PtO2在沸石上提供了額外之吸附活性位置得以吸附更多之乙醇。由於PXRD結果顯示沸石超過550℃以上會造成沸石結構破壞，所以應盡可能降低再生溫度如此才能延長吸附劑之壽命。而吸附飽和之吸附劑經由空氣300℃再生，結果顯示對於NaY而言，乙醇沒辦法完全地被移除，因此導致再生後吸附能力略微下降；而使用鉑金屬則可以催化氧化吸附之乙醇，且從PXRD及EXAFS證據顯示催化氧化過程產生之CO將使PtO2還原成Pt，而Pt對乙醇吸附能力較PtO2為佳，因此空氣再生後些微地增加吸附能力。此結果驅使我們在吸附測試前對PtO2/NaY進行氫氣前處理。結果顯示氫氣還原確實增加了乙醇吸附能力，然而再生後此效應消失，因為再生及還原過程使得鉑金屬顆粒聚集，此結果可由EXAFS得到印證。

The performance of NaY, PtO2-NaY, and V2O5-NaY in removing ethanol from air stream was investigated by a fixed bed adsorber. The structure of catalytic adsorbents was characterized by synchrotron PXRD and EXAFS. The adsorption capacity of these three adsorbents depends on the metal oxide deposited and decreases in the order: Pt-NaY > NaY > V2O5-NaY. EXAFS results suggest that isolated vanadia block adsorption sites on zeolite, leading to a decrease in the adsorption capacity. In contrast, PtO2 clusters on NaY provide additional sites for ethanol adsorption. Since PXRD results indicate the destruction of zeolite structure at 550 C, to extend the adsorbents life cycle, regeneration temperature should be kept as low as possible. Upon air regeneration of the ethanol-saturated adsorbents at 300 C, NaY adsorption capacity decreases slightly, due to the residual ethanol. In the presence of PtO2, ethanol can be completely oxidized catalytically. In addition, evidenced by PXRD and EXAFS, more adsorption sites were induced by CO reduction of PtO2 to Pt clusters after air regeneration. The results motivated us to pre-treat the PtO2-NaY with flowing hydrogen before performance tests. The hydrogen reduction enhances ethanol adsorption capacity whereas after several regeneration cycles the enhancement were depleted by the aggregation of Pt clusters during the air-regeneration and hydrogen reduction cycles, suggested by EXAFS.

目錄
圖目錄 I
表目錄 V
第一章 緒論 1
1.1研究背景 1
1.1.1室內空氣品質與污染簡介 2
1.1.2環保法規之規範 4
1.1.3 文獻回顧 8
1.2吸附劑簡介 12
1.2.1前言 12
1.2.2沸石吸附劑 12
1.2.3吸附之種類 15
1.2.4吸附原理 (Principle of Adsorption) 17
1.3研究動機 21
1.4研究目的 22
第二章 實驗設計與特性分析方法 23
2.1研究方法 23
2.2實驗規劃 25
2.2.1實驗流程 25
2.2.2實驗所用之藥品與氣體 26
2.3吸附劑製備 27
2.3.1觸媒擔體材料 27
2.3.2觸媒製備 28
2.3.3吸附劑之製備 31
2.4吸附劑性能測試實驗 34
2.4.1反應設備 34
2.4.2吸附性能測試 35
2.5特性分析方法 39
2.5.1氣相色層分析（Gas Chromatography；GC） 39
2.5.2傅立葉轉換-紅外線光譜分析 (Fourier Transform Infrared；FT-IR) 40
2.5.3 X光吸收光譜分析 （Analysis of X-ray Absorption Spectrum；XAS） 41
2.5.3a簡介 41
2.5.3b X光吸收近邊緣結構 (XANES) 46
2.5.3c延伸X光吸收精細結構 (EXAFS) 47
2.5.3d量測方法 51
2.5.4粉末X光繞射 (Powder X-ray Diffraction；XRD) 52
第三章 結果與討論 55
3.1 吸附劑吸附性能測試 55
3.1.1 新鮮吸附劑之吸附性能測試結果 55
3.1.2 吸附劑之再生後吸附性能測試結果 55
3.2 吸附劑之特性分析結果 57
3.2.1 釩沸石吸附劑特性分析結果與吸附性能關連性 57
3.2.2 沸石吸附劑特性分析結果與吸附性能關連性 58
3.2.3 鉑沸石吸附劑特性分析結果與吸附性能關連性 58
3.2.4 鉑沸石吸附劑之EXAFS fitting結果 61
3.3 吸附劑再生途徑探討 64
3.4 鉑沸石吸附劑前處理條件不同對吸附性能之影響 67
3.5不同前處理條件之鉑沸石吸附劑特性分析結果 68
3.5.1氫氣前處理之鉑沸石吸附劑特性分析結果與吸附性能關連性 68
3.5.2 前處理條件不同之鉑沸石吸附劑再生後結構比較 69
3.5.3 氫氣前處理鉑沸石吸附劑之EXAFS fitting結果 70
3.6 不同前處理條件之鉑沸石吸附劑再生途徑探討 73
第四章 總結與未來展望 130
4.1總結 130
4.2未來展望 131
參考文獻 132

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