第四章、 結果與討論
4.3 催化效率測試
4.3.4 長效連續測試 (Endurance test)
圖 4-21 為本研究之長效測試與文獻(Hu et al., 2009)比較之結果,
在溫度為 260℃、濃度為 1000ppm、GHSV=15000h-1的相同條件下與 文獻之結果進行測試比較,Hu et al.(2009)使用焚化法(Combustion method)進行材料製備,形成雙金屬 Cu 及 Ce 之氧化物,並進行 36
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根據文獻(Spivey, 1987)指出,在較高溫度能迅速提供所需之能量 給欲處理之污染物,使得附著在觸媒表面的 VOCs 進行催化反應,使 得原本觸媒暫時失活(deactive)現象消失,因此催化效果可維持高且穩 定;相反地,當使用較低的溫度時,占據於觸媒活性位置之 VOCs 反 應速率較慢而使觸媒暫時失活現象明顯,造成觸媒衰退現象,因此 VOCs 轉化率經長效測試即逐漸下降。
Time-on-stream(h)
0 5 10 15 20 25 30 35 40
Conversion(%)
50 60 70 80 90 100
Cu/Ce/ZSM-5(imp.) 1000(ppm) 260(degree C) (Hu et al., 2009) 1000ppm 260 degree C Cu/Ce/ZSM-5(imp.) 500(ppm) 200(degree C)
圖 4-21、Cu/Ce/ZSM-5(imp.)觸媒長效性催化測試與 Hu et al.(2009)結 果比較(Hu et al.(2009)所使用之觸媒為 Cu/Ce 之雙金屬氧化物)
(SV=15000h-1)
79 2 theta(degrees)
20 22 24 26 28 30 32 34 36 38 40
Intensity(a.u.)
after tested before test
CuO CuO
圖 4-22、XRD 圖譜(a) before test and (b) after test for 15h (SV = 15000h-1、conc. = 500ppm、temp. = 200℃)
4.5 複合式吸脫附/觸媒催化系統
本系統為複合式吸脫附/觸媒催化的連續式反應,選擇雙金屬含 浸法之 Cu/Ce/ZSM-5(imp.)作為吸附型觸媒進行連續吸脫附及催化反 應,而反應首先在常溫約 25℃吸附到飽和後,再經由 180℃之脫附溫 度進行脫附,接著再將脫附出來的丙酮氣體通入後端位於高溫爐內之 觸媒催化系統,此高溫爐以 350℃進行持續不斷地加熱,形成連續吸 脫附與觸媒催化連續反應,如此反覆測試 5 次,進流的丙酮濃度保持 在 500ppm,空間速度為 31000h-1。
圖 4-23 為在吸附實驗下反覆五次之吸附曲線,圖 4-24 則列出經 由吸附曲線計算之飽和吸附量。由反覆吸附量曲線可以看出乾淨的材
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81
Fresh Cycle1 Cycle2 Cycle3 Cycle4 Cycle5
Adsorption capacity(mg/g)
82
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圖 4-27、Cu/Ce/ZSM-5(imp.)吸附型觸媒連續吸脫附之丙酮濃度關係
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15000h-1)下,本研究所使用之 Cu/Ce/ZSM-5(imp.)觸媒可以在 36 小時後,仍可維持 96%以上之丙酮轉化率,相較於文獻使用 Cu/Ce
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脫附及 350℃之催化反應後,各次循環實驗結果顯示即使在 20000ppm 以上之丙酮瞬間濃度下,仍可維持在 90%以上之轉化 效率。
5.2 建議
1. 本研究所使用之擔體為以商用的沸石 ZSM-5 加以金屬改質,使用 雙金屬 Cu 及 Ce 負載於其上當作實驗測試之吸附型觸媒,然由許 多文獻中得知使用 Mn 及 Cs 等金屬對於處理 VOCs 亦有不錯的效 果,而中孔洞吸附材因為比表面積高以及孔洞均勻化等優點,亦 逐漸受到重視。未來可使用比表面積較大的中孔洞 MCM-41 及 MSP 等材料進行改良,或使用其他經濟性及反應性都較佳的過渡 金屬進行測試,以獲致更完整之資訊。
2. 本研究目前是選用丙酮作為污染物之處理物種,但高科技廠製程 所排放之污染物亦可能含有其他種類(如異丙醇等),並可能同時 排放多種污染物,彼此之間產生協同或競爭效應,未來可加以討 論多種污染物之處理效果。
3. 本研究受限於時間因而未探討濕度或氧氣濃度之影響,但實際上 水氣或氧氣可能會影響到污染物之處理效果,另外對於銅及鈰雙 金屬之間的交互作用未能深入了解,建議未來可加以探討。
4. 目前進行連續式吸脫附接催化反應時,在於吸附到飽合後才進行 後續之脫附接催化,而於未來探討時,可將吸附時間縮短至約 10min,使其維持較佳的吸附效率,後續的脫附接催化反應時間 也能下降到約 30min,使連續式反應整體循環一次約 40min,較 符合實場上的要求。
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