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研究生:張芊穎
研究生(外文):Chien Ying Chang
論文名稱:水溶液中沸石吸附氨之機制研究
論文名稱(外文):The mechanism of the adsorption of ammonia on zeolite
指導教授:李茂田
指導教授(外文):Maw Tien Lee
學位類別:碩士
校院名稱:國立嘉義大學
系所名稱:應用化學系研究所
學門:自然科學學門
學類:化學學類
論文種類:學術論文
畢業學年度:102
語文別:中文
論文頁數:89
中文關鍵詞:沸石吸附
外文關鍵詞:FT-IRXRD
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本文以不同矽鋁比之Y-型沸石去除氫氧化銨並探討再生溫度對沸石結構之影響。實驗使用不同矽鋁比之Y-型沸石,以離子交換或吸附方式去除氨氮或銨離子,使用過之沸石再分別以不同溫度鍛燒以及離子交換再生沸石吸附劑。為了解氨(銨)吸附行為,研究中以由傅立葉轉換紅外光光譜儀(FT-IR)觀察Y-型沸石吸附前後之官能基變化。並以同步輻射中心之粉末X光繞射儀(PXRD),觀察沸石加熱再生前後之結構變化。FT-IR實驗結果顯示,未經處理的高矽鋁比Y-型沸石相較於低矽鋁比Y型沸石明顯多了一個吸收特徵峰Si-OH的Si-O stretching,(960cm-1),且其吸附銨的特徵峰也明顯的位移許多;由XRD觀察未處理的Y-型沸石之結晶相,高矽鋁比沸石(CBV760;Si/Al : 60)的背景值高於低矽鋁比的許多。此結果顯示高矽鋁比之Y-型沸石,由於鋁被洗出,因而形成結晶缺陷為吸附銨的官能基;結晶缺陷增高PXRD背景,而形成官能基原因是由於isolated Si(OH)4所產生的。較低矽鋁比之沸石CBV712(Si/Al : 11.5)和CBV600(Si/Al : 5.2 ),對銨的吸附行為:一為銨之離子交換、另一種為沸石上之酸性基與NH3上未共用電子對形成配位結合吸附。
批次吸附實驗經由不同吸附等溫線結果顯示,CBV600吸附情形較似於單層吸附的Langmuir等溫線、CBV760吸附情形較似於非均質表面吸附的Freundlich等溫線,再生試驗中發現因以高溫鍛燒會破壞晶體排列而以飽和食鹽水之再生情形較佳。
We investigated the ammonia adsorption using different Si/Al ratio zeolite in the water solution. In this study, the adsorption ammonia by zeolite was observed by measuring the IR spectra and PXRD spectra of fresh and used zeolite. With IR spectra, experimental results showed that only higher Si/Al ratio zeolite (CBV760; Si/Al ratio: 60) has terminal Si-O stretching peak (960cm-1). PXRD spectra showed that CBV760 has higher background, lower peak intensity, and its peak displacement to higher degree. These showed that because of Si/Al ratio zeolite’s aluminium was taken caused the crystal collapse and resulted ammonium adsorption function group. It’s came from isolated Si(OH)4. For lower Si/Al ratio zeolite (CBV600.CBV712), they are relatively hydrophilic. IR spectra results showed that there are two adsorption phenomena, one is ionexchange with ammonium, the other is the effects of counterion on the IR spectrum of ammonia.
Batch adsorption experiments via different adsorption isotherms showed that CBV600 adsorption curve is fit to Langmuir adsorption isotherm, which is relate to monolayer adsorption situation. And CBV760 adsorption curve is fit to Freundlich adsorption isotherm, which is relate to non-homogeneous surface adsorption situation. Regeneration experiments found due to the high temperature calcination will destroy the crystalline arrangement, and with saturated sodium chloride solution was preferred for regeneration.

第一章 緒論 1
1-1 實驗動機 1
1-2 實驗目的 2
第二章 文獻回顧 5
2-1 氨氣簡介 5
2-1.1 氨 5
2-1.2 氨水 5
2-2 氨氣處理 7
2-2.1化學處理 7
2-2.2物理處理 8
2-2.3生物處理 8
2-3 吸附劑簡介 10
2-3.1沸石吸附劑 10
2-3.2沸石分類與型式 13
2-3.3沸石吸附 15
2-4吸附等溫線簡介 18
第三章 材料與方法 25
3-1實驗材料 25
3-2實驗器材與儀器 26
3-2.1傅立葉轉換-紅外線光譜分析儀 28
3-2.2粉末X光繞射 30
3-2.2分光光度計 32
3-3實驗步驟 33
3-3.1水溶液配製 33
3-3.2鍛燒樣品製備 33
3-4實驗步驟流程圖 39
第四章 結果與討論 40
4-1未使用過之沸石 40
4-2吸附批次試驗 40
4-3使用過之沸石 40
4-4吸附等溫線之擬合 40
4-5溫度批次試驗 40
4-6傅立葉紅外線光譜(FT-IR)頻率計算 40
4-7再生試驗 40
第五章 結論 85
第六章 參考文獻 87
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16. Wang, Y.; Kmiya, Y.; Okuhara, T., Removal of low-concentration ammonia in water by ion-exchange using Na-mordenite. Water research 2007, 41 (2), 269-76.

17. Baker, H. M.; Fraij, H., Principles of interaction of ammonium ion with natural Jordanian deposits: Analysis of uptake studies. Desalination 2010, 251 (1-3), 41-46.

18. Zheng, H.; Han, L.; Ma, H.; Zheng, Y.; Zhang, H.; Liu, D.; Liang, S., Adsorption characteristics of ammonium ion by zeolite 13X. Journal of hazardous materials 2008, 158 (2-3), 577-84.

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