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完整後設資料紀錄
DC 欄位 | 值 | 語言 |
---|---|---|
dc.contributor.advisor | 鄭淑芬(Soofin Cheng) | |
dc.contributor.author | Pin-Hao Huang | en |
dc.contributor.author | 黃品豪 | zh_TW |
dc.date.accessioned | 2021-06-08T02:27:40Z | - |
dc.date.copyright | 2015-08-25 | |
dc.date.issued | 2015 | |
dc.date.submitted | 2015-08-17 | |
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dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/19928 | - |
dc.description.abstract | 揮發性有機物(Volatile organic compounds)係指在標準狀態下蒸氣壓大於0.1 mmHg之有機物質,因此容易揮發且具有較低的沸點,其不只對於環境有害,也會讓人體產生嘔吐、噁心等不適症狀,某些揮發性有機物更被證實對人體有致癌性,因此如何有效減少揮發性有機物的汙染是當今急需迫切解決的問題。在各種去除方法中,以吸附法擁有高操作彈性、價錢便宜最為廣泛使用,其中又以活性碳最常被當作吸附劑使用,因其吸附能力佳、造價便宜,但其在吸附時容易造成孔洞阻塞,容易吸水,更有自燃等安全上得虞慮。沸石(Zeolite),因其具有獨特的晶體結構、高熱穩定性與表面積等特性,被認為是非常有潛力作為吸附揮發性有機物的替代材料。
本研究利用矽鋁比不同的Y型與ZSM-5型沸石作為吸附劑捕捉代表性揮發性有機物(甲苯、甲基環戊烷、巴豆醛),並將材料做後修飾:包括與鈉、銀、銅、氫離子做離子交換,或者經過酸鹼溶液處理進行介孔製備,同時也合成含鈦之沸石TS-1進行比較,材料以X光粉末繞射鑑定其晶體結構,使用感應耦合電漿質譜分析儀計算其中各元素含量,並利用氮氣吸附-脫附測量表面積以及孔體積,使用掃描式電子顯微鏡鑑定沸石形貌,並以程溫脫附儀進行吸脫附特性的研究。實驗結果顯示,在相同吸附條件下,影響甲苯吸附量的關鍵因素為陽離子含量(矽鋁比),陽離子含量越多,甲苯吸附量越高,但同時也較吸水;次要因素為離子的型式,鈉離子最對於甲苯與水氣的吸附量最高,氫離子則相反,對於甲苯與水氣的吸附量最低;當矽鋁比相近、離子型式相同時,比較面積的貢獻才會較為明顯,比表面積越大的材料,吸附效果越好。在甲基環戊烷的吸附中,發現到當探針分子與材料孔洞大小相近時,會使分子類似卡在孔洞中的狀況,吸附量提升且不易脫附,如Na-Z120對於甲基環戊烷的吸附量為5.18 wt%,高於其對於甲苯的吸附量3.75 wt%。在巴豆醛的吸附中,我們發現到含有銀、銅、氫離子的Y型與ZSM-5型沸石的吸附的同時會伴隨產生氧化裂解等反應,而TS-1對於巴豆醛僅有單純吸脫附之作用,吸附量約為6 ~ 7 wt%。在經過諸多試驗後,我們也找出在不同條件下適用之吸附劑:若吸附環境為無水的狀態,適合使用經過鹼處理之Na-Y3B,其對於甲苯與甲基環戊烷的吸附量最高,達到了21.0 wt%與13.8 wt%。而若要在一般含水氣的環境下吸附,則氫離子型式的H-Z120最為適合,因其對於水氣的吸附量非常低,具有30.3的甲苯/水選擇率與44.8的甲基環戊烷/水選擇率。 | zh_TW |
dc.description.abstract | Volatile organic compounds (VOCs) are organic chemicals that have high vapor pressure at ambient temperature, and many of them are harmful to the environment and are toxic or even carcinogenic to the human being. Many technologies are available for VOCs control, such as adsorption, condensation, membrane separation, oxidation and biological treatment, among which adsorption is the most applicable technology because of the flexibility of the system, low energy, and inexpensive operation costs. Activated carbon has long been recognized as the most versatile adsorbent due to its low cost and excellent adsorption capacity. However, several drawbacks, such as hygroscopicity, pore clogging,and low thermal stability are associated with its use in adsorption processes. Hence, extensive efforts have been focused on finding alternative adsorbents. Zeolites are microporous molecular sieves with crystalline structures, high specific surfaces and thermal stabilities, have been proposed as potential adsorbents for VOCs adsorption/separation.
In this study, zeolite Y and ZSM-5 were exchanged with different cations, including sodium, silver, copper and hydrogen or been treated with acid and base solution to create mesopores in zeolite structure. Futhermore, we synthesized zeolites with different amounts of Ti/Si ratio and used as the adsorbents of VOCs, including toluene, methylcyclopentane and crotonaldehyde. The materials were characterized by X-ray diffraction, nitrogen sorption, scanning electron microscope and elemental analysis. The uptakes of toluene, methylcyclopentane and steam over these zeolites were investigated by temperature programmed desorption. We found that under same experiment conditions, the amounts of cations was the key point to determine the amount of toluene adsorption; then was cation form; only when the adsorbent had similar cation amount and same cation form, the effect of specific surface area would show up. In the experiment of methylcyclopentane adsorption, we found that when the size of adsorbate molecules were similar to the pore size of adsorbent, adsorption capacity would increase and become hard to drsorb. In the experiment of crotonaldehyde adsorption, Y-type and ZSM-5 with silver, copper and hydrogen form would promote oxidation/cracking of crotonaldehyde, TS-1 only shows the adsorption/desorption peak without other reactions happened, the adsorption capacity was around 6 ~ 7 wt%. If we want to adsorption VOCs in dry condition, Na-Y3B is the best choice, because it has the largest adsorption for both toluene (21.0 wt%) and methylcyclopentane (13.8 wt%). H-Z120 is suitable for adsorption VOCs in normal condition, due to its hydrophobicity, has the highest toluene/steam selectivity (30.3) and methylcyclopentane/steam selectivity (44.8). | en |
dc.description.provenance | Made available in DSpace on 2021-06-08T02:27:40Z (GMT). No. of bitstreams: 1 ntu-104-R02223106-1.pdf: 9542014 bytes, checksum: aab077b1438e4bc4fc071c2f3c8cb6dd (MD5) Previous issue date: 2015 | en |
dc.description.tableofcontents | 謝誌 I
摘要 II Abstract IV 表目錄 IX 圖目錄 XI 第1章 緒論 1 1-1揮發性有機物之定義與種類 1 1-2揮發性有機物之來源與組成 2 1-3揮發性有機物造成之一次汙染 6 1-4揮發性有機物造成之二次汙染 11 1-5揮發性有機物之移除方法與材料 13 1-6沸石與分子篩 14 1-7沸石結構簡介 16 1-8 Y型沸石 20 1-9 ZSM-5型沸石 21 1-10影響吸附之因子 23 1-10-1物理吸附與化學吸附 23 1-10-2吸附劑性質 25 1-10-3吸附質性質 27 1-10-4環境因子 28 1-10-5混合吸附 30 1-11沸石吸附揮發性有機物相關文獻回顧 31 1-11-1沸石骨架中異原子之影響 31 1-11-2沸石不同矽鋁比之影響 32 1-11-3沸石離子交換位置之影響 33 1-11-4沸石結構含中孔洞之影響 36 1-12研究動機與目的 37 第2章 實驗部分 40 2-1化學藥品 40 2-2材料製備 41 2-2-1製備離子交換之沸石 41 2-2-1-1製備鈉離子交換之沸石 41 2-2-1-2製備銀離子交換之沸石 41 2-2-1-3製備銅離子交換之沸石 41 2-2-1-4製備氫離子交換之沸石 42 2-2-2製備含不同鈦比例之沸石 42 2-2-3製備酸鹼處理之沸石 43 2-3鑑定材料之儀器與方法 45 2-3-1 X光粉末繞射(Powder X-ray Diffraction,XRD) 45 2-3-2氮氣吸附-脫附等溫曲線(N2 Adsorption-desorption Isotherm) 46 2-3-3掃描式電子顯微鏡(Scanning electron microscopy, SEM) 48 2-3-4誘導偶極電漿質譜儀(Inductively Coupled Plasma/Mass Spectroscopy,ICP-MS) 48 2-3-5紫外-可見光分光光譜儀(Ultraviolet–visible Spectophotometer,UV-Vis) 49 2-3-6程式控溫脫附儀(Temperature Programmed Desorption,TPD) 49 第3章 結果與討論 59 3-1離子交換之沸石 59 3-1-1 XRD鑑定 59 3-1-2恆溫氮氣吸脫附鑑定 62 3-1-3 ICP-MS鑑定 65 3-1-4 SEM鑑定 65 3-1-5吸附效果鑑定 70 3-2含鈦之沸石 79 3-2-1 XRD鑑定 79 3-2-2 UV-VIS鑑定 79 3-2-3恆溫氮氣吸脫附鑑定 80 3-2-4 ICP-MS鑑定 81 3-2-5 SEM鑑定 82 3-2-6吸附效果鑑定 83 3-3酸鹼處理之沸石 88 3-3-1 XRD鑑定 88 3-3-2恆溫氮氣吸脫附鑑定 89 3-3-3 ICP-MS鑑定 91 3-3-4 SEM鑑定 92 3-3-5吸附效果鑑定 93 3-4巴豆醛吸附 98 3-5吸附影響因素之探討 101 3-6成果與文獻比較 108 第4章 結論 110 參考文獻 112 附錄一 揮發性有機物吸脫附實驗參數 121 附錄二 揮發性有機物檢量線之計算 124 | |
dc.language.iso | zh-TW | |
dc.title | Y型與ZSM-5沸石應用於揮發性有機物之吸脫附特性研究 | zh_TW |
dc.title | Applications of Y and ZSM-5 zeolites in VOCs adsorption | en |
dc.type | Thesis | |
dc.date.schoolyear | 103-2 | |
dc.description.degree | 碩士 | |
dc.contributor.oralexamcommittee | 萬本儒(Ben-Zu Wan),邱靜雯(Ching-Wen Chiu) | |
dc.subject.keyword | Y型沸石,ZSM-5,揮發性有機物,甲苯吸附, | zh_TW |
dc.subject.keyword | Y-type zeolite,ZSM-5,volatile organic compounds,toluene adsorption, | en |
dc.relation.page | 125 | |
dc.rights.note | 未授權 | |
dc.date.accepted | 2015-08-17 | |
dc.contributor.author-college | 理學院 | zh_TW |
dc.contributor.author-dept | 化學研究所 | zh_TW |
顯示於系所單位: | 化學系 |
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