Please use this identifier to cite or link to this item: http://hdl.handle.net/11455/5711
標題: 奈米碳管吸附氣相異丙醇之研究
Adsorption of Isopropyl Alcohol onto Carbon Nanotubes
作者: 許世杰
Hsu, Shih-Chieh
關鍵字: 奈米碳管;CNTs;異丙醇;吸附;IPA;Adsorption
出版社: 環境工程學系所
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摘要: 
奈米碳管(Carbon nanotubes, CNTs)為環境工程應用上的新興材料,文獻上鮮少有針對其吸附特性、吸附行為有完整之研究,應用於有機氣體吸附上之文獻更是缺乏。因此,本研究係應用多壁奈米碳管(Muti-wall carbon nanotubes, MWCNTs)與單壁奈米碳管(Single-wall carbon nanotubes, SWCTNs)為吸附材料。並選用目前常見於高科技產業中,作為清潔及溶劑等用途之異丙醇(Isopropyl Alcohol, IPA)做為吸附質,進行相關研究。
本研究初步直接以實驗方法測試吸附容量,並分離化學性與物理性吸附機制之貢獻量。在材料特性上,CNTs管徑大小與吸附量成反比。並且,SWCNTs的平衡吸附容量(34.58mg/g)明顯高於MWCNTs的最大吸附容量(27.48 mg/g)。本研究並收集文獻上分別用於純化或改質用途之處理分法合併比較,包括(HNO3、HCl及NaOCl三種改質方法)。結果發現經NaOCl氧化處理後的SWCNTs其物理性及化學性吸附能力增加最顯著。由孔洞分佈的結果可以發現,物理性吸附能力主要透過孔洞結構的改變,微孔體積的增加所貢獻,其平均孔徑由3.80nm減少至2.06nm,微孔洞(<2nm)的孔洞體積分佈佔總孔洞體積百分比由25%增加至67%。;化學性吸附能力則透過改質程序對奈米碳管表面進行化學修飾,增加表面官能基,進而增加化學性吸附量。在IPA進流濃度為40與800ppmv的條件下,SWCNTs(NaOCl)吸附容量約為Raw SWCNTs的1.5及3.0倍,其吸附行為並符合Langmuir 及BET等溫吸附模式。
透過吸附熱的計算同時也可以發現,當於低溫吸附環境時,由於物理性吸附較為顯著,因此吸附熱的值相對較小;然而當吸附環境溫度高於25℃時,吸附熱明顯上升,顯示物理吸附受溫度影響抑制,化學性吸附成為主要機制。
與商用活性碳同時進行再生吸附比較,結果發現CNTs較活性碳有優異的再生穩定性,經過數次吸、脫附反應循環後,CNTs仍保有較高的吸附量與去除效率。脫附速率比較結果亦可以發現,奈米碳管對溫度有較高敏感度,因此脫附時,可以偵測到較快速且較高濃縮倍率的出流氣體。顯示CNTs相較活性碳有更長的使用壽命,可重複使用,並同時有脫附所需能量較低的特性。證明CNTs較活性碳於VOCs污染控制技術應用上有更高的潛力。

Commercially available carbon nanotubes (CNTs) were employed as adsorbents to study the adsorption of isopropyl alcohol (IPA) vapor from air stream. Adsorption of IPA vapor onto CNTs increased with decreased outer diameter (dp) of CNTs. At influent IPA concentration of 200 ppmv, the maximum adsorbed capacity of IPA onto single-walled CNTs (SWCNTs, dp<2nm, 34.58 mg/g) was higher than that onto multiwalled CNTs (dp<10 nm, 27.48 mg/g). It was indicated that SWCNTs was optimal adsorbent in all tested CNTs.
Single-walled carbon nanotubes (SWCNTs) were oxidized by HCl, HNO3 and NaOCl solutions and were selected as adsorbents to study their characterizations and adsorption properties of IPA vapor from air streams. The physicochemical properties of SWCNTs were greatly changed after oxidation by HNO3 and NaOCl solutions. These modifications include the increase in surface functional groups, which enhance the chemisorption capacity of IPA, and the decrease in pore size and the increase in surface area of micropores, which improve the physisorption capacity of IPA. The maximum IPA adsorption capacities of SWCNTs, SWCNTs(HCl), SWCNTs(HNO3) and SWCNTs(NaOCl) calculated by Langmuir model are 63.48, 54.34, 72.99 and 103.56 mg/g, respectively.
The SWCNTs(NaOCl) show the best performance of IPA removal and their adsorption mechanism appears mainly attributable to physical force with a relatively low influent IPA concentration but appears attributable to both physical and chemical forces with a relatively high influent IPA concentration.
SWCNTs(NaOCl) was employed to study adsorption kinetics, thermodynamics and desorption of IPA vapor in an air stream. The adsorption capacity of IPA decreased with temperature indicating an exothermic nature of adsorption process and slightly decreased with relative humidity showing a hydrophobic nature of adsorbent surface. The adsorption mechanism appears mainly attributable to physical force in 5-25℃ but appears primarily attributable to chemical force in 25-35℃.
A comparative study on the cyclic IPA adsorption between SWCNTs(NaOCl) and activated carbon (GAC(NaOCl)) was also conducted and the results revealed that the SWCNTs(NaOCl) show better repeated availability of IPA adsorption during 15 cycles of operation than the GAC(NaOCl). In continusely temperature swing experiment, SWCNTs(NaOCl) shows the higher removal efficiency in adsorption regin and higher concentrated rate(Ceff/C0) in desorption regine.
This suggests that the SWCNTs(NaOCl) are efficient IPA adsorbents and can be used in the prolonged cyclic adsorption/desorption operation. It also revealed that SWCNTs(NaOCl) was also more suitable for application in VOCs emitted control, extraction, and chemical sensor.
URI: http://hdl.handle.net/11455/5711
其他識別: U0005-2605200903133700
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