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標題: 多壁奈米碳管吸附揮發性有機氣體之現象與機制
Properties and Mechanisms of Volatile Organic Vapors Adsorption on Multiple Wall Carbon Nanotubes
作者: 李美雪
Li, Mei-syue
關鍵字: multiple wall carbon nanotubes
volatile organic vapors
出版社: 土壤環境科學系所
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摘要: Abstract Two multiwall carbon nanotubes (MWNTs), CNT1 and CNT2, with the nanostructures and the uniform properties that may provide novel and excellent absorption properties of gases were studied. A diverse volatile organic compounds (VOCs) was used as chemical probes to investigate the adsorption mechanisms of MWNTs at room temperature (303K). The adsorption experiments of a variety of VOCs on MWNTs under various relative humidity were performed to get better understanding of the effect of humidity on sorption processes. The photographs of SEM (scanning electron microscopy) and TEM (transmission electron microscopy) showed that both MWNTs were aggregated and had no metal catalysts on the surface. The spectroscopic analysis of these two MWNTs mostly indicated they were similar. CNT2 had a little more diamond-like carbon than CNT1 examined with Raman spectra. 13C NMR (13C nuclear magnetic resonance) and XPS (X-ray photoelectron spectroscopy) measurements detected CNT1 having a tiny more C=C than CNT2. However, the amorphous carbon on the exterior layers of CNT2 was observed by electron microscopies. The adsorption coefficients of VOCs on CNT2 were larger than those on CNT1. It may result from that the impurity of MWNTs provided more sorption capacity to organic chemicals. Under two different humid conditions (55 % and 90 %), adsorption equilibrium coefficients of VOCs on the MWNTs decreased with the increasing of water content. Some adsorption sites for VOCs previously on the MWNTs were occupied by water molecules under humid conditions. The adsorption equilibrium coefficients of trichloroethylene, benzene, n-hexane, and acetone decreased with increasing temperature between 303 K and 363 K. It is an exothermic process. The adsorption heats (ΔH) of trichloroethylene, benzene, and n-hexane on the MWNTs were smaller than 40 kJ/mol. Consequently, the VOCs molecules performed physicosorption on the MWNTs surface. Adsorption equilibrium coefficients of n-alkanes and alcohols on the MWNTs became larger with more carbon atoms on the molecular structures of n-alkane and alcohol and larger with more chloro atoms on the chlorinated compounds. Several LSER (linear solvation energy relationship) equations were obtained by the regression of the sorption coefficients of VOCs on MWNTs. The analysis of the interactions based on these LSERs indicated that the London dispersion force was the major adsorption interaction in the adsorption process on MWNTs. LSERs of MWNTs at high and ambient relative humid were large different at abilities of hydrogen bond donor and acceptor. The ability of hydrogen bond donor was decreased with humidities but the ability of hydrogen bond acceptor was increased with humidity. Several LSERs equations were developed to facilitate the prediction of different organic chemicals on MWNTs which could be potential adsorbents for organic traps, chemical sensors, and gas treatment.
摘要 奈米碳管可作為吸持有機物,化學感測器和處理廢氣或廢水中有機污染物之移除材料。然其吸附有機化合物之機制仍未完全了解。本研究利用具有奈米級的結構尺寸,微觀結構規則完整之二種奈米碳管(CNT1和CNT2)來探討在室溫(303K)下奈米碳管對有機化合物之吸附作用。藉由不同有機化合物特性作為分子碳針,用以探討有機氣體和奈米碳管之間的吸附機制。由於環境中水分是影響吸附之重要因子之ㄧ,本研究也探討不同相對溼度環境下,奈米碳管對有機氣體的吸附行為。另一方面,藉由數個數個LSER方程式了解奈米碳管與不同有機化合物之間的吸附行為。 奈米碳管藉由顯微鏡影像圖觀察到CNT1和CNT2均為有中空管狀且相互糾纏聚集纏繞在一起。從氮氣吸脫附曲線圖可得知奈米碳管的吸附形曲線為S型等溫線的多層吸附型態。從拉曼光譜圖發現CNT2比CNT1含有多一些不規則的石墨結構。13C NMR和XPS顯示 CNT1比CNT2有較多一些之未飽和之碳鍵結且能提供較多之電子。 另外,在不同相對溼度55 % 和90 % 環境下,隨著水份的增加,奈米碳管對於有機化合物的吸附平衡常數有減少的趨勢,這可能是由於水分子也會吸附在奈米碳管上而佔據了有機化合物在奈米碳管上之吸附位置。在溫度方面,303 K與363 K之間,奈米碳管對於三氯乙烯,苯,正己烷和丙酮的吸附平衡常數是隨著溫度的升高而下降,說明吸附過程屬於放熱反應。三氯乙烯,苯和正己烷在奈米碳管上的吸附熱ΔH之絕對值小於40 kJ/mol,並顯示其吸附的過程主要為物理吸附。 在中與高相對溼度,溫度303K環境下之吸附實驗中,LSER(linear solvation energy relationship)結果顯示奈米碳管對於烷類和醇類之化合物的吸附平衡常數皆有隨著含碳數增加而增加的趨勢。而對於氯烷類之化合物的吸附平衡常數皆有隨著含氯數增加而增加的趨勢。以及奈米碳管和有機化合物之間的主要作用力為倫敦分散力。在中與高相對溼度環境下,奈米碳管的LSER參數之比較中可以發現其中碳管隨著水份增加而有明顯改變的性質參數有接受(a)和提供(b)氫鍵的能力。CNT1和CNT2隨著水份增加有接受氫鍵的能力(a)會增加而提供(b)氫鍵的能力會減少。實驗結果所得之數個LSER方程式可預測奈米碳管與不同有機化合物之間的吸附行為。
其他識別: U0005-2508200617220700
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