鈦酸鹽奈米管複合碳球去除水溶液中鉛、銅、鎘、亞甲基藍、苯酚與甲苯之研究

Removal of Pb (II), Cu (II), Cd (II), Methylene Blue, Phenol, and Toluene from Aqueous Solution through TNTs-CSs Adsorbent

艾以曼(ADE IMAS AGUSNINGTYAS)

指導教授 ： 趙煥平 ； 王玉純

中原大學/工學院/環境工程學系/碩士(2020年)

https://doi.org/10.6840/cycu202000472

摘要

摘要

隨著城市工業中的冶金、電子與化學的快速的發展，水資源中很容易發現重金屬、染料和有機化合物trace的蹤跡。 將TiO2奈米鈦管(TNTs)和葡萄糖碳球(CSs)以5:5的比例合成TNTs-CSs吸附污染物，合成的方法則是採用水熱合成(兩階段過程)，然後在300-800℃的溫度下煅燒。完成後的TNTs-CSs成品透過SEM、XPS、XRD、FTIR和BET進行表徵分析。 吸附後的結果證明TNTs-CSs (E300)對鉛(II)具有最大吸附容量(567.16毫克/克), 再來則是銅(II)(452.50毫克/克)、亞甲基藍(610.70毫克/克)和苯酚(374.34毫克/克)，而TNTs-CSs(E800)和TNTs-CSs (E400)具有最大吸附量分別是鎘(II)(504.68毫克/克)和甲苯(252.40毫克/克)，適用於Langmuir吸附等溫模型。在污染物吸附的初始15分鐘時，反應呈連續性且逐漸增加，整體上也符合擬二級動力學模型。此外，TNTs-CSs (E300)吸附苯酚時，只需t0.5 的時間，也就是初始濃度的苯酚，只需3.24分鐘就可以吸附整體的50％。
性能表徵顯示，溫度在結構構成中扮演重要的角色，像是SEM圖在測量經過600 - 800℃鍛燒的樣品時，清楚地顯示出兩種不同形狀的物質在這一溫度下能夠聚合(球體和不規則狀或棒狀結構)，而高溫下加熱時樣品的平均直徑會變得更大。溫度的修正過程使在氧化階段時表徵會受環境的物理與化學變化而變，且與XPS資料中的原子百分比有關聯。另外，XRD數據顯示鍛燒與未鍛燒的TNTs-CSs(E)，結構是以銳鈦礦型態為主，因此非常活躍，這有利於提高吸附能力。吸附過程中也發生了化學反應，因此在FTIR光譜儀中，產生次要與主要的波峰變化。煅燒後的TNTs-CSs(E)表面積，隨者溫度自300、400、500℃上升而上升，表面積分別為34.2、56.5和131.9平方米/克。然而較高的煅燒溫度，表面積會逐漸減少，即在溫度600、700和800℃時，表面積的值分別是64.7、6.7和5.0平方米/克。在溫度300-600°C下，CSs、TNTs-CSs(E)和煅燒後的TNTs-CSs(E)的吸附等溫線屬於國際純化學和應用化學聯合會(IUPAC)分類中的Type II型，而TNTs和TNTs-CSs (E700)屬於Type III型；TNTs-CSs (E800)則是屬於Type V 。此外，CSs、TNTs-CSs (E)和煅燒後的TNTs-CSs (E)，顯示出H3型遲滯曲線，TNTs則是表現出H2 (b)-type型的遲滯曲線。

關鍵詞：吸附，TiO2奈米碳管，碳球，重金屬，染料，有機化合物

關鍵字

吸附，TiO2奈米碳管，碳球，重金屬，染料，有機化合物

並列摘要

ABSTRACT

Heavy metal, dye, and organic compound are very easy to get into water resources with the rapid development of urban industrialization, including metallurgy, electronics, and chemistry. A TiO2 Nanotubes (TNTs) and glucose carbon spheres (CSs) was synthesized as TNTs-CSs to adsorb the contaminants with the ratio of 5:5. The synthesis was applying hydrothermal carbonization method (two-stage processes) and then calcined at the temperature of 300-800°C. The synthesized TNTs-CSs were characterized by SEM, XPS, XRD, FTIR, and BET. The adsorption results demonstrated that TNTs-CSs (E300) have the highest maximum adsorption capacity for Pb (II) (567.16 mg/g), Cu (II) (452.50 mg/g), methylene Blue (610.70 mg/g) and phenol (374.34 mg/g), whereas TNTs-CSs (E800) and TNTs-CSs (E400) have the highest maximum adsorption capacity for Cd (II) (504.68 mg/g) and toluene (252.40 mg/g), respectively that can fit Langmuir isotherm model. The adsorption of contaminant increased consecutively during the initial 15 minutes of the contact interval and is fit with pseudo-second order kinetic model. Moreover, the phenol adsorption onto TNTs-CSs (E300) led all adsorption t0.5 with only 3.24 minutes to adsorb 50% of contaminants from the initial concentration. The characteristics show that temperature plays an important role of the structure.
The SEM images clearly showed an agglomeration of two different shapes when samples calcined at the temperature of 600-800°C (sphere and irregular bricks or rod like structure), and the average diameter of the sample becomes even greater when heating at high temperatures. The occurrence of formal oxidation states and changes in characteristics in the physical or chemical environment resulted from the temperature modification process also correlates with changes of the atomic percentage in the XPS data. The XRD data show the structure of uncalcined or calcined TNTs-CSs (E) was dominated by the anatase phase, which is very useful for increasing adsorption capacity because it is very active. The adsorption also occurred chemically, as there are some minor to major changes in the FTIR spectra. The surface area of calcined TNTs-CSs (E) rises gradually at temperatures of 300, 400 and 500°C in the amount of 34.2, 56.5 and 131.9 m2/g, respectively. Then the higher the calcination temperature, the surface area of the sample decreases, i.e. at temperatures 600, 700, and 800°C, the surface area values are 64.7, 6.7, and 5.0 m2/g, respectively. The adsorption isotherms of CSs, TNTs-CSs (E), and calcined TNTs-CSs (E) at temperature 300-600°C were classified as Type II of the International Union of Pure and Applied Chemistry (IUPAC) classification, while TNTs was classified as the Type III and TNTs-CSs (E700); TNTs-CSs (E800) were classified as Type V. Moreover, CSs, TNTs-CSs (E), and calcined TNTs-CSs (E) exhibit the H3-type hysteresis loop and TNTs exhibit the H2 (b)-type hysteresis loop.

Keywords: Adsorption, TiO2 Nanotubes, Carbon Spheres, Heavy Metal, Dye, Organic
Compound

並列關鍵字

Adsorption, TiO2 Nanotubes, Carbon Spheres, Heavy Metal, Dye, Organic Compound

參考文獻

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