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  • 學位論文

碳球與層狀複合金屬氫氧化物經接枝程序合成複合吸附劑去除水中染料之研究

Removal of dyes though a composite adsorbent of grafted carbon sphere-layered double hydroxides

指導教授 : 趙煥平

摘要


摘要 本研究主要是利用複合材料形式製作出可以同時吸附陽離子與陰離子染料之吸附劑,製備的方法為先合成碳球(CS)與層狀複合金屬氫氧化物(LDHs)之合成複合材料,再將碳球接枝增加COOH官能基,形成新的吸附劑(LDHs-CS-g),然後將所合成之吸附劑在不同 pH條件下吸附之陰離子與陽離子染料,並比較接枝前後之吸附量差異。 研究過程先以水熱合成法將葡萄糖製備成碳球,再將碳球加入包含LDHs製成原料之溶液中,利用再一次水熱合成法製成LDHs-CS,再以硝酸鈰銨將作為初始劑以及丙烯酸提供COOH官能基利用接枝共聚合程序方式增加表面官能基。合成後的吸附劑將以SEM、FTIR、EDS及BET表面積分析儀等儀器分析,分析吸附劑表面特性。吸附質方面則選擇鹼性的亞甲基藍(MB)與亞甲基綠(MG) 染料以及酸性的酸紅(AR1)染料,然後以Langmuir及Freundlich吸附模式進行擬合,並估算在pH3、6 與9的溶液中CSs-LDHs與CSs-LDHs-g對所選擇染料之吸附容量。 由SEM觀察LDHs-CS與LDHs-CS-g,可以發現球狀與片狀結構與單獨形成的CS與LDHs接近。且由傅立葉轉換紅外線光譜儀(FITR)與EDS的分析結果得知,LDHs-CS與LDHs-CS-g同時具備兩種材料的官能基與元素組成;LDHs-CS-g在染料吸附陽離子染料時吸附量遠大於LDHs-CS,又以pH9時吸附效果最好,吸附陰離子染料則略為低於LDHs-CS;透過Langmuir model估算最大吸附容量,可以發現LDHs-CS-g在 pH3、pH6、pH9對MB之吸附量分別為294、833、714 mg/g。LDHs-CS在pH3、pH6、pH9對AR1之最大吸附量分別為99.0、56.2、29.2 mg/g; LDHs-CS-g在pH3、pH6、pH9對MG之最大吸附量分別為476、666、1111mg/g。主要的吸附機制為離子交換外,氫鍵作用力可能是次要的吸附機制,其他作用機制較不重要。 關鍵詞:層狀複合金屬氫氧化物;碳球;複合吸附劑;接枝;染料

並列摘要


Abstract In this study, an adsorbent that can simultaneously adsorb cationic and anionic dyes was fabricated in the form of composite materials. Carbon spheres were grafted to increase COOH functional groups to form a new adsorbent (LDHs-CS-g), and then the synthesized adsorbents were used to adsorb anionic and cationic dyes under different pH conditions, and the difference in adsorption capacity before and after grafting was compared. . In the research process, glucose was first prepared into carbon spheres by hydrothermal synthesis, and then the carbon spheres were added to the solution containing LDHs as raw materials, and LDHs-CS was prepared by another hydrothermal synthesis method, and then cerium ammonium nitrate was used as the initial Agents and acrylic acid provide COOH functional groups to increase surface functional groups by means of a graft copolymerization procedure. The synthesized adsorbent will be analyzed by SEM, FTIR, EDS and BET surface area analyzer to analyze the surface characteristics of the adsorbent. In terms of adsorbate, basic methylene blue (MB) and methylene green (MG) dyes and acidic acid red (AR1) dyes were selected, and then fitted with Langmuir and Freundlich adsorption models, and estimated at pH 3, 6 and 9. The adsorption capacity of CSs-LDHs and CSs-LDHs-g for selected dyes in solution. By SEM observation of LDHs-CS and LDHs-CS-g, it can be found that the spherical and sheet-like structures are close to the CS and LDHs formed separately. And from the analysis results of Fourier transform infrared spectrometer (FITR) and EDS, it is known that LDHs-CS and LDHs-CS-g have functional groups and elements of two materials at the same time; LDHs-CS-g adsorbs cationic dyes when the dyes are adsorbed. The amount is much larger than that of LDHs-CS, and the adsorption effect is the best at pH 9, and the adsorption of anionic dyes is slightly lower than that of LDHs-CS. The maximum adsorption capacity of LDHs-CS-g is estimated by the Langmuir model. The adsorption capacities were 294, 833, and 714 mg/g, respectively. The maximum adsorption capacities of LDHs-CS for AR1 at pH3, pH6, and pH9 were 99.0, 56.2, and 29.2 mg/g, respectively; the maximum adsorption capacities of LDHs-CS-g for MG at pH3, pH6, and pH9 were 476, 666, and 1111 mg, respectively. /g. The main adsorption mechanism is ion exchange, the hydrogen bonding force may be a secondary adsorption mechanism, and other mechanisms are less important. Key words: layered composite metal hydroxide; carbon sphere; composite adsorbent; grafting; dye

參考文獻


參考文獻
https://www.newton.com.tw/wiki/酸性紅1/3290682
https://zh.m.wikipedia.org/zh-tw/亞甲藍
https://zh.wikipedia.org/zh-tw/煌綠
Ay, A.N.; Karan-Zumreoglu, B.; Temel, A. Boron removal by hydrotalcite-like, carbonate-free Mg–Al–NO3-LDH and a rationale on the mechanism. 2007. Microporous and Mesoporous Materials, 98 (1–3), 1–5.

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