| 研究生: |
陳玉茵 Hapsari, Patricia Permana Jati |
|---|---|
| 論文名稱: |
高值化甘蔗渣廢棄物為功能性生質碳應用於轉化CO2 Valorization of Sugarcane Bagasse to Functionalized Biochar for Conversion of Carbon Dioxide into Cyclic Carbonates |
| 指導教授: |
劉守恒
Liu, Shou-Heng |
| 學位類別: |
碩士 Master |
| 系所名稱: |
工學院 - 環境工程學系 Department of Environmental Engineering |
| 論文出版年: | 2018 |
| 畢業學年度: | 106 |
| 語文別: | 英文 |
| 論文頁數: | 68 |
| 中文關鍵詞: | 生物碳 、二氧化碳 、環加成反應 、環氧化物 、甘蔗渣 |
| 外文關鍵詞: | biochar, carbon dioxide, cycloaddition, epoxide, sugarcane bagasse |
| 相關次數: | 點閱:77 下載:0 |
| 分享至: |
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本研究內容為利用甘蔗渣所製備的胺官能化生物碳,使二氧化碳經環加成作用形成環氧丙烯。首先,為了獲得胺官能化的生物碳,本研究先透過微波水熱反應以及氫氧化鉀活化使甘蔗渣碳化,然後在333K下透過氯化鐵六水合物將經過活化和碳化之甘蔗渣進行石墨化。最後,利用3-氨基丙基三乙氧基矽烷進行胺官能化,藉此獲得目標物。此外,為了進行比較,本研究同時也利用純石墨和商業碳黑以相同程序製備觸媒。
經合成之碳觸媒將透過X光繞射儀(X-ray Diffraction, XRD)、掃描電子顯微鏡(Scanning Electron Microscopy, SEM)、穿透式電子顯微鏡(Transmission Electron Microscopy, TEM)、拉曼光譜(Raman Spectroscopy)、傅里葉轉換紅外光譜(Fourier Transform Infrared Spectroscopy, FTIR)、X射線光電子能譜儀(X-ray Photoelectron Spectroscopy, XPS)、元素分析儀(Elemental Analysis, EA)、熱重分析(Thermogravimetric Analysis, TGA)進行特性分析。
而本研究當中所提到之環加成反應,則是藉由作為輔觸媒的季銨鹽或是作為功能性輔助溶劑的N,N-二甲基甲酰胺(DMF),與碳觸媒結合所實現。另外,同時也研究了不同的輔觸媒,如四丁基溴化銨(TBAB)或四丁基碘化銨(TBAI)對於環加成性能的影響。
為了實現碳酸亞丙酯(Propylene Carbonate, PC)的高轉換率和高選擇性,研究中包含各種實驗條件,例如觸媒負載,溫度,二氧化碳壓力和反應時間。而反應後之產物則利用氣相層析儀(gas chromatography-barrier ionization discharge, GC-BID) 確認。
結果表明,不同條件下使用季銨鹽作為輔觸媒,在條件為PO:ASGR:TBAI = 200:300:1、溫度70°C、壓力10kg/cm2、24小時的反應時間,胺官能化甘蔗渣石墨(Amine-Functionalized Sugarcane Bagasse Graphite, ASGR)能有最高的轉化率和選擇性,分別為98%和98%。與此同時,胺官能化甘蔗渣炭黑(Amine-Functionalized Sugarcane Bagasse Carbon Black, ASCB)則是在條件為PO:ASGR:TBAI = 200:75:1、溫度70°C、壓力10kg/cm2、24小時的反應時間,有最佳的轉化率和選擇性,分別為98%和99%。
而在使用DMF作為功能輔助溶劑,在條件為PO:ASGR = 2:3以及PO:DMF = 5:1、溫度180°C、壓力10kg/cm2、24小時的反應時間,ASGR的具有最高轉化率和選擇性,分別為約99%和84%。
In this work, cycloaddition of CO2 to propylene oxide (PO) using amine-functionalized biochars made from sugarcane bagasse (SB) is reported. To obtain amine-functionalized biochars, SB was carbonized through microwave hydrothermal reaction and KOH activation. Then carbonized and activated SBs were further graphitized by using FeCl3.6H2O at 333 K followed by amine-functionalizing via 3-aminopropyltrimethoxysilane (APTMS). For comparison, other catalysts were also prepared from pure graphite and commercial carbon black (CB).
The synthesized carbon catalysts were characterized by X-ray Diffraction (XRD), Scanning Electron Microscopy (SEM), Transmission Electron Microscopy (TEM), Raman Spectroscopy, N2 Adsorption-Desorption, Fourier Transform Infrared Spectroscopy (FTIR), X-ray Photoelectron Spectroscopy (XPS), Elemental Analysis, and Thermogravimetric Analysis (TGA).
Cycloaddition reactions were carried out combining carbon catalysts and quaternary ammonium salts as co-catalysts or N,N-Dimethylformamide (DMF) as functional accessory solvent. Also, effects of different tetrabutylammonium bromide (TBAB) and tetrabutylammonium iodide (TBAI) as co-catalysts on the cycloaddition performance were investigated.
Various reaction conditions, such as catalyst loading, temperature, CO2 pressure, and reaction time, were studied in order to achieve high conversion and high selectivity of propylene carbonate (PC). The products were confirmed by gas chromatography-barrier ionization discharge (GC-BID).
The results showed that under various reaction conditions using quaternary ammonium salts as co-catalyst, the highest conversion and selectivity by amine-functionalized sugarcane bagasse graphite (ASGR) were about 98% and 98%, respectively under the conditions of PO:ASGR:TBAI = 200:300:1, 70 °C, 10 kg/cm2, and 24 hours. Meanwhile, the highest conversion and selectivity by amine-functionalized sugarcane bagasse carbon black (ASCB) were about 98% and 99% respectively under the conditions of PO:ASCB:TBAI = 200:75:1, 70 °C, 10 kg/cm2, and 24 hours.
Under various reaction conditions using DMF as functional accessory solvent, the highest conversion and selectivity by ASGR were about 99% and 84%, respectively under the conditions of PO:ASGR = 2:3, PO:DMF = 5:1, 180 °C, 10 kg/cm2, and 24 hours.
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校內:2023-08-01公開