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研究生:柯順福
研究生(外文):Ko, Shun-Fu
論文名稱:製備高表面積的多孔性氧化鎂中空管固體吸附劑 應用於捕捉二氧化碳氣體之研究
論文名稱(外文):Fabrication of High Surface Area Porous MgO Hollow Tubular Solid Adsorbents for CO2 Capture
指導教授:高立衡高立衡引用關係
指導教授(外文):Kao, Li-Heng
口試委員:林鉉凱莊高樹
口試委員(外文):Lin, Hsuan-KaiChuang, Kao-Shuh
口試日期:2017-06-13
學位類別:碩士
校院名稱:國立高雄應用科技大學
系所名稱:化學工程與材料工程系博碩士班
學門:工程學門
學類:化學工程學類
論文種類:學術論文
論文出版年:2017
畢業學年度:105
語文別:中文
論文頁數:98
中文關鍵詞:聚醚碸氧化鎂相轉化法二氧化碳中空管固體吸附劑吸附/脫附循環吸附熱
外文關鍵詞:polyethersulfonemagnesium oxidephase inversion methodCO2hollow fibersolid adsorbentadsorption / desorption cyclic testisosteric heat of adsorption
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在本實驗中利用相轉化法,以聚醚碸作為高分子溶液,添加不同含量的氧化鎂粉體,製備出三種氧化鎂中空管固體吸附劑(P1M10、P1M15、P1M20),再以水合法改善其吸附二氧化碳能力,製備出三種吸附劑(P1M10hy、P1M15hy、P1M20hy);所得樣品經X光繞射儀鑑定其結構特性,具有MgO晶相以及Mg(OH)2晶相(JCPDS PDF 45-0946 與 44-1482),經傅立葉轉換紅外線光譜儀與核磁共振儀鑑定具有Mg(OH)2、H2O的存在,經比表面積分析儀鑑定具有中孔洞性質;P1M10hy(比表面積56 m2g-1)相對於未處理之氧化鎂粉體(比表面積6 m2g-1),顯示出氧化鎂中空管固體吸附劑增加近九倍比表面積增加量。
觀察吸附/脫附循環圖,得知氧化鎂中空管固體吸附劑對二氧化碳氣體具有高選擇吸附性。以熱重分析儀分析測定,在一大氣壓,溫度25 ℃下,二氧化碳吸附量最大為19.19 wt% (191 mg/g)。以二氧化碳吸附/脫附循環穩定趨勢圖得知,經過10次吸/脫附循環之後,吸附能力會衰退至第一次循環的57%,推測吸附劑在重複吸脫附之後,氧化鎂結晶會失去其活性能力,導致二氧化碳吸附能力下降。
利用比表面積分析儀(ASAP2020)進行吸附熱(Qst)的測定,P1H10hy在一大氣壓下273 K、298 K之二氧化碳吸附,吸附熱從31 kJ/mol,改變至22 kJ/mol。由吸附熱隨吸附量大小而改變,可以定義該吸附系統為非均相。

Three kinds of magnesium oxide (MgO) hollow fibrous solid adsorbents (P1M10, P1M15, P1M20) were prepared with polyethersulfone and different contents MgO powders by phase inversion method. The samples were characterized by X-ray diffractometer, and diffraction peaks of MgO and Mg (OH) 2 are identified unambiguously (corresponding to JCPDS PDF 45-0946 and 44-1482, respectively). From the characteristic absorption peaks of Fourier transform infrared spectrum and Nuclear Magnetic Resonance spectrum confirmed the presence of Magnesium hydroxide and water. P1M10hy (specific surface area 56 m2g-1) exhibited mesoporous properties and increased nearly nine times the amount of surface area than MgO powder (specific surface area 6 m2g-1).

From adsorption/desorption cyclic test, the MgO hollow fibrous solid adsorbent had high selectivity to carbon dioxide (CO2). The maximum adsorption capacity of CO2 was 19.19 wt% (191 mg/g) at 25 ℃ under 1 atm by using thermos-gravimetric analysis. The adsorption / desorption cyclic test showed that after 10 cycles of adsorption/desorption, the adsorption capacity declined to 57% of the first cycle, suggesting that after the repeated adsorption and desorption of the adsorbent, the MgO lost their activity.
The adsorption heat (Qst) of the P1M10hy was carried out at a temperature of 273 K and 298 K with an atmospheric pressure by volumetric adsorption analyzer (ASAP2020). The adsorption heat changed from 31 kJ/mol to 22 kJ/mol. The heat of adsorption decreases with increasing adsorbed implied the adsorption system is heterogeneous.

總目錄
摘要I
ABSTRACT III
誌謝 V
總目錄VII
表目錄IX
圖目錄X
第一章 緒論1
第二章 基本原理與文獻回顧4
2-1溫室效應(Greenhouse effect)4
2-2二氧化碳捕獲系統簡介5
2-2-1燃燒後捕獲(Post-combustion capture)5
2-2-2燃燒前捕獲(Pre-combustion capture)6
2-2-3富氧燃燒捕獲(Oxy-fuel combustion capture)6
2-2-4化學迴圈燃燒(Chemical-looping combustion)8
2-3二氧化碳的捕獲技術簡介8
2-3-1吸收法(Absorption process)10
2-3-2吸附法(Adsorption process)11
2-3-3薄膜分離(Membrane separation)12
2-4二氧化碳再利用與封存技術13
2-4-1礦化封存13
2-4-2地質封存14
2-4-3海洋封存15
2-5中空纖維膜製備方法16
2-5-1擠壓成型法 ( Extrusion Molding )16
2-5-2有機模板法 ( Template method )16
2-5-3靜電紡絲法 ( Electrospinning )17
2-5-4相轉化法( Phase inversion )17
2-6固體吸附劑(Solid sorbents)18
2-6-1氧化鎂之簡介19
2-6-2氧化鎂之應用20
2-7吸附熱21
第三章 實驗方法與步驟25
3-1實驗藥品25
3-2實驗步驟與樣品製備26
3-2-1製備氧化鎂管吸附劑26
3-2-3水合氧化鎂管吸附劑29
3-2-4二氧化碳吸脫附效能測試30
3-3樣品物化特性鑑定31
3-3-1實驗設備31
3-3-2掃描式電子顯微鏡(Scanning Electron Microscope, SEM)33
3-3-3 X光繞射儀(X-ray Diffractometer, XRD)34
3-3-4熱重損失分析儀 (Thermogravimetry Analyzer, TGA)36
3-3-5全自動比表面與孔隙度分析儀37
3-3-6傅立葉轉換紅外光譜儀(FT-IR)39
3-3-7核磁共振光譜儀(NMR)42
第四章 實驗結果與討論43
4-1氧化鎂管二氧化碳吸附劑43
4-1-1樣品表面形態分析43
4-1-2 XRD分析48
4-1-3 BET分析49
4-1-4 FTIR 分析52
4-1-5二氧化碳吸附效能測試54
4-2水合法改善氧化鎂管59
4-2-1樣品表面型態分析59
4-2-2 XRD分析64
4-2-3 BET分析66
4-2-4 FTIR分析68
4-2-5 NMR分析71
4-2-6二氧化碳吸附效能測試74
4-2-7吸附熱分析80
第五章 結論81
第七章 參考文獻83


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