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系統識別號 U0026-1009201314315100
論文名稱(中文) 胺改質高嶺石捕捉二氧化碳之研究
論文名稱(英文) CO2 capture by amine modified kaolinite
校院名稱 成功大學
系所名稱(中) 地球科學系碩博士班
系所名稱(英) Department of Earth Sciences
學年度 101
學期 2
出版年 102
研究生(中文) 呂德隆
研究生(英文) De-Long Lu
學號 L46001117
學位類別 碩士
語文別 中文
論文頁數 120頁
口試委員 指導教授-陳燕華
口試委員-江威德
口試委員-許聯崇
口試委員-劉雅瑄
中文關鍵字 高嶺石  酸改質  胺根修飾  二氧化碳吸附 
英文關鍵字 kaolinite  acidic treatment  amine-modification  CO2 adsorption 
學科別分類
中文摘要 目前全球關注的一項重要議題為二氧化碳排放所造成的溫室效應問題,此溫室氣體導致全球暖化、氣候變遷,進而破壞整個生態圈的平衡,故如何降低大氣中二氧化碳的含量便是科學家們共同努力的目標。高嶺石為層狀的含鋁矽酸鹽類黏土礦物,是一種常見而便宜的天然材料。本研究之目的為:透過改質高嶺石以提高其比表面積;之後,於其上再披覆氨根,以進行二氧化碳吸/脫附實驗,期待此樣品可用來有效降低二氧化碳之濃度。
調變不同濃度的酸改質、不同改質時間等參數加以改質高嶺石;最佳酸改質參數為:3M硫酸、反應溫度95℃、反應10小時。比表面積由酸改質前之18.9 cm2/g,增為酸改質後之74.3 cm2/g。並以此酸改質高嶺石進行二氧化碳吸附實驗,以及二氧化碳多次循環之吸/脫附測試,其二氧化碳吸附效果最佳為3.3 mg/g。
利用酸改質後之高嶺石進行表面OH基潤飾,OH基潤飾使用的溶劑有NaOH以及H2O2,而以H2O2效果較優。之後以胺類MEA:EDA=4:1的比例進行胺之披覆實驗,實驗參數有:(1)有無OH基潤飾、(2)反應溫度、(3)胺/樣品重量比、(4)固液比等。胺根披覆的樣品以XRD、FTIR、BET進行特性分析,以熱重-熱差分析儀進行二氧化碳吸/脫附實驗,以及二氧化碳多次循環之吸/脫附測試。實驗結果顯示:未經OH基潤飾、反應溫度為室溫、胺/樣品重量比為1:1、固液比為1:10之改質參數,其吸附二氧化碳能力最佳為149 mg/g,且在10次二氧化碳吸/脫附循環後,其仍維持52 mg/g之吸附能力。由研究結果可得知:經胺根修飾之高嶺石確實具有潛力捕捉二氧化碳溫室氣體。
英文摘要 The CO2 emission to the atmosphere has gradually increased, and this green house gas results in the global warming and climate change. Therefore it is more important to reduce the CO2 discharge. Kaolinite, a cheap and common material, is the caly mineral with a layered structure of Si-O tetrahedral sheets and Al-O octahedral sheets. In this study, the surface area and porosity of kaolinites are enhanced by acidic treatment. After preparation, the acid-treated kaolinites are modified with amine. These samples are then performed with CO2 adsorption/desorption experiments to evaluate the ability of CO2 capture.
The best acidic treatment parameter is the concentration of 3 M H2SO4, reaction temperature of 95 ℃, reation time of 10 hr, which is tested by different H2SO4 concentrations and reaction time. The specific surface area is promoted from 18.9 to 74.3 m2/g after acidic treatment. Moreover, its CO2 adsorption efficiency is 3.3 mg/g.
Then kaolinites are modified with NaOH and H2O2 to promote the amount of OH group on the surface. The effect on OH group modification with H2O2 is better than that with NaOH. After that, kaolinites are modified with MEA and EDA to enhance the efficiency of CO2 adsorption. Some parameters of amine modification are discussed: (1) OH group modified or not, (2) reaction temperature, (3) the ratio of amine/sample, (4) the ratio of solid/liquid. The amine modified kaolinites are then analyzed by using XRD, FTIR, BET measurements. The CO2 adsorption/desorption and multiple reaction cycles of samples is examined by the thermo-gravimetric analyzer. It is observed that the best amine modified parameter to adsorb CO2 is the kaolinite without modification with NaOH, at room temperature, the ratio of amine/sample=1/1, the ratio of solid/liquid=1/10. And its CO2 efficiency is 149 mg/g, which has a good durability (52 mg/g) of CO2 adsorption/desorption with 10 cycles. From this study, it suggests the amine modified kaolinite is the potential adsorbent to capture CO2.
論文目次 第 一 章 緒論 1
第 二 章 研究背景 3
2-1二氧化碳研究背景 3
2-1-1 捕集 4
2-1-2 封存 6
2-2材料簡介 11
2-2-1高嶺石(kaolinite) 11
2-2-2 高嶺石之應用 12
2-3酸改質之研究 13
2-4胺根改質之研究 15
2-5基礎理論 19
2-5-1吸附劑與吸附質 19
2-5-2 sorption吸收與吸附 19
2-5-3吸附能力 19
2-5-4吸附種類 20
2-5-5吸附理論 21
2-5-6等溫吸附曲線 26
第 三 章 實驗方法 30
3-1 實驗藥品與設備 30
3-1-1 實驗藥品 30
3-1-2 實驗設備 31
3-2 儀器之原理 31
3-2-1 X光繞射儀 31
3-2-2 掃描式電子顯微鏡 32
3-2-3 比表面積分析儀 32
3-2-4 傅立葉轉換紅外線光譜儀 33
3-2-5 熱重-熱差分析儀 34
3-3 實驗流程 35
3-4 樣品處理 36
3-4-1 樣品優化改質方法 36
3-4-2 胺改質方法 39
3-4-3 二氧化碳吸附實驗 48
3-4-4 分析方法 49
第 四 章 結果與討論 50
4-1 酸改質高嶺石之分析 50
4-1-1 高嶺石之比表面積與孔洞分析 50
4-1-2 XRD分析 57
4-1-3 FTIR分析 58
4-1-4 表面形貌分析 61
4-1-5 熱穩定分析 64
4-1-6 二氧化碳吸附實驗 66
4-1-7二氧化碳後吸附後產物之分析 72
4-2 胺改質高嶺石之分析 75
4-2-1 胺改質高嶺石比表面積與孔洞分析 75
4-2-2 XRD分析 82
4-2-3 FTIR分析 84
4-2-4 表面形貌分析 89
4-2-5熱穩定分析 89
4-2-6 胺改質高嶺石之二氧化碳吸附實驗 90
4-2-7 多循環二氧化碳吸附實驗 102
4-2-8二氧化碳吸附後產物之分析 107
第 五 章 結論 109
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