以Y型沸石製備二氧化碳吸附及轉化之雙功能材料

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高佑丞(Yu-Cheng Kao) 查詢紙本館藏

畢業系所

化學工程與材料工程學系

論文名稱

以Y型沸石製備二氧化碳吸附及轉化之雙功能材料
(Preparation of Dual-Functional Materials for Carbon Dioxide Adsorption and Conversion Using Zeolite-Y)

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至系統瀏覽論文 (2029-7-31以後開放)

摘要(中)

隨著工業化的迅速發展，化石燃料的使用量急劇增加，導致溫室氣體排放量不斷上升，其中二氧化碳引發了全球變暖和氣候變化等多種環境問題。本研究參考一種新型的雙功能材料(DFMs)，該材料由擔體、吸附劑和還原觸媒組成，可以有效捕捉和轉化二氧化碳為合成天然氣(SNG)。由於這種材料的化學特性，二氧化碳可以很容易地被DFMs吸附，然後將由可再生能源生成的氫氣注入，促使吸附的二氧化碳分子溢出到觸媒位點並轉化為SNG。本研究將製備雙功能材料，利用SEM/EDS、mapping、BET、XRD及ICP探討材料之表面物理性質，並以熱重分析儀及固定床反應器/氣相分析儀瞭解材料之反應性能。以Y型沸石作為擔體含浸5%MgO後，其穩定平均二氧化碳吸附容量增至4.02*10-2 mmole CO2/g，較單純Y型沸石提高約9.83%。進一步含浸10%及20%還原觸媒後，穩定平均二氧化碳吸附容量分別提高至4.05*10-2 mmole CO2/g及4.63*10-2 mmole CO2/g，相對於5%MgO/Y型沸石含浸10%Ni還原觸媒MgO重量百分比減少至2.14%導致穩定平均二氧化碳吸附容量略增為0.75%，但隨著Ni還原觸媒含浸量增加至20%，使穩定平均二氧化碳吸附容量間接提升至15.17%。在還原甲烷化反應性能測試中，20%Ni-5%MgO/Y型沸石在320℃下具有最佳反應性能，二氧化碳轉化率為99.52%，甲烷選擇率為83.63%，甲烷產率為7.13%。而10%Ni-5%MgO/Y型沸石在相同條件下，甲烷產率提高至12.01%。以綜合性能的角度來看，20%Ni-5%MgO/Y型沸石是更具潛力的雙功能材料組合。

摘要(英)

With recent industrialization, the rapid increase in fossil fuel use has led to rising greenhouse gas emissions, particularly CO2, causing global warming and climate change. This study presents a new dual-functional material (DFMs) that combines an adsorbent and a catalyst to capture and convert CO2 into synthetic natural gas (SNG). The DFMs chemical properties allow for easy CO2 adsorption. Hydrogen gas from renewable sources is introduced to convert the adsorbed CO2 into SNG.
The study focuses on preparing DFMs and analyzing their surface properties using SEM/EDS, mapping, BET, XRD, and ICP. The reaction performance is assessed using a thermogravimetric analyzer and a fixed-bed reactor/gas chromatograph. Using Zeolite-Y as a support and impregnating it with 5%MgO increased its stable average CO2 adsorption capacity to 4.02*10-2 mmole CO2/g, approximately 9.83% higher than pure Zeolite-Y. Further impregnation with 10% and 20% catalysts increased the stable average CO2 adsorption capacity to 4.05*10-2 mmole CO2/g and 4.63*10-2 mmole CO2/g, representing increases of approximately 0.75% and 15.17% compared to 5%MgO/Zeolite-Y. Specifically, the 5% MgO/Zeolite-Y with a 10%Ni catalyst showed a slight increase in adsorption capacity by 0.75%, but with a 20% Ni catalyst, the capacity significantly increased by 15.17%.
In methanation reaction tests, the 20%Ni-5%MgO/Zeolite-Y showed the best performance at 320°C, with a CO2 conversion rate of 99.52%, methane selectivity of 83.63%, and a methane yield of 7.13%. Under the same conditions, the 10%Ni-5%MgO/Zeolite-Y achieved a methane yield of 12.01%. Overall, the 20%Ni-5%MgO/Y-type zeolite is the most promising dual-functional material combination.

關鍵字(中)

★ 二氧化碳捕捉
★ 甲烷化
★ 雙功能材料
★ 沸石

關鍵字(英)

★ Cabon dioxide capture
★ Methanenation
★ Dual-functional materials
★ Zeolite

論文目次

中文摘要 i
Abstract ii
致謝 iii
目錄 v
圖目錄 viii
表目錄 xii
第一章緒論 1
1-1 前言 1
1-2 研究動機 8
1-3 研究目的 11
第二章文獻回顧 12
2-1 碳捕捉途徑及技術 12
2-1-1 碳捕捉途徑 12
2-1-2 碳捕捉技術 15
2-2 碳利用轉化技術 22
2-3 吸附 23
2-3-1 吸附簡介 23
2-3-2 吸附的機制 24
2-3-3 影響吸附因素 26
2-4 沸石 27
2-4-1 沸石結構 27
2-4-2 沸石種類 29
2-4-3 沸石特性及應用 34
2-4-4 沸石為擔體之雙功能材料製備及其應用 36
2-5 還原觸媒 38
2-5-1 觸媒種類 38
2-5-2 影響觸媒活性因素 40
第三章實驗方法 43
3-1 研究流程 43
3-2 實驗藥品及設備 44
3-2-1 實驗藥品、氣體 44
3-2-2 實驗儀器設備 45
3-3 雙功能材料製備步驟 45
3-4 DFMs物理及化學性質分析 47
3-4-1 掃描式電子顯微鏡 (Scanning Electron Microscope, SEM) 47
3-4-2 能量散射光譜 (Energy Dispersive Spectrometer, EDS) 48
3-4-3 比表面積與孔隙分佈分析儀 (Specific Surface Area and Porosimetry Analyzer, BET) 48
3-4-4 熱重分析儀 (Thermogravimetric Analysis, TGA) 49
3-4-5 X光繞射儀 (X-ray Diffractometer, XRD) 49
3-4-6感應耦合電漿光學發射光譜儀 (Inductively Coupled Plasma Optical Emission Spectroscopy, ICP-OES) 49
3-4-7氣相層析儀(Gas Chromatography, GC) 49
3-5 DFMs反應性能實驗 50
3-5-1二氧化碳吸附實驗 50
3-5-2 二氧化碳還原甲烷化實驗 51
第四章結果與討論 53
4-1 DFMs物理特性分析 53
4-1-1 BET分析 53
4-1-2 SEM/EDS、Mapping分析 55
4-1-3 XRD分析 68
4-1-4 ICP分析 73
4-2 DFMs 反應性能測試 75
4-2-1 二氧化碳吸附 75
4-2-2 二氧化碳還原甲烷化 82
第五章結論 88
參考文獻 90

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指導教授

吳子嘉(Albert T. Wu)

審核日期

2024-8-13

推文