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研究生: 廖梓榆
LIAO, TZU-YU
論文名稱: 碳捕捉耦合催化過濾系統中多污染物氧化還原協同調控機制
Redox Mechanisms of synergetic Control for Multiple pollutants by A Catalytic Filtration—Carbon Capture System
指導教授: 林聖倫
Lin, Sheng-Lun
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: 2026
畢業學年度: 114
語文別: 中文
論文頁數: 93
中文關鍵詞: 催化過濾碳捕捉NOxPCDD/FsUiO-66超音波霧化氧化還原協同
外文關鍵詞: Catalytic filtration, Carbon capture, NOx, PCDD/Fs, UiO-66, Ultrasonic
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  • 隨著淨零排放政策與空氣污染標準加嚴,焚化煙氣控制逐漸由單一污染物處理轉向碳排放與多污染物同步治理。本研究建立超音波霧化碳捕捉耦合催化過濾系統,探討低溫煙氣條件下CO₂、NOx與戴奧辛類污染物(polychlorinated dibenzo-p-dioxins and dibenzofurans, PCDD/Fs)之同步控制潛力,並比較不同催化劑金屬組成與載體結構對氧化還原協同反應之影響。
    催化過濾部分以BK、V/W/TiO₂、V/W@UiO-66及Ce/W@UiO-66作為測試材料,比較不同操作溫度、活性金屬組成與載體結構對NOx還原與PCDD/Fs氧化之影響,並透過氣相/粒相分布、單位粒狀物(Particle Matter, PM)上PCDD/Fs負載及氯數同系物組成變化,區分污染物之物理捕集、吸附/脫附與實質催化降解行為。結果顯示以金屬有機骨架材料(Metal-Organic Frameworks, MOFs)作為載體可提供較高比表面積與孔隙結構,其中V/W@UiO-66於NOx與PCDD/Fs協同控制上展現較佳平衡性;然而Ce/W@UiO-66雖具Ce⁴⁺/Ce³⁺循環與氧空位潛力,其PCDD/Fs去除效果未能有更佳的表現;考量到高比表面積之載體未能絕對提升催化過濾整體效果。
    碳捕捉部分則以氫氧化鈣(Ca(OH)₂)、碳酸鉀(K₂CO₃)與飛灰洗滌水作為鹼性吸收液,評估其於CO₂捕捉效率與操作穩定性。結果顯示,Ca(OH)₂於高pH條件下具有較高短期吸收能力,但易受CaCO₃沉澱影響而產生操作波動;K₂CO₃則因可逆碳酸鹽/碳酸氫鹽反應特性,展現較穩定之吸收行為,較具長時間操作潛力;飛灰洗滌水則具資源再利用潛力,但其吸收表現受鹼性來源與溶出成分影響,仍需進一步優化。
    整體而言,初步證實碳捕捉耦合催化過濾系統應用於焚化煙氣多污染物同步控制之可行性,並指出催化性能並非僅由載體比表面積決定,而需同時考量金屬功能、載體結構、活性位點與污染物相分布行為。上述結果可作為後續低溫多污染物協同控制材料設計與整合式煙氣處理系統發展之參考。

    This study evaluated a carbon capture–coupled catalytic filtration system for the simultaneous control of CO₂, NOx, and PCDD/Fs in low-temperature incineration flue gas. The main objectives were to examine how catalyst composition, support structure, and operating temperature affect NOx reduction and PCDD/Fs oxidation, and to compare the CO₂ capture performance of different alkaline absorbents under ultrasonic atomization.
    Blank filter material, commercial V/W/TiO₂, V/W@UiO-66, and Ce/W@UiO-66 were tested in the catalytic filtration system. The catalysts were characterized by SEM, EDS, BET,XRD, and XPS. NOx removal was evaluated under NH₃-SCR conditions, while PCDD/Fs removal was assessed using total concentration, toxic equivalent concentration, gas/particle-phase distribution, PM-bound PCDD/Fs loading, and homologue profiles. CO₂ capture was tested using atomized Ca(OH)₂, K₂CO₃, and fly ash washing water.
    The results showed that UiO-66 improved metal dispersion and pollutant contact through its porous structure. V/W@UiO-66 showed the most balanced performance for NOx and PCDD/Fs control. For CO₂ capture, Ca(OH)₂ provided strong short-term absorption but was affected by CaCO₃ precipitation, whereas K₂CO₃ showed more stable behavior. Overall, the proposed system shows preliminary potential for integrated multi-pollutant flue gas treatment.

    摘要 i Extended Abstract ii 誌謝 vi 目錄 vii 表目錄 ix 圖目錄 x 1 第一章 緒論 1 1.1 研究背景 1 1.2 研究目的與動機 2 2 第二章 文獻回顧 3 2.1 固定污染源多污染物與碳排放控制需求 3 2.1.1 淨零趨勢與固定污染源碳排議題 3 2.1.2 焚化/燃燒系統污染特性 4 2.2 焚化煙氣控制技術與催化過濾發展 9 2.2.1 現有空氣污染防制設施(Air Pollution Control System , APCS) 9 2.2.2 催化過濾技術 9 2.2.3 多污染物協同處理之機制與挑戰 11 2.3 催化劑組成與載體結構 14 2.3.1 酸性位與氧化還原位於協同控制中的角色 14 2.3.2 鈰基(Ce-based)催化劑作為改質方向 16 2.3.3 MOF材料作為催化劑載體 17 2.4 燃燒後碳捕捉(Post-Combustion Capture, PCC)技術與強化策略 19 2.4.1 碳捕捉技術與應用限制 19 2.4.2 化學吸收法—鹼液吸收CO₂ 23 2.4.3 霧化吸收技術 25 3 第三章 研究方法與設備 27 3.1 研究架構與概述 27 3.2 實驗材料與方法 27 3.2.1 催化過濾 27 3.2.2 超音波霧化碳捕捉 36 3.3 各項污染物檢測與分析 40 4 第四章 結果與討論 41 4.1 催化劑表徵測定結果 41 4.1.1 粉末SEM 41 4.1.2 粉末BET/XRD測定 42 4.1.3 催化濾材SEM/EDS 44 4.1.4 催化劑XPS物種能階測定 46 4.2 催化過濾對多污染物控制成效 49 4.2.1 傳統污染物去除成效-氮氧化物(NOx) 49 4.2.2 PCDD/Fs去除成效 52 4.2.3 綜合削減效果 60 4.3 超音波霧化碳捕捉 63 4.4 碳捕捉與催化過濾單元之耦合關係評估 66 5 第五章 結論與建議 68 5.1 結論 68 5.2 建議 68 6 參考文獻 70

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