乙醇及硫酸鹽改質鋯、鈰氧化鋁基觸媒以提升 C4F8 之催化活性

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姓名

馬何莫(Amir Machmud) 查詢紙本館藏

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環境工程研究所

論文名稱

乙醇及硫酸鹽改質鋯、鈰氧化鋁基觸媒以提升 C4F8 之催化活性
(Enhancement of Catalytic Activity of Al2O3 for C4F8 Conversion via Modification with Zr, Ce, Ethanol, and Sulfate)

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摘要(中)

評估經鈰、鋯、硫酸鹽和乙醇改質的氧化鋁基觸媒在 ≤ 650oC 溫度下催化水解 C4F8 的效果。通過酸改質提升觸媒的表面積，並進一步研究稀土元素、酸量和表面積之間的相互作用。此後，進行穩定性測試以評估 ASE (乙醇及硫酸鹽改質 Al2O3 觸媒)、ACSE (乙醇及鈰改質Al2O3 觸媒) 和 AZSE (乙醇及鋯改質 Al2O3 觸媒) 對 C4F8 的轉化性能。穩定性測試結果表明，C4F8在650oC反應24h時的轉化性能ACSE>AZSE>ASE，同時，評估水氣和氧含量的耦合效應。總體而言，ACSE 觸媒在 650oC表現出良好的活性，在沒有水氣的情況下， 650oC 時催化熱解的最高轉化率為 9.56%，而在 550oC 和 38% H2O(g) 的條件下，催化水解的最高轉化率為 100%。此外，在 650oC 和 21% 的氧氣條件下，催化氧化的最高轉化率為 95%，而催化水解和氧化的耦合在 450oC 下實現了 91% 的 C4F8 轉化率。ACSE觸媒對C4F8之催化水解、熱解和氧化的活化能分別為67.2、60.1和79.9 kJ/mol。 C4F8 轉化後的主要產物包括 CO2、CO 和 COF2，同時也產生少量的CHF3、C2F4、C3F6O。本研究證實以鈰、硫酸鹽和乙醇對觸媒進行改質，可有效提高氧化鋁基觸媒轉化C4F8的活性和穩定性。

摘要(英)

The effectiveness of alumina-based catalysts modified by cerium, zirconium, sulfate, and ethanol in the catalytic hydrolysis of C4F8 at temperatures ≤ 650oC is evaluated. Modification of catalysts enhances the acid amount and surface area. The interplay among rare earth elements, acid amount, and surface area is further investigated. Thereafter, a stability test was carried out to evaluate the performance of ASE (sulfate-modified-Al2O3 catalysts), ACSE (cerium-modified-Al2O3 catalysts), and AZSE (zirconium-modified-Al2O3 catalysts) for C4F8 destruction. Ethanol was used to modify catalysts and is designated with the symbol (E). The results of the stability test show that the performances ACSE>AZSE>ASE for C4F8 conversion at 650oC during 24 h reaction. Coupling effects of water and oxygen content have been evaluated. Overall, the ACSE catalyst shows good performance at 650oC. The highest conversion by catalytic pyrolysis was 9.56 % at 650oC in the absence of water vapor. The highest conversion by catalytic hydrolysis was 100% at 550oC with 38% H2O(g). Furthermore, the highest conversion by catalytic oxidation was 95% at 650oC with 21% oxygen. Coupling of catalytic hydrolysis and oxidation achieves 91% C4F8 conversion at 450oC. The activation energies of ACSE catalysts in catalytic hydrolysis, pyrolysis, and oxidation are 67.2, 60.1, and 79.9 kJ/mol, respectively. The major products from C4F8 conversion include CO2, CO, and COF2. Small amounts of CHF3, C2F4, C3F6O were also identified as products. This study has confirmed that modifying alumina-based catalysts with cerium, sulfate, and ethanol improves the activity and stability of alumina-based catalysts for C4F8 conversion.

關鍵字(中)

★ 氧化鋁基觸媒
★ 活化能
★ 全氟化合物

關鍵字(英)

★ alumina-based catalysts
★ activation energy
★ C4F8

論文目次

Abstract...................................................................................................................I
Table of Content..................................................................................................III
List of Tables........................................................................................................ V
List of Figures......................................................................................................VI
Chapter 1 Preface ...............................................................................................1
1.1. Background and Motivation .....................................................................1
1.2. Purposes of the Research ..........................................................................3
Chapter 2 Literature Review ..............................................................................4
2.1. Contribution of PFCs as Greenhouse Gases ...............................................4
2.2. Usage of C4F8 ..............................................................................................7
2.3. Basic Physicochemical Characteristics of C4F8..........................................8
2.4. PFCs Treatment Technology.....................................................................10
2.5. Mechanism of Catalytic Abatement..........................................................13
2.6. The Kinetic Study of Plug Flow Reactor ..................................................16
Chapter 3 Experimental Design .......................................................................21
3.1. Material .....................................................................................................21
3.2. Thermal Catalytic System.........................................................................21
3.3. Catalyst Preparation, Characterization, and Gases ...................................23
3.4. Experimental Setup ...................................................................................25
3.5. The Equation Used in the study ................................................................27
Chapter 4 Results and Discussion ....................................................................28
4.1. Catalyst characterization ...........................................................................28
4.2. Thermal Pyrolysis of C4F8.........................................................................33
4.3. Effect of Ce and Zr addition on the activity of alumina-based catalyst ...34
4.4. Effect of SO4-2 addition on the activity of alumina-based catalyst...........36
4.5. Effect of adding CH3CH2OH on the activity of alumina-based catalyst ..37
4.6. Effect of adding CH3CH2OH and SO4-2 on the activity of alumina-based
catalyst..............................................................................................................38
4.7. Time-on-stream analysis ...........................................................................41IV
4.8. Effect of water content on C4F8 decomposition........................................44
4.9. Effect of oxygen content on C4F8 decomposition.....................................46
4.10. Effect coupling of catalytic hydrolysis and oxidation on the
decomposition of C4F8 .....................................................................................47
4.11. Kinetic study of ACSE catalyst...............................................................49
4.12. Removal mechanism and by-product formation.....................................51
Chapter 5 Conclusions and Recommendations................................................57
5.1. Conclusions ...............................................................................................57
5.2. Recommendations .....................................................................................58
References ...........................................................................................................59

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指導教授

張木彬(Chang Moo Been)

審核日期

2021-10-29

推文