| 摘要: | 由於溫室氣體效應和PM2.5的排放增加已導致全球暖化和海平面上升，減少二氧化碳排放已成為未來幾十年的重要目標。除了減少排放和推動替代能源外，利用二氧化碳生產產品或新材料是一種更有效且具前景的方法。
本研究採用二氧化碳與乙烷進行反應，透過乾重組與氧化脫氫反應生成乙烯和合成氣體（H2和CO）。在觸媒合成階段，採用了一步到位的蒸發誘導自組裝法（Evaporation-Induced Self-Assembly, EISA），成功合成了具有二維六角結構的有序介孔材料。此方法合成的觸媒具有大比表面積和高熱穩定性的優點，能使附載金屬高度分散在有序介孔通道中，有效延緩附載顆粒的遷移和聚集。並透過XRD、氮氣吸附-脫附實驗、HR-TEM、H2-TPR、CO2-TPD、NH3-TPD和XPS等方法對觸媒進行分析，確認成功合成了預期的介孔材料。本研究選用Fe和Ni作為附載金屬，其中Fe具有良好的氧化還原性能，Ni具有優異的催化活性，並選用具有良好熱穩定性的γ-Al2O3作為載體，透過一步到位的EISA方法，合成了不同Fe和Ni附載比例的xFe-yNi/Al2O3有序介孔金屬-氧化物觸媒。
本研究主要探討不同Fe-Ni比例的xFe-yNi/Al2O3有序介孔金屬-氧化物觸媒在不同反應條件下的影響。在活性測試中觀察到，更高的Ni附載比例促進乾重組反應，生成更多的合成氣體；而更高的Fe附載比例則可以增加觸媒的抗積碳能力。然而，在較高的反應溫度下，即使沒有觸媒，仍可觀察到乙烯的生成，這表明溫度是影響乙烷轉化為乙烯的主要因素。活性測試結果顯示，透過調整Fe和Ni的比例，可以在一定程度上控制生成產物的比例。
總結來說，我們利用EISA方法開發了介孔材料，並探討了Fe-Ni附載比例及附載量對反應的影響。這些結果將幫助我們更深入了解觸媒對反應的影響，從而優化觸媒的反應效果。
;Due to the increase in greenhouse gas effects and PM2.5 emissions, global warming and rising sea levels have become pressing issues. Reducing carbon dioxide emissions has become a crucial goal for the coming decades. In addition to reducing emissions and promoting alternative energy sources, utilizing carbon dioxide to produce products or new materials is a more effective and promising approach.
This study employs the reaction between carbon dioxide and ethane to produce ethylene and syngas (H2 and CO) through dry reforming and oxidative dehydrogenation reactions. During the catalyst synthesis phase, a one-step Evaporation-Induced Self-Assembly (EISA) method was used to successfully synthesize ordered mesoporous materials with a two-dimensional hexagonal structure. Catalysts synthesized by this method have the advantages of high surface area and thermal stability, allowing the metal to be highly dispersed in the ordered mesoporous channels, effectively delaying the migration and aggregation of metal particles. The catalysts were analyzed using XRD, nitrogen adsorption-desorption experiments, HR-TEM, H2-TPR, CO2-TPD, NH3-TPD, and XPS, confirming the successful synthesis of the expected mesoporous materials. Fe and Ni were selected as the supported metals for this study, where Fe exhibits good redox properties, and Ni demonstrates excellent catalytic activity. γ-Al2O3, with its good thermal stability, was chosen as the support. Through the one-step EISA method, xFe-yNi/Al2O3 ordered mesoporous metal-oxide catalysts with different Fe and Ni loading ratios were synthesized.
This study mainly investigates the impact of different Fe-Ni ratios in xFe-yNi/Al2O3 ordered mesoporous metal-oxide catalysts under various reaction conditions. In activity tests, it was observed that higher Ni loading promotes the dry reforming reaction, producing more syngas, while higher Fe loading increases the catalyst′s resistance to coking. However, at higher reaction temperatures, ethylene formation was observed even in the absence of a catalyst, indicating that temperature is a major factor influencing ethane conversion to ethylene. The activity test results show that by adjusting the Fe and Ni ratios, the proportion of the produced products can be controlled to some extent.
In summary, we developed mesoporous materials using the EISA method and investigated the effects of Fe-Ni loading ratios and amounts on the reaction. These results will help us gain a deeper understanding of the catalyst′s impact on the reaction, thereby optimizing the catalyst′s performance. |
