2026-11-092026-11-09https://scholars.csmu.edu.tw/handle/123456789/38668Because of the fast industry development, energy consumption, especial petroleum consumption, is increasing rapidly and air pollution becomes more and more serious. The greenhouse effect as a result of CO2 causes the raise of earth temperature and unusual weather phenomenon. Nowadays it is an important topic to find the way of CO2 reduction. The amount of carbon dioxide emission has to be cut down in the future due to global treaty (Kyoto Protocol, 200502). Though mitigation of the release of carbon dioxide is important, reuse of carbon dioxide is the following work that has to be done. For example, CO2 reforming of methane to syngas, which is suitable for Fischer-Tropsch synthesis, is a pratically important reaction for the utilization of the green-house gases (CO2 and CH4). In the previous studies, supported metal catalysts such as Rh, Ru, Ni, Pt, Pd, Ir, Co, and Fe are known as active catalysts for CO2 reforming. However, CO2 reforming catalysts still suffer from many disadvantages: (1) low selectivity; (2)low thermal stability; (3) water be easily condensed; (4) the participation of support in sulfation reaction is occurred;(5) high sensitive to carbon deposition. In the area of catalyst research, Al2O3, SiO2 and activated carbon were used as supports for catalyst preparation. The catalyst is defined as microporous catalyst with large specific surface area, and it shows the low catalytic activity for gaseous chemical reaction. Effective diffusion coefficients of gaseous molecules were decided by the porous diameter of the catalyst supports, while gaseous catalytic reaction. In the present case, the raising of average pore size diameter results: (1) the diffusion of metal precursors into the pores were improved during the catalyst preparation, and the active sites dispersion on the catalyst would be better; (2) the medium and small gaseous molecules were easily diffused into the pores to react with active sites, as a result the adsorption capacity of the catalyst was increases and the catalytic efficiency was enhanced. This research was mainly focused on the preparation of mesoporous catalysts, and compared the catalytic activity of carbon nanotube (CNT) supported catalyst with zeolite (SBA-15 ) supported catalyst. The activity tests of CO2 reforming over mesoporous catalysts were studied in the different operating condition, including reaction temperature, space velocity, and composition of reaction gas (CO2, CH4, and H2 ), and the catalyst with the best performance and coke resistance was picked up. In addition, the reaction mechanisms of CO2 reforming over mesoporous catalysts were studied. Characterization of catalyst was done to find their effect on the catalytic activity by using the techniques BET, XRPD, EA, FESEM, EDS, TEM, ICPMS, and FTIR.因工業快速地發展，使能源之消耗特別是石油消耗劇增，空氣污染也日益嚴重，二 氧化碳造成的溫室效應使得全球溫度不斷升高，全球各地的氣候異常，因此如何有效降 低大氣中二氧化碳的含量便成為重要的課題。二氧化碳的排放主要來自於石化工業的燃 燒，由於世界性公約(京都議定書)的限定，未來二氧化碳排放量勢必得較目前降低。減 緩二氧化碳排放量是首要工作，而將回收後的二氧化碳再生利用則是後續所需開發的工 作。例如，藉由二氧化碳甲烷重組反應即可將二氧化碳轉化為合成氣體供Fischer-Tropsch 合成反應所用同時也達到將二氧化碳再利用之目的。 由過往的研究發現，二氧化碳轉換觸媒使用之活性大多為VIII 族金屬(Rh、Ru、Ni、 Pt、Pd、Ir、Co、Fe)，然而於進行催化二氧化碳轉換反應過程中卻仍然會遭遇了許多問 題，如：低選擇率、低熱穩定性、水氣遮蔽效應、擔體硫酸化及高積碳性等缺點。目前 於觸媒的研究領域中，除氧化鋁外，僅有某些特定材質如氧化矽及活性碳等物質被使用 作為被擔持觸媒之擔體材質。綜觀這些擔體可發現大多為比表面積大且孔徑分布屬於微 孔的材質，然而就將觸媒應用於氣體催化反應而言，屬於微孔材質的觸媒並不適用，乃 因進行氣體催化反應時，氣體分子的有效擴散係數取決於擔體的孔隙半徑，因此若能增 加觸媒擔體的平均孔徑，將可: (1)提升觸媒製備過程中金屬前驅物離子於孔洞內的擴散 行為，提高活性相於擔體上的分散性; (2)增加反應用過程時對氣體分子的吸附能力，使 得中、大粒徑的氣體分子可以順利擴散至孔洞內與活性相進行催化反應，進而提升觸媒 的反應效率。因此，本研究採用新興中孔洞型奈米材料，將奈米碳管與SBA-15 使用為 擔體材料進行觸媒製備，比較SBA-15 沸石、奈米碳管等不同中孔洞結構擔體所組成的 觸媒之催化活性，探討反應溫度、氣體流率與氣體組成( CO2、CH4、H2 )等不同反應條 件對二氧化碳轉化反應之影響。對於中孔洞擔體觸媒進行活性測試，評估活性最佳並能 抗積碳的觸媒，並建立二氧化碳於奈米碳管與SBA-15 型中孔洞擔體觸媒上之再生反應 機制。並輔以BET、XRPD、EA、FESEM、EDS、TEM、ICPMS、FTIR 等進行物化特 性分析，以找出影響觸媒活性的原因。SBA-15 沸石奈米碳管溫室效應二氧化碳重組反應中孔洞擔體觸媒碳沉積SBA-15CNTgreenhouseCO2 reformingmesoporous catalystcarbondepositionProject