藉由二氧化碳的甲烷氧化重組反應，以減少溫室氣體二氧化碳，且轉化為合成氣極具有研發價值。本實驗以研發高性能的觸媒為目標，觸媒可用於部分甲烷氧化及二氧化碳的甲烷重組反應。前者放出的熱量可以提供重組反應所需熱能。針對此研究課題，研究分為兩部份。首先，參照Ce-Zr氧化物擔體與Ni-Mg-Al類水滑石製備參數加以改質，尋求最佳的製備條件和比例，並對改質後的觸媒進行活性測試，也對進料成份比的影響予以探討，挑選出活性最佳並具抗積碳能力的觸媒及反應條件。其次，將挑選出的觸媒進行各項物理及化學的鑑定，找出影響觸媒活性的主要因素與可能的反應機制。
本研究中，製備觸媒是以沈積沉澱法將多種改質類水滑石擔載於Ce-Zr氧化物擔體上，結果顯示：當Ni/Mg/Al=4/2/2時，Ni/Mg/Al-Ce0.75Zr0.25O2的活性最佳。在反應物的進料流速(GHSV)固定於105 l/kg.h，甲烷/二氧化碳/氧氣/氬氣比例為35/20/12.5/32.5的條件下，此觸媒在150℃即可引發甲烷的氧化反應，並部分生成CO和H2；且於550℃下，甲烷轉化率可達50%以上，且生成H2和CO的產率比値接近於1。另以反覆的觸媒試驗與長時間活性測試，發現此種觸媒擁有不錯的耐久性與穩定性，也具備抗積碳的能力。
最後，根據以上列觸媒所進行CH4-TPR與CO2-TPO的結果，對反應機制予以分析，並與轉化率-溫度曲線相比較，發現觸媒被甲烷還原與被二氧化碳氧化皆發生於相近的溫度，而且活性測試於此溫度範圍亦有極高轉化現象。根據這些事實，我們可以證實觸媒具有還原態與氧化態，而且二氧化碳的甲烷重組反應是遵循Mars-Van Krevelen 模式。

The process of methane oxidative reforming of carbon dioxide, which consumes two greenhouse gases and produces synthesis gas, is worth developing. The objective of this study, is to develop a catalyst with high catalytic activity for this reforming reaction. The catalysts can be used for both partial oxidation of methane and methane reforming of carbon dioxide. The former is an exothermic reaction and can supply heat energy for the reforming reaction. The research includes two parts. In the first part, the proper preparation parameters for Ce-Zr mixed oxide support and Ni-Mg-Al hydrotalcite-like catalyst were investigated and further improved. The activity tests of the improved catalysts were carried out and the effect of inlet ratio on the reaction rates and fractional yields of H2 and CO were explored. Moreover, the catalyst with the best performance and the highest coke resistance was picked up. In the next part, the physical and chemical properties of catalysts were characterized for elucidating their effects on the catalytic activity and reaction mechanism.
The Ce-Zr mixed oxide-supported hydrotalcite-like catalysts were prepared by deposition-precipitation method, the results show that a ratio of Ni/Mg/Al = 4/2/2 for Ni/Mg/Al-Ce0.75Zr0.25O2 catalyst gives the best activity. A gas mixture has the ratios of methane/carbon dioxide /oxygen /argon equal to 35/20/12.5/32.5 and the gas hourly space velocity of 105 l/kg.h feed to the packed bed reactor, the catalyst can ignite the partial oxidation of methane and produce CO and H2 at 150℃. The temperature for 50% conversion of methane is only about 550℃, and the stoichiometric ratio of synthesis gas with H2/CO is close to unit. Furthermore, the catalyst shows an excellent durability during a long time activity test. This fact suggests that this improved catalyst can impede carbon deposition and has a high stability.
Finally, because the results of CH4-TPR and CO2-TPO experiments reveal that the oxidation of methane and reduction of carbon dioxide come about the same temperature range, and the conversion-temperature curve shows that the reforming reaction takes place at the similar temperature range. We can conclude that the oxidized and reduced active sites coexist in the catalyst, and the reaction of methane reforming of carbon dioxide proceeds with the Mars-Van Krevelen mechanism.

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