本研究的目的是開發出適合的金屬-有機框架材料 (metal-organic framework, MOF) 衍生觸媒材料，可用以催化甲烷雙重組：甲烷乾式重組反應結合甲烷蒸氣重組反應，以生成可調控H2/CO比例之合成氣。
第一部份研究中，我們利用傳統含浸法或溶劑熱沉積法，將鎳擔載在高度多孔的鈰 (IV) 基金屬有機框架 (MOF) 中，並通過碳化摻鎳的Ce-MOF-808製備NiCeO2@C用於甲烷雙重組反應。結果顯示，MOF衍生觸媒材料可以在較低溫度下催化BRM，並且與傳統含浸法相比，使用自限性後修飾在Ce-MOF中安裝空間分散的鎳位點可以有效地延緩鎳在長時間催化BRM時的燒結現象。這項研究表明，使用MOF衍生材料作觸媒催化甲烷雙重組反應是可行的，並且利用自限性安裝活性物質在MOF中有利於設計更耐燒結的MOF衍生催化劑。
第二部分研究中，我們成功利用氣溶膠式技術合成出MOF材料，Ni/ZIF-8@Al2O3，並藉由二次煅燒後獲得NiZnAl-H樣品作為觸媒材料用以催化甲烷雙重組反應。在甲烷雙重組反應方程式係數比為進料比例進行活性測試，並且利用不同進料比例在650 °C進行10小時的穩定性測試。結果表明，此觸媒擁有良好的活性結果和10小時內的相當穩定催化活性。此外，也證實了反應物中加入水蒸氣確實能有效抑制積碳生成速率，預防觸媒失活，並且藉由調整進料比例，可調控H2/CO比率。然而，由於鋅的低沸點特性，此觸媒不適合於過高的溫度下進行催化，並且其無法完全抑制低溫區間的水煤氣反應，故二氧化碳轉化率在低溫下依然呈現些微負轉化。
本研究提供了運用MOF製備混成式奈米結構材料以及運用甲烷雙重組反應之可行性，對於CO2再利用技術提供一有效途徑。

The objective of this study is to develop suitable MOF-derived catalyst materials for bi-reforming of methane (BRM), which combines dry reforming of methane and steam reforming of methane.
In the first part of the work, we incorporate the catalytically active nickel into a highly porous cerium(IV)-based metal-organic framework (MOF), by utilizing conventional impregnation or self-limiting post-synthetic modification. The nanosized MOF-derived ceria-supported nickel prepared by carbonizing the nickel-incorporated Ce-based MOF is used as catalyst for the bi-reforming of methane (BRM). The results show that the presence of MOF-derived carbon is necessary to initiate the BRM at a lower temperature, and compared to the conventional impregnation, the use of post-synthetic modification to install the spatially separated nickel sites in the parent MOF can effectively retard the agglomeration of nickel in the final MOF-derived catalyst during the long-term BRM. Findings here suggest that the feasibility of using MOF-derived materials as catalysts for bi-reforming of methane. Besides, the use of post-synthetic modification to install the catalytically active species in MOFs is beneficial for designing the MOF-derived catalysts that are more resistive to sintering.
In the second part of the study, we successfully synthesize MOF materials, Ni/ZIF-8@Al2O3, using a facile aerosol-based method to obtain NiZnAl-H samples as catalysts for BRM through two-step calcination. The activity of the catalyst is evaluated under the stoichiometric feed ratio of BRM. Furthermore, stability tests are performed at 650 °C for 10 hours using different feed ratios. The results demonstrate that this catalyst exhibited high activity and maintained considerable catalytic stability within the 10-hour testing period. In addition, the presence of steam is proven to effectively suppress the carbon deposition rate of the dry reforming, preventing catalyst from deactivation. Besides, adjusting the feed ratio enables the modulation of the H2/CO ratio. However, due to the low boiling point of zinc, this catalyst is not suitable for catalysis at excessively high temperatures. The negative conversion of CO2 is still identified due to the insufficient suppression of the water-gas shift reaction in the low-temperature range by the catalysts.
This study demonstrates the feasibility of employing MOFs for preparing hybrid nanostructured materials and the utilization of methane bi-reforming, which offers a promising approach towards the development of CO2 utilization technologies.

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