因應全球暖化問題與日益嚴重的溫室氣體排放，如何有效減少大氣中的二氧化碳成為當前重要的研究課題。二氧化碳甲烷化反應是將溫室氣體二氧化碳轉化為甲烷的關鍵碳資源再利用技術，不僅有助於減緩氣候變遷衝擊，還能實現碳循環與能源儲存的雙重目標。固體觸媒的使用是推動此反應的重要策略，然而其活性往往受到金屬與載體之間界面結構的顯著影響。但目前針對此類界面結構的定量表徵方法仍相當有限，特別是在「反結構催化劑」的系統中。 本研究主要在探討 ZrO2/Ni 反結構催化劑系統中氧化物－金屬界面對二氧化碳甲烷化反應活性的影響，並提出的界面定量指標。為系統性研究不同界面結構的形成與活性關聯，本研究分別使用四種不同的製備方法含浸法、沉積沉澱法、溶膠-凝膠法、以及共沉澱法，合成了四種結構不同的 ZrO2/Ni 反結構催化劑。催化性能評估顯示，各催化劑在二氧化碳甲烷化反應下均展現出良好的低溫活性，顯示反結構催化劑的界面對於促進二氧化碳活化與氫化步驟扮演關鍵角色。為進一步釐清界面數量與催化活性的關係，本研究提出利用氫氣程序升溫還原分析的圖譜質心作為 ZrO2/Ni 反結構催化劑界面數量的指標。透過比較不同製備方法所得樣品的圖譜質心位置與其反應速率，發現兩者呈現高度正相關性，可以運用其預測反結構催化劑的反應速率。本研究的結果不僅驗證了 Ni–ZrO2 反結構催化劑界面對低溫二氧化碳甲烷化反應的促進效果，也為界面結構的定量評估提供了新的分析工具。利用氫氣程序升溫還原的圖譜質心作為界面指標的方法簡便易行，有助於未來催化劑界面設計與開發，對於深入理解氧化物－金屬界面在催化反應中的作用機制，以及發展高效低溫二氧化碳甲烷化催化劑，具有重要的學術與應用價值。 ;In response to the challenges of global warming and increasingly severe greenhouse gas emissions, effective reduction of atmospheric carbon dioxide has become a critical research focus. The CO2 methanation reaction is a key carbon resource recycling technology that converts greenhouse gas CO2 into methane, contributing not only to mitigating climate change but also achieving both carbon recycling and energy storage. The use of solid catalysts is an important strategy for promoting this reaction; however, their activity is often significantly influenced by the interfacial structure between the metal and the support. Currently, there is a lack of quantitative characterization methods for such interfacial structures, especially in so-called “inverse catalyst” systems. This study investigates the effect of the oxide－metal interface on the activity of ZrO2/ Ni inverse catalysts in the CO2 methanation reaction and proposes a quantitative interfacial descriptor. To systematically study the relationship between different interfacial structures and catalytic activity, four distinct preparation methods：impregnation, deposition–precipitation, sol–gel, and co-precipitation were employed to synthesize ZrO2/Ni inverse catalysts with varied structures. Catalytic performance evaluations demonstrated that all catalysts exhibited good low-temperature activity for CO2 methanation, indicating that the inverse catalyst interface plays a critical role in facilitating CO2 activation and hydrogenation.To further clarify the relationship between interfacial quantity and catalytic activity, this study proposes using the peak centroid of hydrogen temperature-programmed reduction (H2-TPR) profiles as an indicator of the interfacial quantity in ZrO2/Ni inverse catalysts. By comparing the TPR centroid positions of samples prepared by different methods with their reaction rates, a strong positive correlation was observed, suggesting its potential to predict the reaction rate of inverse catalysts. The results of this study not only verify the promoting effect of Ni–ZrO2 interfaces on low-temperature CO2 methanation but also provide a new analytical tool for quantitative interfacial evaluation. The use of the H2-TPR peak centroid as a simple and practical interfacial descriptor offers valuable guidance for future catalyst interface design and development. It also contributes to a deeper understanding of the role of oxide–metal interfaces in catalytic reactions and supports the development of efficient low-temperature CO2 methanation catalysts with significant academic and practical value.
