在本研究的第一部分中，展示了一種基於氣溶膠的連續合成金屬有機框架（MOF）衍生材料的方法，並結合實時氣相電泳進行材料表徵，用於製備通過CO2和CO聯合氫化反應生產甲醇的混合催化劑。以銅基（HKUST-1）和鋅基（ZIF-8）MOF膠體為模板，合成了兩種負載在Al2O3或CeO2上的Cu-ZnO催化劑。結果表明，差動遷移分析（DMA）的結合實現了氣溶膠MOF衍生材料的實時分析，從而增強了連續生產的可追溯性。在甲醇生產中，可以實現90.52%的最佳選擇性和7.50 mmol．gcat-1h-1的時空產率。甲醇的時空產率顯示出與催化材料的金屬表面積成線性關係，其中具有較高表面積的Al2O3負載樣品表現出比CeO2負載樣品更高的催化活性。本研究展示了通過氣溶膠相合成和實時表徵實現MOF衍生混合催化劑材料連續生產的重大進展。所開發材料在CO2和CO聯合氫化生成甲醇中的高催化性能在CO2利用領域具有應用前景。
在本研究的第二部分中，鑑於對可持續化學過程的迫切需求，本研究介紹了一種創新的一鍋反應系統，該系統有效地將溫室氣體轉化為甲醇，同時將聚對苯二甲酸乙二醇酯（PET）轉化為對苯二甲酸二甲酯（DMT）和乙二醇（EG）。我們的方法核心在於使用氣溶膠輔助合成方法開發由金屬有機框架（MOF）衍生的混合材料。這些催化劑具有在不同載體上調諧的Cu/ZnO活性相，專為一氧化碳（CO）和二氧化碳（CO2）的氫化而設計。本研究證實，將PET甲醇解與（CO2+CO）氫化過程相結合，顯著提高了2.5倍的轉化率，從而顯著增強了碳減排效果。這些催化劑的優異性能在優化條件下實現了5.57 mmol．gcat-1h-1的時空產率和92.35%的DMT選擇性。這些結果不僅突顯了MOF衍生材料在促進複雜化學轉化中的多功能性，還對環境可持續性做出了重要貢獻。這種雙功能系統為塑料廢物和溫室氣體的利用提供了實際解決方案，體現了向循環經濟原則邁進的重要一步。

In the first part of this study, a continuous aerosol-based synthesis of metal-organic framework (MOF) derived materials, in combination with real-time gas-phase electrophoresis for material characterization, is demonstrated for the preparation of hybrid catalyst used in methanol production via combined CO2 and CO hydrogenation reactions. Cu-based (HKUST-1) and Zn-based (ZIF-8) MOF colloids were prepared as the templates for the synthesis of two types of the Cu-ZnO catalysts supported on either Al2O3 or CeO2. The results show the incorporation of differential mobility analysis (DMA) enabled real-time analysis of aerosol MOF-derived materials, thereby enhancing traceability of continuous production. Optimal selectivity of 90.52%, and space-time yield of 7.50 mmol．gcat-1h-1 can be achieved toward methanol production. The space-time yield of methanol was shown to be linearly proportional to the metal surface area of the catalyst material, where the Al2O3-supported samples with a higher surface area possessed a higher catalytic activity than the CeO2-supported samples. This study demonstrated significant advances in the continuous production of MOF-derived hybrid catalyst materials through the aerosol-phase synthesis with real-time characterization. The high catalytic performance of the developed materials in the combined CO2 and CO hydrogenation to methanol bears promise for applications in the field of CO2 utilization.
In the second part of this study, driven by the urgent need for sustainable chemical processes, this study introduces an innovative one-pot reaction system that efficiently converts greenhouse gases into methanol while simultaneously processing polyethylene terephthalate (PET) into dimethyl terephthalate (DMT) and ethylene glycol (EG). The core of our approach involves the development of hybrid materials derived from metal-organic frameworks (MOFs) using an aerosol-assisted synthesis method. These catalysts, featuring a Cu/ZnO active phase on various support, are finely tuned for hydrogenation of both carbon monoxide (CO) and carbon dioxide (CO2). This study confirms that integrating PET methanolysis with the (CO2+CO) hydrogenation process significantly boosts their conversion rates by 2.5 times, thereby markedly enhancing the carbon reduction effect. The exceptional performance of these catalysts was highlighted by achieving a space-time yield of 5.57 mmol．gcat-1h-1 and selectivity of 92.35% for DMT production under optimized conditions. These results not only underscores the versatility of MOF-derived materials in facilitating complex chemical transformations but also makes a significant contribution to environmental sustainability. This dual-function system offers a practical solution for the utilization of plastic waste and greenhouse gases, embodying a pivotal step forward in the pursuit of circular economy principles.

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