Ce-MOFs衍生物CeO2的制备及其催化CO2和甲醇合成碳酸二甲酯的性能

Preparation of Ce-MOFs derivatives CeO2 catalysts and performance in the synthesis of dimethyl carbonate from CO2 and methanol

  • 摘要: 采用水热法合成了Ce-MOF-808、Ce-UiO-66和Ce-BTC,然后在不同温度下热解制得Ce-MOFs对应的衍生物CeO2,并用于催化CO2和甲醇制备碳酸二甲酯(DMC)。利用XRD、N2等温吸脱附测试、SEM、NH3-程序升温脱附(TPD)、CO2-TPD和XPS等技术对催化剂的结构性质进行了表征。在450℃下热解的3种Ce-MOFs衍生物CeO2均表现最高的氧空位浓度以及催化活性,其中CeO2-BTC-450的活性最好,DMC时空收率为1.77 mmol·g−1·h−1。本研究提出了一种利用Ce-MOFs作为前驱体来制备高氧空位浓度的CeO2基催化剂的策略。

     

    Abstract: Ce-MOF-808, Ce-UiO-66 and Ce-BTC were synthesized by hydrothermal method. Then derivatives CeO2 corresponding to Ce-MOFs was prepared by pyrolysis at different temperatures. Finnally CeO2 was used as catalyst for synthesis of dimethyl carbonate (DMC) from CO2 and methanol. The samples were characterized by XRD, N2 isothermal adsorption and desorption, SEM, NH3-temperature programmed desorption (TPD), CO2-TPD and XPS. All the Ce-MOFs derivatives CeO2 catalysts which pyrolysis at 450℃ exhibited the highest relative oxygen vacancy concentration as well as catalytic activity. Among them, CeO2-BTC-450 showed the best catalytic activity with a DMC space-time yield of 1.77 mmol·g−1·h−1. In this study, a strategy to prepare CeO2-based catalysts with high oxygen vacancy concentration by using Ce-MOFs as precursor was proposed.

     

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