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Ce-MOFs衍生物CeO_(2)的制备及其催化CO_(2)和甲醇合成碳酸二甲酯的性能

Preparation of Ce-MOFs derivatives CeO_(2)catalysts and performance in the synthesis of dimethyl carbonate from CO_(2) and methanol
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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CeO_(2),并用于催化CO_(2)和甲醇制备碳酸二甲酯(DMC)。利用XRD、N_(2)等温吸脱附测试、SEM、NH_(3)-程序升温脱附(TPD)、CO_(2)-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CeO_(2)均表现最高的氧空位浓度以及催化活性,其中CeO_(2)-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CeO_(2)基催化剂的策略。 Ce-MOF-808,Ce-UiO-66 and Ce-BTC were synthesized by hydrothermal method.Then derivatives CeO_(2)corresponding to Ce-MOFs was prepared by pyrolysis at different temperatures.Finnally CeO_(2)was used as catalyst for synthesis of dimethyl carbonate(DMC)from CO_(2)and methanol.The samples were characterized by XRD,N_(2)isothermal adsorption and desorption,SEM,NH_(3)-temperature programmed desorption(TPD),CO_(2)-TPD and XPS.All the Ce-MOFs derivatives CeO_(2)catalysts which pyrolysis at 450℃exhibited the highest relative oxygen vacancy concentration as well as catalytic activity.Among them,CeO_(2)-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 CeO_(2)-based catalysts with high oxygen vacancy concentration by using Ce-MOFs as precursor was proposed.
作者 肖婉婧 李文杰 王馨雨 李心灵 Marc Pera-Titus 邓志勇 XIAO Wanjing;LI Wenjie;WANG Xinyu;LI Xinling;Marc Pera-Titus;DENG Zhiyong(Air Environmental Modeling and Pollution Controlling Key Laboratory of Sichuan Higher Education Institutes,ChinaSerbia"the Belt and Road"Joint Laboratory on Environment and Energy,College of Resources and Environment,Chengdu University of Information Technology,Chengdu 610225,China;Cardiff Catalysis Institute,School of Chemistry,Cardiff University,UK CF103AT)
出处 《复合材料学报》 北大核心 2025年第7期3844-3856,共13页 Acta Materiae Compositae Sinica
基金 四川省中央引导地方科技发展专项(2022ZYD0049,24ZYCXCP0031) 四川省科技计划(2021YFG0225,2024ZHCG0126)。
关键词 衍生物 碳酸二甲酯 CO_(2) 氧空位 酸碱位点 催化剂 derivatives DMC CO_(2) oxygen vacancy acid-base sites catalysts
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