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MgFeCe Ternary Layered Double Hydroxide as Highly Efficient and Recyclable Heterogeneous Base Catalyst for Synthesis of Dimethyl Carbonate by Transesterification

机译:MgFece三元层状双氢氧化物作为高效且可回收的异质基础催化剂,用于通过酯交换合成碳酸二甲酯

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摘要

A series of Mg-3:Fe-x + Ce1-x LDHs (3:1) were synthesized by co-precipitation method by varying molar ratio of Fe:Ce between 1:0 to 0:1 (LDH-1 to LDH-6). All synthesized LDHs were characterized by XRD, FT-IR, TEM, N-2 sorption, benzoic acid titration and XPS in detail and evaluated for selective synthesis of dimethyl carbonate by transesterification of ethylene carbonate with methanol. It was demonstrated that the structural and basic properties of synthesized LDHs were strongly dependent on the Fe:Ce molar ratio (Ce concentration). The correlation between their physicochemical properties and catalytic performance was studied in detail. Among all synthesized LDHs the best result was obtained with LDH-3 (Fe:Ce = 0.85:0.15) where LDH structure remained intact, and showed high number of strong basic sites on LDH surface. LDH-3 was recycled 7 times while maintaining high catalyst activity and selectivity towards DMC. The obtained results elucidate the important role of Ce in modifying the basic properties of LDH in enhancing the catalytic activity for DMC synthesis.
机译:采用共沉淀法合成了一系列Mg-3:Fe-x+Ce1-x水滑石(3:1),改变Fe:Ce的摩尔比为1:0~0:1(LDH-1~LDH-6)。通过XRD、FT-IR、TEM、N-2吸附、苯甲酸滴定和XPS对所合成的LDH进行了详细的表征,并对碳酸乙烯酯与甲醇酯交换合成碳酸二甲酯的选择性进行了评价。结果表明,合成的LDH的结构和基本性能强烈依赖于Fe:Ce摩尔比(Ce浓度)。详细研究了它们的物理化学性质与催化性能之间的关系。在所有合成的LDH中,LDH-3(Fe:Ce=0.85:0.15)的效果最好,其中LDH结构保持完整,并在LDH表面显示出大量强碱性位点。LDH-3循环使用7次,同时保持较高的催化剂活性和对DMC的选择性。所得结果阐明了铈在修饰LDH的基本性质、提高DMC合成催化活性方面的重要作用。

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