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Pd catalyst supported on CeO2 nanotubes with enhanced structural stability toward oxidative carbonylation of phenol

机译:CeO2纳米管上负载的Pd催化剂对苯酚的氧化羰基化具有增强的结构稳定性

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Ordered CeO _(2) nanotubes (CeO _(2) -T) were prepared via a hydrothermal synthesis process using the triblock copolymer polyethylene oxide-polypropylene oxide-polyethylene oxide (P123) as a morphology control agent. CeO _(2) -T characterization demonstrated the formation of single crystal structures having lengths between 1–3 μm and diameters < 100 nm. A supported Pd catalyst (Pd/CeO _(2) -T) was also prepared through hydrothermal means. H _(2) -temperature reduction profile and Raman spectroscopy analyses showed that the oxygen vacancies on the CeO _(2) surface increased and the reduction temperature of the surface oxygen decreased after Pd loading onto CeO _(2) -T. Pd/CeO _(2) -T was employed as a catalyst toward the oxidative carbonylation of phenol and the reaction conditions were optimized. Phenol conversion was 53.2% with 96.7% selectivity to diphenyl carbonate under optimal conditions. The integrity of the tubular CeO _(2) structure was maintained after the catalyst was recycled, however, both activity and selectivity significantly decreased, which was mainly attributed to the Pd active component significantly leaching during the reaction.
机译:使用三嵌段共聚物聚环氧乙烷-聚环氧丙烷-聚环氧乙烷(P123)作为形态控制剂,通过水热合成法制备有序的CeO_(2)纳米管(CeO_(2)-T)。 CeO _(2)-T表征证明形成了长度在1-3μm之间且直径<100 nm的单晶结构。还通过水热法制备了负载型Pd催化剂(Pd / CeO_(2)-T)。 H _(2)-温度降低曲线和拉曼光谱分析表明,在Pd负载到CeO _(2)-T上之后,CeO _(2)表面的氧空位增加,表面氧的还原温度降低。以Pd / CeO_(2)-T为催化剂,对苯酚进行氧化羰基化反应,优化了反应条件。在最佳条件下,苯酚的转化率为53.2%,对碳酸二苯酯的选择性为96.7%。催化剂回收后,管状CeO_(2)结构的完整性得以保持,但活性和选择性均显着降低,这主要归因于反应过程中Pd活性组分的明显浸出。

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