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负载在CeO纳米管上的钯催化剂,对苯酚氧化羰基化具有增强的结构稳定性。

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

作者信息

Fu Zengjie, Wang Zhimiao, Wang Hongjuan, Li Fang, Xue Wei, Wang Yanji

机构信息

Hebei Provincial Key Laboratory of Green Chemical Technology & High Efficient Energy Saving, Tianjin Key Laboratory of Chemical Process Safety, Hebei University of Technology Tianjin 300130 China

出版信息

RSC Adv. 2019 Apr 11;9(20):11356-11364. doi: 10.1039/c8ra10090j. eCollection 2019 Apr 9.

Abstract

Ordered CeO nanotubes (CeO-T) were prepared a hydrothermal synthesis process using the triblock copolymer polyethylene oxide-polypropylene oxide-polyethylene oxide (P123) as a morphology control agent. CeO-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-T) was also prepared through hydrothermal means. H-temperature reduction profile and Raman spectroscopy analyses showed that the oxygen vacancies on the CeO surface increased and the reduction temperature of the surface oxygen decreased after Pd loading onto CeO-T. Pd/CeO-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 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.

摘要

通过水热合成法,以三嵌段共聚物聚环氧乙烷-聚环氧丙烷-聚环氧乙烷(P123)作为形貌控制剂制备了有序的CeO纳米管(CeO-T)。CeO-T表征显示形成了长度在1-3μm之间且直径小于100nm的单晶结构。还通过水热法制备了负载型Pd催化剂(Pd/CeO-T)。氢气程序升温还原曲线和拉曼光谱分析表明,在CeO-T上负载Pd后,CeO表面的氧空位增加,表面氧的还原温度降低。Pd/CeO-T用作苯酚氧化羰基化反应的催化剂,并对反应条件进行了优化。在最佳条件下,苯酚转化率为53.2%,碳酸二苯酯选择性为96.7%。催化剂循环使用后,管状CeO结构保持完整,然而活性和选择性均显著下降,这主要归因于反应过程中Pd活性组分的大量浸出。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/7070/9063361/75169385b753/c8ra10090j-f1.jpg

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