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LaCoO3钙钛矿氧化物的环己烯环氧化性能
石斌,章彬,张学龙,刘欢,钱洋慧,阮小云,李忠涛
(中国石油大学(华东)重质油国家重点实验室,山东青岛 266580)
摘要:
以硝酸钴和硝酸镧等为原料在碱性条件下共沉淀制备出LaCoO3钙钛矿复合氧化物,通过XRD、SEM、XPS及N2吸附-脱附等方法证实LaCoO3基本粒径为80~120 nm,比表面积为9.0 m2/g。在高压釜中以LaCoO3钙钛矿为催化剂,以氧气为氧源,研究以异丁醛为催化助剂、N,N-二甲基甲酰胺(DMF)为溶剂的环己烯环氧化过程。结果表明:在pH=8,20 ℃常温沉淀,焙烧温度为700 ℃和焙烧时间为4 h的条件下制备的LaCoO3钙钛矿复合氧化物催化剂的催化活性最高;在催化剂质量为0.2 g、环己烯质量为2.0 g、氧气压力为4 MPa、反应温度为50 ℃、反应时间为5 h的条件下,环己烯转化率达到64.9%,环氧环己烷的选择性达到68.6%。
关键词:  钙钛矿  环己烯  催化氧化  分子氧  沉淀  选择性
DOI:10.3969/j.issn.1673-5005.2021.02.019
分类号::TQ 426.8
文献标识码:A
基金项目:
Epoxidation of cyclohexene on LaCoO3 perovskite oxides
SHI Bin, ZHANG Bin, ZHANG Xuelong, LIU Huan, QIAN Yanghui, RUAN Xiaoyun, LI Zhongtao
(State Key Laboratory of Heavy Oil Processing in China University of Petroleum (East China), Qingdao 266580, China)
Abstract:
The LaCoO3 perovskite composite oxides were prepared with Co(NO3)2 and La(NO3)2 under alkaline condition by coprecipitation. The oxides were characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), N2 adsorption-desorption. It is found that the basic particle size of LaCoO3 perovskite is 80-120 nm and the specific surface area is 9.0 m2/g. The catalytic epoxidation of cyclohexene was conducted in an autoclave with LaCoO3 perovskite, O2 as oxidant, isobutyraldehyde as catalytic auxiliary, and N,N-dimethyl formamide (DMF) as solvent. The results show that the LaCoO3 perovskite prepared by coprecipitation could achieve the highest activity under the conditions of pH=8,20 ℃ of precipitation temperature, calcination temperature of 700 ℃ and calcination time of 4 h. The best catalytic epoxidation condition is O2 pressure 4 MPa, reaction temperature 50 ℃, reaction time 5 h with catalyst mass 0.2 g and cyclohexene mass 2.0 g. The conversion of cyclohexene and the selectivity of epoxycyclohexane could reach 64.9% and 68.6%, respectively.
Key words:  perovskite  cyclohexene  catalytic oxidation  molecular oxygen  precipitation  selectivity
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