催化学报

催化学报 ›› 2010, Vol. 31 ›› Issue (9): 1139-1144.DOI: 10.3724/SP.J.1088.2010.00131

• 研究论文 • 上一篇    下一篇

磷酸镍纳米管的合成及其催化环己烯环氧化反应性能

武光 1,2, 王安杰 1, 李翔 1, 王瑶 1, 胡永康 1   

  1. 1 大连理工大学精细化工国家重点实验室, 辽宁大连 116012 2 黑龙江大学化学化工与材料学院, 黑龙江哈尔滨 150080
  • 收稿日期:2010-09-30 出版日期:2010-09-30 发布日期:2014-01-25

Synthesis of Nickel Phosphate Nanotubes and Their Catalytic Performance for Cyclohexene Epoxidation

WU Guang1,2, WANG Anjie1,*, LI Xiang1, WANG Yao1, HU Yongkang1   

  1. 1State Key Laboratory of Fine Chemicals, Dalian University of Technology, Dalian 116012, Liaoning, China 2School of Chemistry and Material Sciences, Heilongjiang University, Harbin 150080, Heilongjing, China
  • Received:2010-09-30 Online:2010-09-30 Published:2014-01-25

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960

被引次数

13

摘要： 在不添加有机模板剂的情况下, 通过尿素缓慢分解调节局部 pH 值, 水热法合成了具有均一孔道直径的磷酸镍纳米管材料 (NiPO-NTs). 采用 N2 吸附-脱附、吡啶吸附红外光谱和氨程序升温脱附对材料进行了表征, 并将其用于催化 H2O2 氧化的环己烯反应中, 考察了反应条件对环氧化反应性能的影响. 结果表明, NiPO-NTs 具有狭窄的孔径分布, 比表面积为 96.6 m2/g, 其表面酸中心以弱 Lewis 酸为主. 该反应中以乙腈为溶剂较为适宜, 高温和高 H2O2/环己烯摩尔比有利于提高环己烯转化率; 而低温和高 H2O2/环己烯摩尔比有利于提高环氧环己烷选择性. 在 60 oC, H2O2/环己烯摩尔比为 3, 反应 6 h 时, 环己烯转化率可达 50.6%, 环氧环己烷选择性为 72.1%.

关键词: 磷酸镍, 纳米管, 尿素, 环己烯, 环氧化, 环氧环己烷

Abstract: Nickel phosphate nanotubes (NiPO-NTs) with a uniform pore size distribution were prepared by urea-assisted hydrothermal synthesis in the absence of any organic template. Calculations from N2 adsorption-desorption isotherms of NiPO-NTs revealed a narrow pore distribution around 2.7–4.2 nm and a surface area of 96.6 m2/g. NiPO-NTs was used to catalyze the epoxidation of cyclohexene using hydrogen peroxide as the oxidant. Infrared spectroscopy of adsorbed pyridine and NH3 temperature-programmed desorption characterization results showed that the weak Lewis acid was predominant on the surface of NiPO-NTs. CH3CN was found to be a suitable solvent for the epoxidation. The reaction conversion increased with increasing reaction temperature and H2O2/cyclohexene molar ratio, whereas the selectivity for epoxycyclohexane increased with decreasing temperature and increasing H2O2/cyclohexene molar ratio. High cyclohexene conversion (50.6%) and selectivity for epoxycyclohexane (72.1%) were obtained at 60 oC, 6 h, and H2O2/cyclohexene of 3.

Key words: nickel phosphate, nanotube, urea, cyclohexene, epoxidation, epoxycyclohexane