纳微尺度铜金属有机框架催化过氧化氢氧化异丁香酚

doi:10.11944/j.issn.1000-0518.2016.10.150465

摘要/Abstract

摘要：

通过水热法及沉淀法,合成了纳微尺度铜金属有机框架催化剂。通过FT-IR、TG及TEM等技术手段对其性能和结构进行了表征。系统考察了催化剂、溶剂种类及用量、反应时间等因素对异丁香酚氧化制备香草醛的影响。结果表明,用均苯三甲酸根(BTC)作配体时制备的催化剂Cu-BTC性能较佳。以Cu-BTC为催化剂、30%(质量分数)H₂O₂为氧化剂、乙腈为介质,当n(异丁香酚):n(H₂O₂)=1:2.4时,50 ℃,反应8 h,异丁香酚转化率为94.4%,香草醛产率达到81.8%。纳微尺度(粒径30~300 nm)Cu-BTC催化剂体现了良好的重复使用性能,连续反应5次,异丁香酚转化率保持在90%左右。

关键词: 铜金属有机框架, 纳微尺度, 香草醛, 过氧化氢, 异丁香酚

Abstract:

Nano/microscale copper metal-organic framework(MOF) catalysts were synthesized via hydrothermal method or precipitation and characterized by FT-IR, TG and TEM, respectively. The effects of these catalysts, solvent, and reaction time on the oxidation of isoeugenol to vanillin were investigated. Cu-BTC containing BTC(1,3,5-benzenetricarboxylate) ligand is found to exhibit the best catalytic performance. When employing Cu-BTC as catalyst, 30%(mass fraction)H₂O₂ as oxidant, 94.4% conversion of isoeugenol and 81.8% yield of vanillin are achieved with n(isoeugenol):n(H₂O₂)=1:2.4 after 8 h reaction at 50 ℃ in acetonitrile. Additionally, nano/microscale Cu-BTC(diameter ca. 30~300 nm) exhibits good reusability and ~90% conversion of isoeugenol can be maintained in 5 recycles.

Key words: copper metal-organic framework, nano/microscale, vanillin, hydrogen peroxide, isoeugenol

肖毅, 杨晰雅, 姜小英, 史慧珍, 黄红梅, 尹笃林, 毛丽秋. 纳微尺度铜金属有机框架催化过氧化氢氧化异丁香酚[J]. 应用化学, 2016, 33(10): 1168-1174.

XIAO Yi, YANG Xiya, JIANG Xiaoying, SHI Huizhen, HUANG Hongmei, YIN Dulin, MAO Liqiu. Oxidation of Isoeugenol with Hydrogen Peroxide Catalyzed by Nano/Microscale Copper Metal-Organic Frameworks[J]. Chinese Journal of Applied Chemistry, 2016, 33(10): 1168-1174.

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