| H2O2氧化苯一步羟基化制备苯酚连续流动反应体系 |
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| 引用本文： | 张丽,刘慧慧,李桂英,胡常伟.H2O2氧化苯一步羟基化制备苯酚连续流动反应体系[J].化学物理学报,2012,25(5):585-591. |
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| 作者姓名： | 张丽 刘慧慧 李桂英 胡常伟 |
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| 作者单位： | 四川大学化学学院绿色化学与技术教育部重点实验室，成都610064;四川大学化学学院绿色化学与技术教育部重点实验室，成都610064;四川大学化学学院绿色化学与技术教育部重点实验室，成都610064;四川大学化学学院绿色化学与技术教育部重点实验室，成都610064 |
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| 摘 要： | 采用连续流动反应器研究了苯一步羟基化制备苯酚的反应. 利用载铁活性炭为催化剂，H2O2为氧化剂，乙腈为溶剂，得到苯酚收率为28.1%，选择为98%，基于铁计算的转化数为3 h-1. 对催化剂进行N2吸附、XRD、XPS、FTIR等表征发现，负载的Fe可能与活性炭表面羧基发生作用，形成了化学环境类似于乙酸铁的铁物种，该结构是催化反应的活性中心. 计算得出，反应的阿伦尼乌斯活化能为13.4 kJ/mol，苯和H2O2的反应级数分别为0.2和0.7，总反应级数约为1.
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| 关 键 词： | 连续流动体系，过氧化氢，催化活性，羧基，苯酚 |
| 收稿时间： | 4/2/2012 12:00:00 AM |
Continuous Flow Reactor for Hydroxylation of Benzene to Phenol by Hydrogen Peroxide |
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| Li Zhang,Hui-hui Liu,Gui-ying Li and Chang-wei Hu.Continuous Flow Reactor for Hydroxylation of Benzene to Phenol by Hydrogen Peroxide[J].Chinese Journal of Chemical Physics,2012,25(5):585-591. |
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| Authors: | Li Zhang Hui-hui Liu Gui-ying Li and Chang-wei Hu |
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| Institution: | Key Laboratory of Green Chemistry and Technology, Ministry of Education; College of Chemistry, Sichuan University, Chengdu 610064, China;Key Laboratory of Green Chemistry and Technology, Ministry of Education; College of Chemistry, Sichuan University, Chengdu 610064, China;Key Laboratory of Green Chemistry and Technology, Ministry of Education; College of Chemistry, Sichuan University, Chengdu 610064, China;Key Laboratory of Green Chemistry and Technology, Ministry of Education; College of Chemistry, Sichuan University, Chengdu 610064, China |
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| Abstract: | The direct hydroxylation of benzene to phenol catalyzed by activated carbon-supported Fe (Fe/AC) in acetonitrile using H2O2 as the oxidant was studied in a continuous flow reactor. Results showed that the continuous operation could obtain high phenol yield of 28.1%, coupled with the turnover frequency of 3 h-1, and high selectivity of 98% under mild condition. The catalyst was characterized by N2 adsorption/desorption, Boehm titration, X-ray photoelectron spectra, and Fourier transform infrared spectroscopy. It was observed that iron may interact with the carboxyl group forming iron-carboxylate like species, which act as the active phase. The apparent activation energy obtained by fitting an Arrhenius model to the experimental data was 13.4 kJ/mol. The reaction order was calculated to be about 1, 0.2 for benzene and 0.7 for H2O2. |
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| Keywords: | Continuous flow reactor Hydroxylation Activated carbon Iron-carboxylate Active phase Activation energy |
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