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Continuous Flow Reactor for Hydroxylation of Benzene to Phenol by Hydrogen Peroxide
Li Zhang,Hui-hui Liu,Gui-ying Li*,Chang-wei Hu*
Author NameAffiliationE-mail
Li Zhang Key Laboratory of Green Chemistry and Technology, Ministry of Education; College of Chemistry, Sichuan University, Chengdu 610064, China  
Hui-hui Liu Key Laboratory of Green Chemistry and Technology, Ministry of Education; College of Chemistry, Sichuan University, Chengdu 610064, China  
Gui-ying Li* Key Laboratory of Green Chemistry and Technology, Ministry of Education; College of Chemistry, Sichuan University, Chengdu 610064, China gchem@scu.edu.cn 
Chang-wei Hu* Key Laboratory of Green Chemistry and Technology, Ministry of Education; College of Chemistry, Sichuan University, Chengdu 610064, China chwehu@mail.sc.cninfo.ne 
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.
Key words:  Continuous flow reactor, Hydroxylation, Activated carbon, Iron-carboxylate, Active phase, Activation energy
FundProject:
H2O2氧化苯一步羟基化制备苯酚连续流动反应体系
张丽,刘慧慧,李桂英*,胡常伟*
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.
关键词:  连续流动体系,过氧化氢,催化活性,羧基,苯酚
DOI:10.1088/1674-0068/25/05/585-591
分类号: