米冠杰,李建伟,范卓,陈标华

• 1:北京化工大学化工资源有效利用国家重点实验室

摘要(Abstract)：

根据实验现象和对积炭物组成进行的GC-MS分析结果,提出了N2O和苯在Fe-ZSM-5分子筛催化剂上进行催化氧化反应的的失活动力学模型,即产物苯酚引起的连串失活。采用固定床积分反应器系统测定了由催化剂失活引起的N2O转化率随运行时间的变化,所得实验数据用于失活动力学模型参数估值。模型表明:较低反应温度和苯相对N2O过量都可减缓催化剂的失活速率。模型统计检验表明:所得失活动力学方程在显著性水平α=0.05下有较高的拟合精度和可信度。该模型对深入了解N2O一步氧化苯制苯酚反应及指导反应器和再生器设计均具有重要的意义。

关键词(KeyWords)： N2O;苯;苯酚;Fe-ZSM-5催化剂;失活动力学

Abstract:

Keywords:

基金项目(Foundation): 国家杰出青年科学基金(20625621)

作者(Author): 米冠杰,李建伟,范卓,陈标华

参考文献(References)：

• [1]LI Yu-fang(李玉芳).Production technique progress for phenol at home and oversea(国内外苯酚生产技术进展)[J].China Petroleum and Chemical Industries(中国石油和化工),2004,12(8):40-42.
• [2]Reitzmann A,Klemm M,Emig G.Kinetics of the hydroxylation of benzene with N2O on modified ZSM-5zeolites[J].J Chem Eng,2002,90(1-2):149-164.
• [3]Hiemer U,Klemm E,Scheffler F et al.Microreaction engineering studies of the hydroxylation of benzene with nitrous oxide[J].J Chem Eng,2004,101(1-3):17-22.
• [4]Batholomew C H.Catalyst deactivation[J].J Chem Eng,1984,91(23):96-117.
• [5]XU Ou-guan(徐欧官),SU Hong-ye(苏宏业),JIN Xiao-ming(金晓明)et al.Kinetic model for hydroisomerization reaction of C8-aromatics(八碳芳烃临氢异构化反应动力学模型)[J].J Chem Eng of Chinese Univ(高校化学工程学报),2007,21(3):429-435.
• [6]ZHANG Li-chang(张立昌),XU Xian-kun(许先焜),WENG Hui-xin(翁惠新).Hydrodemetallization kinetic model for Maoming’s residue hydrodesulfurization treatment unit(渣油加氢脱金属动力学模型研究)[J].J Chem Eng of Chinese Univ(高校化学工程学报),2006,20(2):227-232.
• [7]ZHANG Xian-guo(张宪国).Preparation and Performance Analysis on the Catalysts of One-Step Oxidation of Benzene to Phenol with Nitrous Oxide(N2O一步氧化苯制苯酚的催化剂研制与性能分析)[D].Beijing(北京):Beijing University of Chemical Technology(北京化工大学),2006.
• [8]Levenspiel O.Chemical Reaction Engineering,2nd ed[M].London:Wiley and Sons,1972.
• [9]GUO Quan-hui(郭泉辉).The Study of N2O Catalytic Decomposition and One-Step Oxidation Benzene to Phenol over Zeolites(分子筛上N2O催化分解及其一步氧化苯制苯酚的研究)[D].Beijing(北京):Beijing University of Chemical Technology(北京化工大学),2007.
• [10]Pirutko L V,Chernyavsky V S,Uriarte A K et al.Oxidation of benzene to phenol by nitrous oxide:Activity of iron in zeolite matrices of various composition[J].Appl Catal A:Gen,2002,227(1/2):143-157.
• [11]TENG Su-zhen(滕素珍),FENG Jing-hai(冯敬海).Mathematical Statistics(数理统计学)[M].Dalian(大连):Dalian University of Technology Press(大连理工大学出版社),2005.