Kinetics of Synthesis of ETBE Over Mesoporous Molecular Sieve Catalys t SBA -15 -HSO3

Journal of Liaoning Petrochemical University ›› 2007, Vol. 27 ›› Issue (4): 27-30.

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Kinetics of Synthesis of ETBE Over Mesoporous Molecular Sieve Catalys t SBA -15 -HSO₃

1 .S chool of Petrochemical Engineering , Liaoning University o f Petroleum &Chemical Technology ,Fushun Liaoning 113001 , P .R .China;
2 .Lanz hou Petrochemical Company Research Institute of Chemical I nd ustry , Lanz hou Gansu 730060 , P .R .China

Received:2007-07-10 Published:2007-12-20 Online:2017-07-05

介孔分子筛SBA -15 -HSO₃ 合成ETBE 反应本征动力学研究

赵　昕¹ , 沈　健^{1 ＊} , 焦宏宇²

1.辽宁石油化工大学石油化工学院, 辽宁抚顺113001;
2.兰州石油化工公司研究院, 甘肃兰州730060

作者简介:赵昕(1982 -), 男, 北京市, 在读硕士。

Abstract

Abstract:

Well-ordered meso porous organic -inorganic hybrid SBA-15- HSO₃containing alkyl(methy1)and sulfonic acid groups was directly synthesized via hydro the rmaltechnique and characterized by XRD and nitrogen adsorption.The results show that catalyst SBA -15- HSO₃, a highly ordered two -dimensional hexagonal me so porous structure , has greater specific surface area , pore size and pore volume .Ethyl tertiary -butyl ether (ETBE)was synthesized by the reaction of ethyl alcohol and tertiary butyl alcohol with SBA -15 -HSO₃ as a catalyst , and the reaction dynamics model had been established.The reaction process carries on in the steel sealed rhythmic reaction cauldron without the influence of internal and external diffusion.The etherification reaction kinetic experiment data could be obtained with the change of the raw material density and the reaction temperature , then such a kinetic model r=kC^1.5_AC^-0.5_B , would be obtained, finally got the frequency factor 1 .3 ×10⁷ h^-1and activation energy 52.86kJ/mo l.At the same time , a theoretica1 mode1 r=k′C^1.5_A C^-0.5_B would be obtained according to the reaction mechanism , with frequency factor 1 .2 ×10⁷ h^-1and activation energy 52 .56kJ/mol .So the surface reaction could be considered as the rate -determining step.

Key words: SBA -15, , Ethyl tertiary -buty l ether (ETBE), , Etherification reaction, , Dynamics

摘要： 　用水热法直接合成了含磺酸基的介孔分子筛SBA -15 -HSO₃ 。采用X 射线衍射、N₂ 吸附-脱附分析方法对试样进行了表征。表征结果显示, 制得的SBA -15 -HSO₃ 具有高度有序的介孔二维六角结构, 并且有较大的比表面积、孔容和孔径。以乙醇和叔丁醇为原料, SBA -15-HSO₃ 为催化剂合成乙基叔丁基醚(ETBE), 建立了反应动力学模型。反应过程在钢密封间歇反应釜中进行, 且消除了内外扩散的影响。改变原料浓度和反应温度得到了醚化反应本征动力学实验数据。线性回归得动力学方程r=kC^1.5_AC^-0.5_B , 求得频率因子为1 .3 ×10⁷ h^-1 , 活化能为52 .86 kJ/ mo l。根据机理近似推导出的动力学方程r=k′C^1.5_A C^-0.5_B , 频率因子为1 .2×10⁷ h^-1 , 活化能为52 .56kJ/ mol。因此, 可近似认为表面反应是反应的速率控制步骤。

关键词: SBA-15, , 　乙基叔丁基醚, 　醚化反应, 　动力学

ZHAO Xin, SHEN Jian, JIAO Ho ng -yu. Kinetics of Synthesis of ETBE Over Mesoporous Molecular Sieve Catalys t SBA -15 -HSO₃[J]. Journal of Liaoning Petrochemical University, 2007, 27(4): 27-30.

赵　昕, 沈　健, 焦宏宇. 介孔分子筛SBA -15 -HSO₃ 合成ETBE 反应本征动力学研究[J]. 辽宁石油化工大学学报, 2007, 27(4): 27-30.

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Kinetics of Synthesis of ETBE Over Mesoporous Molecular Sieve Catalys t SBA -15 -HSO₃

介孔分子筛SBA -15 -HSO₃ 合成ETBE 反应本征动力学研究

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