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裂解汽油中噻吩硫在Co-Mo/Al2O3上的催化加氢宏观动力学
引用本文:李建伟,李英霞,陈标华,李成岳,张小工.裂解汽油中噻吩硫在Co-Mo/Al2O3上的催化加氢宏观动力学[J].燃料化学学报,2005,33(5):576-581.
作者姓名:李建伟  李英霞  陈标华  李成岳  张小工
作者单位:1. The Key Laboratory of Science and Technology of Controllable Chemical Reactions, Ministry of Education, Beijing University of Chemical Technology, Beijing 100029, China;2. Catalyst Division of Lanzhou Petrochemical Institute, Petrochemical Company Limited, Lanzhou 730060, China
基金项目:中国石油天然气集团公司资助(990813-19).
摘    要:采用绝热管式固定床积分反应器,在2.5MPa~3.9MPa、513K~655K、氢/裂解汽油摩尔比1.8~3.5和裂解汽油中噻吩、单甲基噻吩和双甲基噻吩质量分数为838×10-6、137×10-6~723×10-6和192×10-6~723×10-6下,对Co-Mo/Al2O3催化剂上裂解汽油催化加氢脱硫的宏观动力学进行了研究。以Powell优化法和Merson迭代法对动力学实验数据进行非线性参数估值,建立了良好吻合实验数据的、裂解汽油催化加氢脱硫的幂函数型宏观动力学模型。噻吩、单甲基噻吩和双甲基噻吩的反应级数分别为0.721、0.735和0.87,对应的加氢反应宏观活化能依次为70.0kJ·mol-1、67.9kJ·mol-1和59.9kJ·mol-1。各噻吩基硫的转化率均随反应压力的提高而增加,3.5MPa以上时,增加的趋势减缓;反应温度的提高有利于噻吩基硫转化率的增加;593K以上时,各硫化物的转化率随温度的增加呈现线性增加的趋势。

关 键 词:加氢脱硫  动力学  裂解汽油  噻吩基硫  
文章编号:0253-2409(2005)05-0576-06
收稿时间:12 8 2004 12:00AM
修稿时间:09 25 2005 12:00AM

Macrokinetics for catalytic hydrogenation of thiophenic sulfides in pyrolysis gasoline over Co-Mo/Al2O3 catalyst
LI Jian-wei,LI Ying-xia,CHEN Biao-hua,LI Cheng-yue,ZHANG Xiao-gong.Macrokinetics for catalytic hydrogenation of thiophenic sulfides in pyrolysis gasoline over Co-Mo/Al2O3 catalyst[J].Journal of Fuel Chemistry and Technology,2005,33(5):576-581.
Authors:LI Jian-wei  LI Ying-xia  CHEN Biao-hua  LI Cheng-yue  ZHANG Xiao-gong
Institution:LI Jian-wei1,LI Ying-xia1,CHEN Biao-hua1,LI Cheng-yue1,ZHANG Xiao-gong2
Abstract:The macro-kinetic investiqations for catalytic hydrodelsulfurization of pyrolysis gasoline over an industrial Co-Mo/Al2O3 catalyst were carried out in an adiabatic tubular fixed bed reactor under the conditions: 2.5MPa~3.9MPa, 513K~655K, H2/pyrolysis gasoline molar ratio 1.8~3.5, and the mass concentration of thiophene, methylthiophene and dimethylthiophene in the feed pyrolysis gasoline, 838×10-6, 137×10-6~723×10-6 and 192×10-6~723×10-6, respectively. By means of Powell optimal method and Merson integral method, the power-law type macro kinetic models for the catalytic hydrodelsulfurization of pyrolysis gasoline were developed. The reaction orders of thiophene, methylthiophene and dimethylthiophene are 0.721, 0.735 and 0.870, respectively, and the activation energies are 70.0kJ·mol-1, 67.9kJ·mol-1 and 59.9kJ·mol-1, respectively. The conversion of thiophenic sulfides increases with the reaction pressure, but this increase is obviously slowed down at the reaction pressure above 3.5MPa. The increase of reaction temperature is beneficial to the conversion enhancement of thiophenic sulfides, especially above 563K. When the reaction temperature increases above 593K, the correlation between the conversion of thiophenic sulfides and temperature is almost linear. Therefore, for the Co-Mo/Al2O3 catalyst used, the favorable operating pressure is about 3.5MPa, and the reaction temperature should be higher than 593K.
Keywords:hydrodesulfurization  kinetics  pyrolysis gasoline  thiophenic sulfide compounds
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