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摘要: 采用绝热管式固定床积分反应器,在2.0MPa~4.0MPa、524K~644K、氢/裂解汽油摩尔比1.5~3.5和反应器入口环戊烯、3乙基1戊烯、苯乙烯和1己烯的分压分别为0.87kPa~5.60kPa、1.09kPa~7.01kPa、1.14kPa~7.35kPa和0.25kPa~0.97kPa下,对CoMo/Al2O3催化剂上裂解汽油中单烯烃催化加氢的宏观动力学特性进行了系统研究。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,建立了与实验数据吻合良好、裂解汽油中单烯烃催化加氢的幂函数型宏观动力学模型。其中,环戊烯、3乙基1戊烯、苯乙烯和1己烯的反应级数分别为1.725、0.685、0.7和0.655,对应的加氢反应宏观活化能依次为63455 J·mol-1, 61781 J·mol-1, 52105 J·mol-1和54181 J·mol-1。实验所用CoMo/Al2O3催化剂对环戊烯、3乙基1戊烯和苯乙烯加氢具有明显的催化作用,对1己烯加氢具有一定的催化作用,但对1庚烯加氢基本无催化活性。加氢反应压力控制在3.5MPa左右更为适宜。Abstract: The macrokinetic experiments of olefin hydrogenation in pyrolysis gasoline over an industrial CoMo/Al2O3 catalyst were carried out in an integral tubular fixedbed reactor under the following conditions: 2.0MPa~4.0MPa, 524K~644K, H2/pyrolysisgasoline molar ratio 1.5~3.5 and the partial pressure at reactor inlet for cyclopentene, 3ethyl1pentene, styrene and 1hexene 0.87kPa~5.60kPa, 1.09kPa~7.01kPa, 1.14kPa~7.35kPa and 0.25kPa~0.97kPa, respectively. By means of Powell optimal method and Merson integral method, the powerlaw type macrokinetic models of catalytic hydrogenation of olefin in pyrolysis gasoline were developed, and a good agreement with experimental data and those calculated by the kinetic models estimated was obtained. The reaction orders of cyclopentene, 1hexene, styrene and 3ethyl1pentene were 1.725, 0.685, 0.7 and 0.655, respectively. And the activation energies of hydrogenation reaction of theirs were 63455J·mol-1, 61781J·mol-1, 52105J·mol-1 and 54181J·mol-1, respectively. The CoMo/Al2O3 catalyst here shows a good catalytic activity for 1hexene hydrogenation, a better activity for the hydrogenation of cyclopentene, 3ethyl1pentene and styrene, but a poor activity for 1heptene hydrogenation. The favorable operating pressure is about 3.5MPa for this catalyst.
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Key words:
- catalytic hydrogenation /
- kinetics /
- pyrolysis gasoline /
- olefin
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