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超临界流体对固定床甲醇合成反应促进作用的研究
1.中国石化催化剂有限公司,北京 100029;
2.华东理工大学化学工程联合国家重点实验室,上海 200237
Effect of Methanol Hydrogen Bond Association in Supercritical Medium on Methanol Synthesis
1. Catalyst Company Limited, SINOPEC, Beijing 100029, China;
2. State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China
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摘要 为了阐明超临界流体对甲醇合成反应的促进作用,在固定床反应器中实验考察了超临界正己烷中合成气制甲醇反应。结果表明:忽略催化剂内扩散阻力时,氮气中甲醇合成反应的反应器出口甲醇浓度低于平衡值,而超临界正己烷介质中甲醇合成反应的反应器出口甲醇浓度远高于平衡值。此外,建立了固定床反应器内超临界正己烷中甲醇合成反应的浓度分布模型,模拟考察了甲醇四缔合体的存在对反应结果的影响,发现由于甲醇分子间的氢键缔合大大降低了催化剂表面单体甲醇浓度,促进平衡向着甲醇合成反应方向进行,使得固定床出口甲醇浓度大于平衡值。
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吴思操1
2
顾松园1
程振民2
汪华林2
关键词 超临界流体甲醇合成氢键缔合    
Abstract:To elucidate the promoting effect of supercritical fluid on methanol synthesis, the synthesis of methanol using supercritical n-hexane was investigated in a fixed-bed reactor. The results show that the methanol concentration (in the nitrogen) in the outlet of the methanol synthesis reactor is lower than that of the equilibrium value when the diffusion resistance of the catalyst was ignored, while the methanol concentration exported from the reactor in supercritical n-hexane medium was much higher than the equilibrium value. In addition, the concentration distribution model of the methanol synthesis in supercritical n-hexane in the fixed-bed reactor was established. The influence of the existence of methanol tetrameric species on the reaction results was simulated. It was found that the methanol monomer concentration on the surface of the catalyst was greatly reduced due to the hydrogen bond association between the methanol molecules, which promoted the equilibrium toward the direction of the methanol synthesis reaction, and the methanol concentration in the fixed-bed outlet was higher than the equilibrium value.
Key wordssupercritical fluid    methanol synthesis    hydrogen bond    aggregate   
收稿日期: 2016-03-28     
作者简介: 吴思操(1986—),男,工程师。E-mail:wusc.sshy@sinopec.com。
引用本文:   
吴思操1,2,顾松园1等. 超临界流体对固定床甲醇合成反应促进作用的研究[J]. 化学反应工程与工艺, 2016, 32(5): 432-437.
Wu Sicao 1,2,Gu Songyuan 1 et al. Effect of Methanol Hydrogen Bond Association in Supercritical Medium on Methanol Synthesis[J]. 化学反应工程与工艺, 2016, 32(5): 432-437.
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