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甲醇直接气相羰基化反应动力学
引用本文:彭峰,沈秋英.甲醇直接气相羰基化反应动力学[J].燃料化学学报,2001,29(6):570-573.
作者姓名:彭峰  沈秋英
作者单位:华南理工大学,化学工程系,
基金项目:国家自然科学基金 ( 2 990 30 0 3),广东省自然科学基金 ( 970 438)~~
摘    要:甲醇直接气相羰基化研究 ,是在无任何促进剂下 ,CO与甲醇直接进行羰基化反应 ,这与目前公认的甲醇必须有碘化物作用下构成催化循环的间接羰化不同 ,在催化理论上有可能提出新的羰基化机理。彭峰等在甲醇直接气相羰基化方面 ,对具有高活性与选择性的非铑非卤素Mo C催化剂体系进行了系列研究 ,并取得了较好的实验结果1~ 5] 。有碘甲烷参与的甲醇羰基化液相或者气相反应 ,大多数文献认为控制步骤是碘化物中C -I键的解离及CO的插入 ,羰基化反应是由一系列平行和连串反应组成的6~ 8] 。催化剂类型不同得到的动力学参数也不相同 ,难…

关 键 词:甲醇  气相羰基化  催化剂  动力学    乙酸甲酯
文章编号:0253-2409(2001)06-0570-04
修稿时间:2001年6月4日

KINETICS OF DIRECT VAPOR-PHASE CARBONYLATION OF METHANOL
PENG Feng,SHEN Qiu ying.KINETICS OF DIRECT VAPOR-PHASE CARBONYLATION OF METHANOL[J].Journal of Fuel Chemistry and Technology,2001,29(6):570-573.
Authors:PENG Feng  SHEN Qiu ying
Abstract:A novel heterogeneous sulfided Mo/C catalyst was used for the direct vapor phase carbonylation of methanol Experiments were designed with the elimination of mass transfer resistances to obtain data The data of primary reactions in the carbonylation were collected via a differential tubular reactor Feed composition was varied to examine the effect of partial pressures of reactants on the reaction rate Power law rate models were employed to express the conversion of methanol and the formations of methyl acetate and methane Adequate results were obtained with the models to represent the experimental data The reaction orders of methyl acetate formation with respect to methanol and CO were found to be 1 2 and 0 35 respectively on the novel Mo/C catalyst, and the reaction activation energy was 106?kJ/mol At the same time, the reaction mechanism of direct vapor phase carbonylation of methanol was presented The initial step of this reaction was suggested to be the cleavage of methanol to form CH 3 M, followed by adsorbed CO insertion into the metal methyl bond to form CH 3C(O) M, which further interacts with methanol to form methyl acetate
Keywords:methanol  vapor phase carbonylation  kinetics  catalyst  carbonylation  Mo/C
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