摘要
通过计算和实验研究相结合的方法研究丙烷甲醇共进料制烯烃反应热力学及动力学过程.热力学过程采用Gibbs最小自由能法模拟丙烷甲醇制烯烃反应体系的平衡组成,同时结合响应面分析法建立了温度、压力、丙烷甲醇进料摩尔比对产物中丙烯的摩尔分数的函数关系,通过回归方程分析最佳工艺范围.热力学分析了反应条件对平衡产物的影响,随着反应温度升高,平衡产物丙烯的质量分数先增高后降低;平衡产物中丙烯的质量分数随着丙烷甲醇进料中丙烷摩尔比增高而增高,但是实际的反应状态和催化剂也是相关的,因此研究了存在催化剂情况下,丙烷脱氢和丙烷甲醇共进料反应的活化能.反应活化能动力学实验表明,通过添加少量甲醇可以降低耦合过程中丙烷脱氢表观活化能.
The paper mainly studies the thermodynamic and kinetic process of propane and methanol to olefins reaction by calculation and experiment.The Gibbs minimum free energy method was used to simulate the equilibrium composition of the propane methanol to olefin reaction system.At the same time,combined with the response surface analysis method,the functional relationship between temperature,pressure,propane methanol feed molar ratio,and the molar fraction of propylene in the product is established.The optimal process range is analyzed by the regression equation.The effect of reaction conditions on the equilibrium product was analyzed by thermodynamics.With the increase of reaction temperature,the mass fraction of equilibrium product propylene increased first and then decreased.The mass fraction of propylene in the equilibrium product increases with the increase of propane methanol feed molar ratio,but the actual reaction state is also related to the catalyst.Therefore,the activation energy of propane dehydrogenation and propane methanol co-feed reaction in the presence of a catalyst is studied.The kinetic experiments show that the apparent activation energy of propane dehydrogenation in the coupling process could be reduced by adding a small amount of methanol.
作者
黄羚翔
李海岩
马跃
杜巍
申宝剑
HUANG Ling-xiang;LI Hai-yan;MA Yue;DU Wei;SHEN Bao-jian(State Key Laboratory of Heavy Oil Processing,Beijing 102249,China;College of Chemical Engineering and Environment,China University of Petroleum,Beijing 102249,China;Daqing Chemical Research Center,China Petroleum and Petrochemical Research Institute,Daqing 163714,China)
出处
《分子催化》
CAS
CSCD
北大核心
2023年第1期12-22,I0001,共12页
Journal of Molecular Catalysis(China)
基金
国家自然科学基金创新研究群体项目(22021004)
国家自然科学基金面上项目(21776304)。
关键词
丙烷脱氢热耦合
响应面分析法
Gibbs最小自由能
Hess定律
表观活化能
endothermic exothermic coupling in propane dehydrogenation
response surface analysis
Gibbs minimum free energy
hess law
apparent activation energy
