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在动态过程中,由于表面上吸附物种的浓度随时间而变化,因此有可能提供稳态流动法不可能获得的信息。本文提出了能够获得反应物峰矩量值的催化反应色谱理论,并以此理论初步考察了噻吩氢解和环己烷脱氢反应,测定了不同温度下反应的吸附和表面反应速率,获得了分离的吸附和表面反应速率常数值,得到了两反应的吸附热和表面反应活化能值。环己烷的吸附速率常数>10~6可以认为瞬时达到平衡;噻吩加氢的吸附速率在约270℃时有一转折,结果表明,不需假设单一速率控制步骤即可分别地测定吸附和表面反应速率,从而对催化反应的动力学特性和反应机理有可能作较深人的了解。
In the dynamic process, it is possible to provide information that steady-state flow methods can not obtain because the concentration of adsorbed species on the surface varies over time. In this paper, we proposed a catalytic reaction chromatogram theory that can obtain the peak value of the reactant. Based on this theory, the thiophene hydrogenolysis and cyclohexane dehydrogenation were investigated. The adsorption and surface reaction rates were measured at different temperatures. The adsorption and surface reaction rate constants were separated and the heat of adsorption and the surface activation energy of the two reactions were obtained. Cyclohexane adsorption rate constants> 10 ~ 6 can be considered instantaneous equilibrium; thiophene hydrogenation adsorption rate at about 270 ℃ when there is a turning point, the results show that without the assumption that a single rate control step can be separately measured adsorption and surface reaction Rate, and thus the kinetic characteristics of the catalytic reaction and the reaction mechanism may be more in-depth understanding.