程序升温连续流动反应器技术及其应用

在运用连续流动反应(CFR)技术(尾气技术)的基础上提出了1种可筛选催化剂并能进行非均相催化动力学研究的实验原理和方法--程序升温连续流动反应器(TPCFR)技术。在用此法筛选过的Cu-Ni催化剂上对甲醇分解反应和甲醇水蒸汽重整反应进行了系统研究,证明这种方法合理、可信。利用1条TPCFR曲线可求出各个动力学参数。

The Technique of Temperature Programmed Continuous Flow Reactor and Its Application

On the basis of the technique of Continuous Flow Reaction (CFR), a new experimental method, using in the sieving of catalyst and the kinetic studies of heterogeneous catalytic reactions, was proposed and it is the technique of Temperature Programmed Continuous Flow Reactor (TPCFR). The difference from CFR is that the temperature of reactor is controlled by a temperature programmed controller, and the products directly go into Gas Chromatography TCD. Using this method, the relationships between conversion and temperature, selectivity and temperature are obtained respectively by once experiment only. Thus, the amount of experimental work was greatly reduced. Combining with the conditions of reduction of samples, the catalysts of Cu-Ni for methanol steam reforming were sieved. In this paper, the reactions of methanol reforming and methanol steam reforming on Cu-Ni catalyst were studied by TPCFR, and the experimental results were compared with that of CFR. It was found that the results of TPCFR and CFR are identical, The TPCFR curves of methanol reforming were quantitatively analyzed.The results showed that the apparent activation energy was 58.6kJ/mol, reaction order was 1.4, and the raising rate of temperature did not obviously affects the best temperature of reaction, reaction order and the apparent activation energy. Methanol steam reforming on Cu0.5Ni0.5 catalyst, was studied by TPCFR. It was found that this reaction carried on with two steps, the first was methanol reforming, it's apparent activation energy E1 =65.3kJ/mol,reaction order was 1.4,the second was water gas shift reaction with 80% CO2 selectivity, it's apparent activation energy E2 =99.6kJ/mol, reactionorder was 1.2. It was proved that the method is reasonable and feasible. The method of TPCFR has some peculiarities i.e. convenient, fast, and the kinetic parameters were determined with a single program operation of TPCFR compared with isothermal method.