摘要
采用过渡应答方法对甲烷化反应中引起催化剂失活的CO歧化反应进行了研究。提出了J 105 Ni催化剂上歧化反应可能遵循的机理,并用数学优化方法求出了所提动力学模型的参数,通过求取各基元步骤的活化能,进一步验证了所提机理的正确性。
The adsorption behavior of carbon monoxide and its dispropollionation mechanism on J105 Ni catalyst was studied by the transient response method. Under the reaction temperature, there are reversible CO adsorption and irreversible CO adsorption on Ni catalyst, and the latter predominates over the former. When the reaction temperature is above 150℃, CO2 is observed. CO2 increaces with increasing the temperature. A mechanism of CO disproportionation is proposed, in which the dissociation of CO and desorption of CO2 are slower steps. CO dissociates into surface oxygen and surface carbon which have high reactivity for the formation of carbon dioxide and methane. By using the non-linear optimization technique, the optimum values of all the rale constant are determined, the calculated results arc consistent well with the quantitalive predication and also with Arrhenius law.
基金
国家自然科学基金
