CAJ | 학술논문

为了有效控制动力学振荡行为以提高反应的转化率，利用Monte Carlo方法研究了甲烷催化部分氧化过程中的强制振荡行为，探讨了原料气周期性变化对振荡动力学和转化率的影响。研究表明原料气周期性变化不仅可以有效调控振荡的动力学行为，产生如短周期振荡和双峰振荡等特殊动力学过程，而且还可以提高反应的转化率。当强制过程的周期从T/3增大到2T(T为自发振荡过程的平均周期)，振荡过程从短周期振荡变化为双峰振荡。对反应过程中CO的转化率进行了计算，结果表明原料气周期性变化可以有效提高反应的转化率。振荡动力学的改变和转化率的提高主要是因为强制振荡过程使得催化剂表面发生了从氧化态向还原态的转变。
위료유효공제동역학진탕행위이제고반응적전화솔，이용Monte Carlo방법연구료갑완최화부분양화과정중적강제진탕행위，탐토료원료기주기성변화대진탕동역학화전화솔적영향。연구표명원료기주기성변화불부가이유효조공진탕적동역학행위，산생여단주기진탕화쌍봉진탕등특수동역학과정，이차환가이제고반응적전화솔。당강제과정적주기종T/3증대도2T(T위자발진탕과정적평균주기)，진탕과정종단주기진탕변화위쌍봉진탕。대반응과정중CO적전화솔진행료계산，결과표명원료기주기성변화가이유효제고반응적전화솔。진탕동역학적개변화전화솔적제고주요시인위강제진탕과정사득최화제표면발생료종양화태향환원태적전변。
To control the kinetic oscil ations for the purpose of obtaining a high conversion rate, external forcing of methane oxidation on metal catalysts was studied with kinetic Monte Carlo simulations. The influence of composition cycling of the feed on the dynamics and conversion rate was investigated. The results showed that the composition cycling of feed cannot give rise to different kinetic behavior, such as short periods or double-peaks, but does bring about a higher conversion rate. It was shown that with forcing periods from T/3 to 2T (T is the average period of autonomous oscil ations), the oscil ations changed from short periods and smal amplitudes to typical double-peak oscil ations. The conversion rate can also be calculated, and the results showed that the mean conversion was slightly higher with forced oscil ations. The changing of the kinetics can be attributed to phase transition of the metal catalysts from the oxidized surface to a partial y reduced state.