CAJ | 학술논문

采用乙炔顺序加氢的反应机理,利用已报道的密度泛函理论(DFT)计算结果进行了乙炔加氢反应的微观反应动力学模拟,所得的乙炔加氢反应动力学具有共同的特征.利用实验获得的Pd/α-Al2O3催化乙炔加氢反应动力学数据,对上述DFT数据进行校验,发现经过不超过0.1 eV的调整,微观反应动力学模拟结果与实验结果符合很好,说明DFT数据是良好的微观反应动力学参数来源.利用优化后的动力学参数模拟了工业生产范围内的动力学,获得了速率控制步骤和表面物种等信息,可为双曲动力学模型的建立提供参考.
채용을결순서가경적반응궤리,이용이보도적밀도범함이론(DFT)계산결과진행료을결가경반응적미관반응동역학모의,소득적을결가경반응동역학구유공동적특정.이용실험획득적Pd/α-Al2O3최화을결가경반응동역학수거,대상술DFT수거진행교험,발현경과불초과0.1 eV적조정,미관반응동역학모의결과여실험결과부합흔호,설명DFT수거시량호적미관반응동역학삼수래원.이용우화후적동역학삼수모의료공업생산범위내적동역학,획득료속솔공제보취화표면물충등신식,가위쌍곡동역학모형적건립제공삼고.
The microkinetic modeling of hydrogenation of acetylene following a sequential hydrogenation mechanism was carried out based on density functional theory(DFT) results from other researchers. All the modeling results showed that the kinetic behavior of acetylene hydrogenation had some common characteristics. The kinetic parameters from the DFT results were adjusted according to the kinetic data obtained from the experiments over the Pd/α-Al2O3 catalyst. It was found that the microkinetic modeling results fitted well to the experimental results after adjustment within 0.1 eV, which indicated that DFT results could be a good resource for practical reaction kinetic modeling. Some key information for macrokinetic model building, rate determine steps and surface coverage were obtained from the microkinetic modeling using the optimized parameters under the industrial operation conditions.