CAJ | 학술논문

采用密度泛函理论( DFT)计算研究铁原子与NO反应的相关微观反应机理。全参数优化了四重态和六重态反应势能面上各驻点的几何结构，用频率分析方法和内禀反应坐标( IRC)方法对过渡态进行了验证，得到了该反应的反应势能面曲线，并讨论了势能面的交叉情况。结果表明，该反应为典型的两态反应，反应通道一中出现了一个势能交叉点，反应通道二中出现了两个势能交叉点，反应通道三中出现了三个势能交叉点。势能面上的交叉点能够有效降低反应的活化能，增加反应放热，这在动力学和热力学上都是有利的。
채용밀도범함이론( DFT)계산연구철원자여NO반응적상관미관반응궤리。전삼수우화료사중태화륙중태반응세능면상각주점적궤하결구，용빈솔분석방법화내품반응좌표( IRC)방법대과도태진행료험증，득도료해반응적반응세능면곡선，병토론료세능면적교차정황。결과표명，해반응위전형적량태반응，반응통도일중출현료일개세능교차점，반응통도이중출현료량개세능교차점，반응통도삼중출현료삼개세능교차점。세능면상적교차점능구유효강저반응적활화능，증가반응방열，저재동역학화열역학상도시유리적。
Density functional theory ( DFT) calculations have been carried out to study the micro-mechanism for reaction of iron atom with NO. The geometry optimizations of reactants, transition states, intermediates and products of the reactions of sextet and quartet states were completely optimized, and all the transition states were verified by the vibrational analysis and the intrinsic reaction coordinate calculations. Then the potential energy surface ( PES) were obtained and crossing points were investigated. Results showed that the reaction of iron atom with NO was a typical two-state reaction(TSR). One crossing point appeared in the reaction channels 1, Two crossing points appeared in the reaction channels 2 , while three crossing points appeared in the reaction channels 3 between the quartet and the sextet potential energy surfaces, which would effectively reduce the activation ener-gy and increase the release of reaction heat, play a significant and beneficial role in the kinetic and thermody-namic aspects of this catalytic reaction.