FeO^＋(^6Σ^＋)催化CO还原N2O的理论研究

Theoretical Studies on the Reduction of N_2O by CO on FeO^+(~6Σ^+)

在B3LYP/6-311+G(2d)//B3LYP/6-31G(d)计算水平下,考察了FeO+(6Σ+)分子如何催化CO还原N2O微观机理.计算结果表明,FeO+(6Σ+)是一种有效的催化剂,其可从N2O中夺取一个O原子,然后再传递给CO,完成整个氧转移过程.结果发现,反应中可能生成各种过氧[Fe(O2)+]或双端氧(OFeO+)物种,其中前者比较稳定,后者更活泼.

The reduction of N2O by CO was investigated at the level of B3LYP/6-311＋G（2d）//B3LYP/6-31G（d）,using FeO＋ as a model catalyst.The calculation results show that FeO＋ is an effective catalyst which can pick up the O atom from N2O and then deliver it to CO to accomplish the overall O-transfer.Two species,Fe（O2）＋ and OFeO＋,were located during the reactions.While Fe（O2）＋ is found to be more stable than OFeO＋;the latter is shown to be more active than the former.