Co原子在NC载体表面的吸附及苯甲醇氧化的反应机制

Adsorption of Co atom on NC support and reaction mechanism of benzyl alcohol oxidation

针对氮掺杂碳材料(NC)负载Co单原子催化剂,采用了第一性原理计算方法,对NC负载Co单原子的结构以及Co-N4构型催化剂在苯甲醇(BnOH)氧化反应过程中的作用进行了相关计算,结果表明,双C空位缺陷的NC相比于单C空位缺陷NC更有利于Co单原子的锚定。计算表明,Co单原子将O_(2)分子活化后,活性氧与BnOH反应得到苯甲醛,BnOH与苯甲醛之间存在的能量差有利于反应向正向进行,相关计算为反应研究提供了理论依据。

For the study of the performance of the Co single-atom catalyst supported by nitrogen-doped carbon material(NC),the first principle calculation method is used to calculate the structure of Co single-atom supported by NC and the role of Co-N4 catalyst in the oxidation process of benzyl alcohol(BnOH).The results showed that:NC with the di-vacancy defect is more conducive to the anchoring of Co atoms than the NC with the single-vacancy defect.Calculations show that after the activation of O_(2) molecules by Co atoms,benzaldehyde is obtained by the reaction of the activated oxygen with BnOH,and the energy difference between BnOH and benzaldehyde is favourable for the reaction to proceed in a positive direction.The calculations provide a theoretical basis for the study of the reaction.