氧掺杂石墨烯体系负载Pt团簇催化性能的理论研究

Theoretical study on catalytic property of Pt clusters supported on oxygen-doped graphene

基于密度泛函理论的第一性原理方法研究了氧原子掺杂石墨烯衬底负载Pt4团簇体系的稳定结构和催化性能.观察3个不同结构的Pt4团簇在石墨烯衬底相互转换的反应过程,结果表明:结构1和结构2转化为结构3需要克服较小的能量势垒,结构3的Pt4团簇在石墨烯衬底形成最稳定构型.在研究不同反应气体吸附特性的基础上,对比两种反应机理对CO氧化反应过程的影响.本研究为设计石墨烯纳米功能材料提供重要的理论参考.

The stable configuration and catalytic property of tetrahedral Pt4 clusters anchored on oxygen- doped graphene（ O- graphene） substrate were studied using the first- principles calculations based density functional theory. The structural interconversions between adsorbed Pt4 clusters on the O- graphene were investigated,it is found that the configuration 1 and 2 can easily interconvert into the configuration 3 with small energy barriers,and the configuration 3 has the most stability on the O- graphene. Based on the adsorption property of reactive gases,two mechanisms for the sequential CO oxidation reaction on the Pt4/ O- graphene were investigated for comparison.The study provides a valuable guidance on fabricating graphene- based functional nanomaterials.