The adsorption and activation of oxygen molecule on nickel clusters doped graphene-based support by DFT

Abstract The catalytic activation of O2 on nickel nanoclusters doped upon diff ;erent functionalized graphene substrates (monovacancy as well as one, two and three pyridinic nitrogen decorated) was investigated through the density functional theory calculation. We can observed the adsorption characteristics and the catalytic activation of O2 on catalysts is related to the support effect of diff ;erent functionalized graphene supports. The charge of Ni aotms has a good correlation with the adsorption energy of O2 on Nin clusters with different graphene-based support. The electron mainly transferred from the Ni clusters to the O2, and the graphene-based substrates plays a minor role in the electron transfer process. In addition, the Transition State Scaling are suitable for O2 dissociation reaction, and Transition State Scaling verify the accuracy of the O2 dissociation reaction calculation. Furthermore, in accordance with the energy barrier and the thermodynamic analysis of O2 activation reaction, the Ni3 clusters catalyst anchored single vacancy graphene decorated with three nitrogen atoms may be the most promising catalyst for O2 activation reaction. At the same time, this research will cast insight into activation reaction mechanism of O2 on metal nanoclusters catalysts and lay the foundation for the investigation of metal nanoclusters catalysts for the activation reaction of O2.