Theoretical study on elucidation of the mechanism of oxygen reduction reaction and development of carbon alloy electrodes.

采用密度泛函方法计算了碳合金电极上的氧还原反应，并建立了电晕烯等石墨烯的分子模型。氧分子不吸附在未取代的石墨烯上，而是通过不成对电子的相互作用吸附在氮取代的石墨烯上。吸附取决于未配对电子的大小，并且在分子的外围位置比在内部位置更强。这可以从sp2+p到sp3的杂化变化的灵活性来解释，后者可以与氧分子形成更强的键合。

Oxygen reduction reaction on carbon alloy electrodes was investigated at the elementary step level using the density functional method calculation and model molecules for graphene such as coronene. Oxygen molecule is not adsorbed on unsubstituted graphene but is adsorbed on nitrogen substituted graphene through the interactions of unpaired electrons. Adsorption depends on the magnitude of unpaired electrons, and is stronger at the peripheral sites than at the inner sites within molecules. This is explained in terms of flexibility of the hybridization change from sp2+p to sp3, the latter can make a stronger bonding with oxygen molecules.