Mechanism of fullerene hydrogenation by polyamines:<i>Ab initio</i>density functional calculations

Abstract

We use ab initio density functional calculations to study the microscopic mechanism underlying the recently demonstrated hydrogenation of the ${\text{C}}_{60}$ fullerene by diethylenetriamine reagent. Our results indicate that the optimal monoaddition reaction is exothermic, involving an $\ensuremath{\approx}0.5\text{ }\text{eV}$ high activation barrier associated with the simultaneous docking of the polyamine functional group and H transfer to ${\text{C}}_{60}$. Our calculated vibrational frequencies can be used to experimentally confirm the presence of hydroamination adducts as a necessary prerequisite for successful hydrogenation of ${\text{C}}_{60}$.