Mechanism of fullerene hydrogenation by polyamines:: Ab initio density functional calculations

We use ab initio density functional calculations to study the microscopic mechanism underlying the recently demonstrated hydrogenation of the C(60) fullerene by diethylenetriamine reagent. Our results indicate that the optimal monoaddition reaction is exothermic, involving an approximate to 0.5 eV high activation barrier associated with the simultaneous docking of the polyamine functional group and H transfer to C60. Our calculated vibrational frequencies can be used to experimentally confirm the presence of hydroamination adducts as a necessary prerequisite for successful hydrogenation of C(60).