Modification of a Carbon Nanobelt with Actinides Th-Am: A Density Functional Theory Study

Recently, the carbon nanobelt (CNB) comprising a closed loop of fully fused edge-sharing benzene rings has been reported in an experiment. To explore its potential molecular properties and applications, we performed scalar relativistic density functional theory investigations on the interaction mechanisms of the CNB with a series of actinide atoms (An = Th-Am). Computations indicate that doping of actinide (An) atoms onto the surface of the CNB can result in the formation of stable actinide endohedral An@CNB compounds, along with the formation of C-An-C rings as well as a drastic structural transformation of the CNB. Compared to transuranium actinides, Th, Pa, and U exhibit a stronger adsorption affinity to the CNB in terms of the calculated binding energies. The adaptive natural density partitioning analysis shows that there form five 3c-2e bonds and two 5c-2e bonds in An@CNB for An = Th, Pa, and U, with fewer multicenter bonds for An = Np, Pu, and Am. These theoretical results provide a new strategy for chemical modification and functionalization of the CNB by actinide doping in the future.