Metallofullerenes as Robust Single-Atom Catalysts for Adsorption and Dissociation of Hydrogen Molecules: A Density...

Hydrogen is currently considered as the best alternative for traditional fuels due to its sustainable and ecofriendly nature. Additionally, hydrogen dissociation is a critical step in almost all hydrogenation reactions, which is crucial in industrial chemical production. A cost-effective and efficient catalyst with favorable activity for this step is highly desirable. Herein, transition-metal-doped fullerene (TM@C₆₀) complexes are designed and investigated as single-atom catalysts for the hydrogen splitting process. Interaction energy analysis (E_int) is also carried out to demonstrate the stability of designed TM@C₆₀ metallofullerenes, which reveals that all the designed complexes have higher thermodynamic stability. Furthermore, among all the studied metallofullerenes, the best catalytic efficiency for hydrogen dissociation is seen for the Sc@C₆₀ catalyst E_a = 0.13 eV followed by the V@C₆₀ catalyst E_a = 0.19 eV. The hydrogen activation and dissociation processes over TM@C₆₀ metallofullerenes is further elaborated by analyzing charge transfer via the natural bond orbital and electron density difference analyses. Additionally, quantum theory of atoms in molecule analysis is carried out to investigate the nature of interatomic interactions between hydrogen molecules and TMs@C₆₀ metallofullerenes. Overall, results of the current study declare that the Sc@C₆₀ catalyst can act as a low cost, highly efficient, and noble metal-free single-atom catalyst to efficiently catalyze hydrogen dissociation reaction.