Transition Metal-Doped C<sub>20</sub> Fullerene-Based Single-Atom Catalysts with High Catalytic Activity for Hydrogen Dissociation Reaction
Sehrish Sarfaraz, Muhammad Yar, Nadeem S. Sheikh, Imene Bayach, Khurshid Ayub
Abstract
High Resolution Image Download MS PowerPoint Slide Hydrogen dissociation is a key step in almost all hydrogenation reactions; therefore, an efficient and cost-effective catalyst with a favorable band structure for this step is highly desirable. In the current work, transition metal-based C 20 ( [email protected] 20 ) complexes are designed and evaluated as single-atom catalysts (SACs) for hydrogen dissociation reaction (HDR). Interaction energy ( E int ) analysis reveals that all the [email protected] 20 complexes are thermodynamically stable, whereas the highest stability is observed for the [email protected] 20 complex ( E int = −6.14 eV). Moreover, the best catalytic performance for H 2 dissociation reaction is computed for the [email protected] 20 catalyst ( E ads = 0.53 eV) followed by [email protected] 20 ( E ads = 0.65 eV) and [email protected] 20 ( E ads = 0.76 eV) among all considered catalysts. QTAIM analyses reveal covalent or shared shell interactions in H 2 * + [email protected] 20 systems, which promote the process of H 2 dissociation over [email protected] 20 complexes. NBO and EDD analyses declare that transfer of charge from the metal atom to the antibonding orbital of H 2 causes dissociation of the H–H bond. Overall outcomes of this study reveal that the [email protected] 20 catalyst can act as a highly efficient, low-cost, abundant, and precious metal-free SAC to effectively catalyze HDR.