Sc cluster supported on two-dimensional biphenylene for CO2 reduction

Transition metals are frequently employed in electrocatalytic reactions owing to their exceptional catalytic properties and wide applicability. The development of various carbon allotropes has opened new avenues for catalyst innovation. As a novel two-dimensional carbon allotrope, biphenylene offers a promising direction for catalyst design and synthesis. In this study, we examined the structural and catalytic properties of Sc clusters on biphenylene using density functional theory and thermodynamic calculations. Our findings reveal that among 3d transition metals, Sc exhibits the strongest atomic binding energy (close to the binding energy of Sc bulk) and has a tendency to form cluster on biphenylene. The configuration of the most stable Sc3 cluster is identified. In air, the Sc3 cluster has a tendency towards oxidation and is favorable to adsorbing five O2 molecules. In an aqueous electrocatalytic environment, most of catalytic sites on Sc3-5O2 are occupied by H+, but the resultant Sc3-5O212H cluster maintains robust CO2 reduction activity, with an onset potential of 0.57 V to produce CH3OH. These insights are expected to guide the design of catalysts based on biphenylene.