Enhancement of single-atom catalytic activity by the synergistic effect of interlayer charge transfer and magnetic coupling in an electride-based heterostructure.

2D material-based single-atom catalysts have rapidly emerged and flourished in recent years due to their exceptional atomic utilization efficiency, adjustable catalytic activity, and remarkably high selectivity. The interface matching mechanism of 2D materials, influenced by van der Waals (vdW) interactions, presents a novel opportunity for constructing a heterostructure, further augmenting catalytic efficiency. In this work, the mechanism of performance regulation of magnetic transition-metal decorated MoS single-atom catalysis by importing a GdC electride substrate is investigated using first-principles calculations. The localization of d orbitals in transition-metals is weakened by adding a GdC substrate, thereby modulating the catalytic performance. Our findings demonstrate that the formation of an electron layer at the interface of the heterostructure by electride GdC induces a modification in the chemical environment of the MoS surface. The electron layer enhances the electron transfer during catalysis. Additionally, for the catalyst containing magnetic atoms, GdC can also achieve catalytic performance adjustment due to the magnetic coupling, similar to the effect of external magnetic fields. This study offers a novel concept and a pathway for enhancing the performance of single-atom catalysts through the construction of a heterostructure, capitalizing on the distinctive electron layer of an electride and its inherent high magnetic moments.