Enhancement of single-atom catalytic activity by interlayer charge transfer in electride-based heterostructures

Abstract

The growing interest in single-atom catalysts (SACs) can be attributed to the continuous updates and iterations in their synthesis process. SACs exhibit remarkable advantages, including exceptional catalytic activity, excellent selectivity, and tunable reactivity to meet the specific requirements of diverse reactions. Consequently, SACs have emerged as pivotal players in numerous scientific domains. The hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), as pivotal fundamental reactions, hold significant research value. In this work, a novel kind of SAC based on an electride/monolayer MoS₂ heterostructure is predicted by using first-principles calculations. The anionic electron layer formed between the electride and MoS₂ can effectively modulate the charge distribution on the surface of MoS₂, thereby enabling indirect manipulation of the performance of the SACs. There exists a robust linear correlation between the adsorption energy and charge variation, which serves as a pivotal descriptor of catalyst performance. The energy difference between the O* process structure and slab structure exhibits a strong linear correlation with the overpotential in the OER, making it a valuable criterion for efficient screening of electride-based heterogeneous catalysts which streamlines the screening process for OER catalysts. The present study offers a novel strategy for enhancing the catalytic performance of SACs.