Enhanced layer‐layer interaction via a tunable C60 layer in Mo2CTx‐based catalyst for ammonia synthesis

Abstract Molybdenum (Mo) serves as the key site in the nitrogenase enzyme, catalyzing the conversion of N 2 into NH 3 under ambient conditions. However, the strong affinity of Mo sites for N 2 hinders H 2 adsorption due to the competitive nature of N 2 and H 2 on a single site, resulting in an unsatisfactory ammonia synthesis performance. Here, we propose an approach of intervening C 60 layer as a second site for H 2 adsorption on two‐dimensional Mo 2 CT x . The C 60 layer thickness is readily tunable by varying its loading content. An optimal C 60 layer significantly enhances the electronic interaction between the C 60 layer and the Mo 2 CT x layer, leading to a remarkable decrease in the work function and an increase in the electron density of Mo atoms. Therefore, the separate adsorption of N 2 and H 2 on distinct sites is substantially facilitated. The present work offers insights into the correlation between structure and performance in NH 3 synthesis catalysts.