First principle study of feasibility of dinitrogen reduction to ammonia on two-dimensional transition metal phthalocyanine monolayer

The current remarkable catalysts for natural and artificial ammonia (NH3) synthesis are transition-metal (TM) atoms as binding site and catalytic center. Herein several TM atoms were embedded regularly and separately on phthalocyanine monolayer as N-2 capture and reduction catalysts and theirs catalytic activity were investigated in this work by performing density functional theory simulations. The results showed that single molybdenum atom embedded phthalocyanine monolayer exhibited outstanding performances on N-2 capture and reduction to NH3 at ambient conditions. N-2 reduction reaction prefers to proceed through distal reaction pathway with a rate determining barrier 0.70 V, suggesting its good catalytic performance for N-2 reduction. Our work also demonstrated the Pc monolayers can act as an excellent substrate for the design of single-atom catalysts. Our study provides a novel pathway for achieving conversion of N-2 into NH3 at ambient conditions.