Anchoring Mo on C_(9) N_(4) monolayers as an efficient single atom catalyst for nitrogen fixation

摘要

Electrochemical nitrogen fixation via a convenient and sustainable manner,exhibits an intriguing prospect for ammonia generation under ambient conditions.Currently,the design and development of high-efficiency and low-cost electrocatalysts remains the major challenge confronting nitrogen reduction reaction(NRR).Herein,anchoring the single Mo atom on the C_(9) N_(4) substrate(Mo@C_(9)N_(4)) to form an efficient single-atom catalyst(SAC) is proposed for the conversion of N2 to NH3.By employing density functional theory(DFT) calculations,we demonstrated that gas phase N2 can be sufficiently activated and efficiently reduced to NH3 on the surface of Mo@C_(9) N_(4).Meanwhile,we found that the NRR dominantly occurred on the Mo center via a preferred distal pathway with favorable limiting potential of 0.40 V.Importantly,the as-established Mo@C_(9) N_(4) catalyst exhibits an outstanding structural stability and good selectivity toward NRR.These findings provide a promising platform for designing Mo-based SACs for electrochemical N2 fixation.