In Situ Synthesis of MoS2 on C3N4 To Form MoS2/C3N4 with Interfacial Mo-N Coordination for Electrocatalytic Reduction of N-2 to NH3

Electrocatalytic nitrogen reduction reaction (NRR), as an alternative to synthetic ammonia under mild condition, provides a promising method for storage and sustainable utilization of ammonia. However, the catalytic performance of the NRR electrocatalyst still requires a systematical investigation and improvement. Herein, this paper reports that MoS2/C3N4 is prepared by in situ controllable synthesis through a one-step pyrolysis process of thiourea and ammonium molybdate. A thorough characterization reveals that the strong interactions between MoS2 and C3N4 of MoS2/C3N4 lead to the formation of an interface with Mo-N coordination, which promotes electron transfer across the MoS2/C3N4 interface. Meanwhile, it is clarified that the formation of interfacial Mo-N coordination is beneficial to improve the catalytic activity and acts as the main active sites for catalyzing NRR. As a result, the as-prepared electrocatalyst exhibits an excellent NH3 yield rate of 19.86 mu g h(-1) mg(cat.)(-1) and an enhanced faradaic efficiency of 6.87% at -0.5 V (vs reversible hydrogen electrode) in 0.1 M Na2SO4, placing it as one of the most promising NRR electrocatalysts.