In Situ Synthesis of MoS₂ on C₃N₄ To Form MoS₂/C₃N₄ with\nInterfacial Mo–N Coordination for Electrocatalytic Reduction\nof N₂ to NH₃

Abstract

Electrocatalytic\nnitrogen reduction reaction (NRR), as an alternative\nto synthetic ammonia under mild condition, provides a promising method\nfor storage and sustainable utilization of ammonia. However, the catalytic\nperformance of the NRR electrocatalyst still requires a systematical\ninvestigation and improvement. Herein, this paper reports that MoS₂/C₃N₄ is prepared by in situ controllable\nsynthesis through a one-step pyrolysis process of thiourea and ammonium\nmolybdate. A thorough characterization reveals that the strong interactions\nbetween MoS₂ and C₃N₄ of MoS₂/C₃N₄ lead to the formation of an interface\nwith Mo–N coordination, which promotes electron transfer across\nthe MoS₂/C₃N₄ interface. Meanwhile,\nit is clarified that the formation of interfacial Mo–N coordination\nis beneficial to improve the catalytic activity and acts as the main\nactive sites for catalyzing NRR. As a result, the as-prepared electrocatalyst\nexhibits an excellent NH₃ yield rate of 19.86 μg\nh^–1 mg_cat.^–1 and an\nenhanced faradaic efficiency of 6.87% at −0.5 V (vs reversible\nhydrogen electrode) in 0.1 M Na₂SO₄, placing\nit as one of the most promising NRR electrocatalysts.