Enhancing Electrocatalytic Nitrogen Fixation over Core-Shell P-Sb2S3/MoS2 Heterojunction by Vacancy and Interface Modulation

Electrochemical synthesis of ammonia is a green and sustainable way for nitrogen fixation, but the development of efficient electrocatalysts still faces challenges. The modulation of electronic structure through interface engineering and vacancy engineering is a new approach to enhance the performance of electrocatalysts. In this work, a phosphorus-doped core–shell heterojunction P-Sb2S3/MoS2 was designed and synthesized by combining antimony, which is inert to H+ adsorption, with molybdenum, which has good affinity and reducibility with nitrogen. The synthesis involved both interfacial engineering and vacancy engineering strategies.DFT calculations demonstrate that the formationofSb2S3/MoS2 heterojunction enhances the creation of a built-in electric field, thereby expediting electron flow.Additionally, phosphorus doping induced the formation of abundant sulfur vacancies, significantly enhancing nitrogen adsorption performance in this material.As a result, our designed structure exhibited excellent NRR performance with an ammonia production rate of 41.22 μg·h−1·mg−1cat and a Faraday efficiency of 15.70 %.The unique structural of this catalyst contribute to a more optimal balance between the rate of ammonia production and the Faraday efficiency. The successful preparation of the highly efficient P-Sb2S3/MoS2 heterojunctionsprovidesanew strategyfor catalyst design in electrocatalytic nitrogen reduction.