Preparation And Electrocatalytic Nitrogen Reduction Reaction Study Of Carbon Nitrogen Iron-based Compound Materials

Ammonia is considered as one of the most important chemical industrial raw material,also it is necessary for producing chemical fertilizer and chemical fiber.Electrochemical nitrogen reduction reaction（ENRR）is substitute for traditional Haber-Bosch Process,which is considered as the most eco-friendly method to produce ammonia.It does not require a high temperature and pressure environment and does not produce carbon dioxide emissions during the process.However,for electrocatalytic nitrogen reduction to synthesize ammonia,the low selectivity of the catalyst,low ammonia yield and low Faraday efficiency all limit the development of electrocatalytic nitrogen reduction to synthesize ammonia.Among many transition metals,Fe is the most reserved element on the earth,which has empty d orbit and good ENRR activity.Carbon-Nitrogen materials attract many studiers due to its high electrical conductivity and good ductility.So,in this article Carbon-Nitrogen iron based catalyst was studied in ENRR,which includes two parts of experimental content:（1）In order to obtain a nitrogen reduction reaction catalyst with high-performance,in this article,ZIF-67 precursor was used to prepare amorphous Co S-NC through solution sulfidation and calcination,and then etched by iron ion.It is obvious that the carbon-based composite material has a tendency to transform from the 12-sided morphology of the precursor ZIF-67 to a cube through SEM characterization,meanwhile,Fe₂O₃ is mainly distributed on the surface of the cube.The research shows that this amorphous Fe₂O₃/Co S-NC material has good electrocatalytic nitrogen reduction reaction performance with 23.78μg/h/cm² yield and 11.17%FE.（2）Secondly,to study more iron composite carbon-based material catalysts.In this paper,a carbon-based material composed of iron and iron oxide was prepared by the complex method.Ingeniously selecting specific reactants and controlling the calcination atmosphere method,micron-sized Fe-N-C（Particles）and Fe₃O₄-N-C with porous structure were prepared.Electrochemical test results show that the Fe-N-C catalyst has good electrocatalytic nitrogen reduction reaction performance in 0.1M Na₂SO₄ solution with123μg/h/cm² yield and 78.16%FE.