Abstract
The electroreduction of nitrate to ammonia is both an alternative strategy to industrial Haber-Bosch ammonia synthesis and a prospective idea for changing waste (nitrate pollution of groundwater around the world) into valuable chemicals, but still hindered by its in-process strongly competitive hydrogen evolution reaction (HER), low ammonia conversion efficiency, and the absence of stability and sustainability. Considering the unique electronic structure of anti-perovskite structured Fe4N, a tandem disproportionation reaction and nitridation-carbonation route for building a multi-layer core-shell oxide/nitride/C catalyst, such as MoO2/Fe4N/C, is designed and executed, in which abundant Fe-N active sites and rich phase interfaces are in situ formed for both suppressing HER and fast transport of electrons and reaction intermediates. As a result, the sample's NO3RR conversion displays a very high NH3 yield rate of up to 11.10 molNH3 gcat.-1 h-1 (1.67 mmol cm-2 h-1) with a superior 99.3% faradaic efficiency and the highest half-cell energy efficiency of 30%, surpassing that of most previous reports. In addition, it is proved that the NO3RR assisted by the MoO2/Fe4N/C electrocatalyst can be carried out in 0.50-1.00 M KNO3 electrolyte at a pH value of 6-14 for a long time. These results guide the rational design of highly active, selective, and durable electrocatalysts based on anti-perovskite Fe4N for the NO3RR.
Talk to us
Join us for a 30 min session where you can share your feedback and ask us any queries you have
Schedule a callDisclaimer: All third-party content on this website/platform is and will remain the property of their respective owners and is provided on "as is" basis without any warranties, express or implied. Use of third-party content does not indicate any affiliation, sponsorship with or endorsement by them. Any references to third-party content is to identify the corresponding services and shall be considered fair use under The CopyrightLaw.
