Iron Nanoparticles Protected by Chainmail-structured Graphene for Durable Electrocatalytic Nitrate Reduction to Nitrogen.

The electrochemical nitrate reduction reaction (NO3RR) is an appealing technology for regulating the nitrogen cycle. Metallic iron is one of the well-known electrocatalysts for NO3RR, but it suffers from poor durability due to leaching and oxidation of iron during the electrocatalytic process. In this work, a graphene-nanochainmail-protected iron nanoparticle (Fe@Gnc) electrocatalyst is reported. It displays superior nitrate removal efficiency and high nitrogen selectivity. Notably, the catalyst delivers exceptional stability and durability, with the nitrate removal rate and nitrogen selectivity remained ~96% of that of the first time after up to 40 cycles (24 h for one cycle). As expected, the conductive graphene nanochainmail provides robust protection for the internal iron active sites, allowing Fe@Gnc to maintain its long-lasting electrochemical nitrate catalytic activity. This research proposes a workable solution for the scientific challenge of poor lasting ability of iron-based electrocatalysts in large-scale industrialization.