Facile synthesis of coral-like nitrogen and sulfur co-doped carbon-encapsulated FeS2 for efficient electroreduction of nitrate to ammonia

Abstract

Electro-reduction of nitrate (NO3–) to ammonia is a promising method to transform the environmental contaminant NO3– to value-added ammonia. Since diverse end-products might be formed and a convenient material preparation process is preferable, it is of great importance to facilely synthesize a high-performance electro-catalyst towards ammonia generation with high selectivity. Herein, a coral-like nitrogen (N) and sulfur (S) co-doped carbon-encapsulated FeS2 composite material (FeS2@NSC) was successfully fabricated for effective electro-reduction of high-concentration of NO3– to ammonia through a simple one-step pyrolysis method. The FeS2@NSC-400 material exhibited remarkable electrocatalytic NH3 production performance with the NH3 yield of 4428.35 μg h−1 cm−2 and NH3 Faraday efficiency of 84.75 % at −1.4 V vs. Ag/AgCl, which outperforms many of the reported electrocatalysts. The unique small cluster coral-like core–shell structure, N, S co-doping and the interaction between inner FeS2 and the outer carbon layer greatly enhanced the electrical conductivity and stability of the material and the adsorption of NO3– and intermediate products, thereby facilitating the electrocatalytic performance of nitrate-to-ammonia. The FeS2@NSC material induced the electrocatalytic reduction of NO3– mainly through direct electron transfer instead of the indirect atomic H* mediation, and the main reduction product NH3 was speculated to derive from the pathway of NO3–* → NO2–* → NO* → HNO* → H2NO* → H2NOH* → NH3.