Abstract
Electrocatalytic Nitrogen Reduction Reaction (ECNRR) is a promising alternative NH3 production method relative to Haber-Bosch process. However, the ECNRR still suffers from rather low NH3 yield and selectivity (Faradaic efficiency (FE)) due to the poor catalytic activity of catalysts. Herein, benefiting from interface engineering, FeNi2S4/NiS hetero-interface electrocatalysts with unique electronic structures are successfully constructed, which the optimized catalyst can enhance the adsorption of N2 molecules meanwhile inhibit H atoms adsorption. Significantly, the NH3 yield and FE of FNS/CC-2 are reached to 128.398±1.32 μg h−1 cm−2 and 28.64 ± 0.18% which are higher than most of non-noble metal-based NRR electrocatalysts in alkaline electrolyte reported. Detailed experimental investigation and DFT calculations reveal that the enhanced electrocatalytic performance and selectivity of FeNi2S4/NiS towards N2 are attributed to the changes of the D-band center and electronic structure of electrocatalyst surface. The construction strategy of this NRR electrocatalyst provides a new avenue on electrocatalytic research.
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