C18-thiol modified Fe-MoSe2 nanosheets for efficient electrocatalytic nitrogen fixation
Achieving high ammonia yield and Faraday efficiency is a long-sought-after goal in electrochemical N 2 fixation. Yet, the competitive hydrogen evolution in nitrogen reduction process and the low local concentration of nitrogen on the working electrode still limited the electrocatalytic performance. In the present contribution, a Fe-MoSe 2 nanosheet functioned with C18-thiol as a nano-hydrophobic surface was rationally constructed, which efficiently facilitated the three-phase contact of gas (N 2 ), liquid (H 2 O electrolyte), and solid (electrocatalyst). The fabrication of modified hydrophobic surface not only overcame the mass transfer limitation of N 2 and increased the local concentration of N 2 molecules on the catalyst, but also reduced the proton contact with electrocatalyst to inhibit HER. The three-phase electrocatalytic system achieved a high NH 3 yield of 34.75 μg h −1 mg −1 and outstanding Faraday efficiency of 23.31%. The adsorption and activation processes during NRR process were systematically investigated by the combination of experimental results and density function theory (DFT) simulations.
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