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A Janus Fe‐SnO<sub>2</sub>Catalyst that Enables Bifunctional Electrochemical Nitrogen Fixation

279

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55

References

2020

Year

Abstract

Electrochemical N<sub>2</sub> reduction reactions (NRR) and the N<sub>2</sub> oxidation reaction (NOR), using H<sub>2</sub> O and N<sub>2</sub> , are a sustainable approach to N<sub>2</sub> fixation. To date, owing to the chemical inertness of nitrogen, emerging electrocatalysts for the electrochemical NRR and NOR at room temperature and atmospheric pressure remain largely underexplored. Herein, a new-type Fe-SnO<sub>2</sub> was designed as a Janus electrocatalyst for achieving highly efficient NRR and NOR catalysis. A high NH<sub>3</sub> yield of 82.7 μg h<sup>-1</sup> mg<sub>cat.</sub> <sup>-1</sup> and a Faraday efficiency (FE) of 20.4 % were obtained for NRR. This catalyst can also serve as an excellent NOR electrocatalyst with a NO<sub>3</sub> <sup>-</sup> yields of 42.9 μg h<sup>-1</sup> mg<sub>cat.</sub> <sup>-1</sup> and a FE of 0.84 %. By means of experiments and DFT calculations, it is revealed that the oxygen vacancy-anchored single-atom Fe can effectively adsorb and activate chemical inert N<sub>2</sub> molecules, lowering the energy barrier for the vital breakage of N≡N and resulting in the enhanced N<sub>2</sub> fixation performance.

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