A Janus Fe‐SnO2 Catalyst that Enables Bifunctional Electrochemical Nitrogen Fixation. Issue 27 (8th May 2020) - Zhang, Linlin
Abstract: Electrochemical N2 reduction reactions (NRR) and the N2 oxidation reaction (NOR), using H2 O and N2, are a sustainable approach to N2 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‐SnO2 was designed as a Janus electrocatalyst for achieving highly efficient NRR and NOR catalysis. A high NH3 yield of 82.7 μg h −1 mgcat. −1 and a Faraday efficiency (FE) of 20.4 % were obtained for NRR. This catalyst can also serve as an excellent NOR electrocatalyst with a NO3 − yields of 42.9 μg h −1 mgcat. −1 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 N2 molecules, lowering the energy barrier for the vital breakage of N≡N and resulting in the enhanced N2 fixation performance. Abstract : NRR and NOR : Fe‐SnO2 was synthesized as an electrocatalyst for both N2 reduction and oxidation (NRR and NOR). The Fe in Fe‐SnO2 acts as oxygen vacancy anchored Fe and lattice doped Fe, which enhances the adsorption and activation of N2 on SnO2 and improves the electrical conductivity of SnO2 . The catalyst exhibited excellent catalytic performance (NRR: NH3 yield 82.7 μg h −1 mgcat. −1, FE 20.4 %; NOR: NO3 − yield 42.9 μg h −1 mgcat. −1, FE 0.84 %).