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Bio-Inspired Aerobic-Hydrophobic Janus Interface on Partially Carbonized Iron Heterostructure Promotes Bifunctional Nitrogen Fixation.

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Zong, Wei 
Gao, Haiqi 
Ouyang, Yue 
Chu, Kaibin 
Guo, Hele 


Competition from hydrogen/oxygen evolution reactions and low solubility of N2 in aqueous systems limited the selectivity and activity on nitrogen fixation reaction. Herein, we design an aerobic-hydrophobic Janus structure by introducing fluorinated modification on porous carbon nanofibers embedded with partially carbonized iron heterojunctions (Fe3 C/Fe@PCNF-F). The simulations prove that the Janus structure can keep the internal Fe3 C/Fe@PCNF-F away from water infiltration and endow a N2 molecular-concentrating effect, suppressing the competing reactions and overcoming the mass-transfer limitations to build a robust "quasi-solid-gas" state micro-domain around the catalyst surface. In this proof-of-concept system, the Fe3 C/Fe@PCNF-F exhibits excellent electrocatalytic performance for nitrogen fixation (NH3 yield rate up to 29.2 μg h-1  mg-1 cat. and Faraday efficiency (FE) up to 27.8 % in nitrogen reduction reaction; NO3 - yield rate up to 15.7 μg h-1  mg-1 cat. and FE up to 3.4 % in nitrogen oxidation reaction).



Aerobic-Hydrophobic, Bio-Inspired, Janus, Nitrogen Fixation, Quasi-Solid-Gas State

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Angew Chem Int Ed Engl

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National Natural Science Foundation of China (52161135302, 52211530489, 22075042)
Fonds Wetenschappelijk Onderzoek (G0F2322N, 1298323N, G983.19N, G0A5817N, VS06523N, ZW15_09-G0H6316N)
Natural Science Foundation of Shanghai (20ZR1401400, 18ZR1401600)