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Boosting Faradic efficiency of dinitrogen reduction on the negatively charged Mo sites modulated via interstitial Fe doping into a Mo2C nanowall catalyst
- Source :
- Chemical Engineering Journal. 417:127924
- Publication Year :
- 2021
- Publisher :
- Elsevier BV, 2021.
-
Abstract
- The electrochemical nitrogen reduction reaction (eNRR) provides a sustainable way to generate ammonia (NH3) but its Faradaic efficiency (FE) is relatively low and could be further improved, especially on the highly active molybdenum carbide (Mo2C) electrocatalyst. Our theoretical calculations suggest that unlike substitute doping model, interstitial Fe doping into Mo2C is highly eNRR-selective due to decreasing hydrogen evolution activity and unique surface-hydrogenation mechanism on negatively charged Mo sites around Fe atoms. Inspired by this prediction, we successfully developed a novel interstitial Fe doped Mo2C electrocatalyst by the pyrolysis of Fe-doped Mo/Zn bimetallic imidazolate frameworks (Fe-Mo/Zn BIFs) as a precursor where Fe atoms substitute Zn sites to obtain the spatial confinement effect. When evaluated in eNRR catalysis, Fe/Mo2C catalyst therefore exhibits a much higher FE of 20.1% at −0.45 V vs. RHE (reversible hydrogen electrode), which is almost double that of pristine Mo2C and substitute type. Moreover, the Fe/Mo2C catalyst also exhibits high ammonia yield rate with excellent durability over the six continuous cycles.
- Subjects :
- Materials science
General Chemical Engineering
Inorganic chemistry
Doping
02 engineering and technology
General Chemistry
010402 general chemistry
021001 nanoscience & nanotechnology
Electrochemistry
Electrocatalyst
01 natural sciences
Industrial and Manufacturing Engineering
0104 chemical sciences
Catalysis
chemistry.chemical_compound
chemistry
Imidazolate
Environmental Chemistry
Reversible hydrogen electrode
0210 nano-technology
Bimetallic strip
Faraday efficiency
Subjects
Details
- ISSN :
- 13858947
- Volume :
- 417
- Database :
- OpenAIRE
- Journal :
- Chemical Engineering Journal
- Accession number :
- edsair.doi...........fe033834499b5b0324373be9ef0fac01