Single-atom catalysts templated by metal-organic frameworks for electrochemical nitrogen reduction

The electrocatalytic nitrogen reduction reaction (NRR) has much prospect for substituting the energy-consuming Haber-Bosch process. Nevertheless, its sluggish reaction kinetics and the competing hydrogen evolution reaction always result in limited ammonia yield and low faradaic efficiency (FE). In t...

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Bibliographic Details
Published in:Journal of materials chemistry. A, Materials for energy and sustainability Materials for energy and sustainability, 2019, Vol.7 (46), p.26371-26377
Main Authors: Zhang, Rui, Jiao, Long, Yang, Weijie, Wan, Gang, Jiang, Hai-Long
Format: Article
Language:English
Subjects:
Ammonia
Catalysts
Chemical reduction
Electrochemistry
Hydrogen evolution reactions
INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Iron
Metal-organic frameworks
Metals
Nitrogen
Reaction kinetics
Single atom catalysts
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Summary:The electrocatalytic nitrogen reduction reaction (NRR) has much prospect for substituting the energy-consuming Haber-Bosch process. Nevertheless, its sluggish reaction kinetics and the competing hydrogen evolution reaction always result in limited ammonia yield and low faradaic efficiency (FE). In this work, an Fe-decorated porphyrinic metal-organic framework (MOF) is employed as a precursor to construct single-atom Fe implanted nitrogen-doped carbon catalysts (Fe 1 -N-C) through a mixed ligand strategy. Benefiting from the highly dispersed single-atom Fe sites, hierarchically porous structure and good conductivity, Fe 1 -N-C shows a FE of 4.51% and an ammonia yield rate of 1.56 × 10 −11 mol cm −2 s −1 at −0.05 V versus the reversible hydrogen electrode, superior to those of Co 1 -N-C and Ni 1 -N-C. Theoretical calculations reveal that Fe 1 -N-C shows the lowest energy barrier of the rate-determining step during the NRR process, consistent with its highest activity obtained in experiments. This work reveals the unique potential of single-atom catalysts for the electrochemical NRR and provides in-depth insights into the catalytic mechanism of the NRR. Metal-organic framework precursors were employed to fabricate single-atom catalysts, where Fe implanted nitrogen-doped carbon (Fe 1 -N-C) exhibits excellent performance for electrocatalytic nitrogen reduction in acidic media.
ISSN:2050-7488
2050-7496
DOI:10.1039/c9ta10206j