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6CCVD Research

Electrocatalytic nitrogen reduction on defective graphene modulated from single atom catalyst to aluminium clusters

At a Glance

Section titled ā€œAt a Glanceā€
MetadataDetails
Publication Date2023-03-15
JournalApplied Surface Science
AuthorsAshakiran Maibam, SaĆÆlaja Krishnamurty, Ravichandar Babarao
InstitutionsAcademy of Scientific and Innovative Research, National Chemical Laboratory
Citations7

Abstract

Section titled ā€œAbstractā€

Density Functional Theory (DFT) investigation on the most earth-abundant Al-based catalysts, has been conducted detailing its electronic properties and catalytic efficacy for nitrogen reduction at ambient condition. The Al-based catalysts have been modulated to perform as par a highly performing, but rare, Ru-single atom catalytic center by varying number of Al atoms, shape, and size. The coalesce of band-center, work function and electronic properties in metal atom catalysts along with N-N bond activation has been demonstrated to be responsible for an efficient nitrogen reduction reaction (NRR) with Ī”Gmax of 0.78 eV in Al5 supported on N-doped double vacancy graphene (Al5@N4-DVG) catalyst. Electron localization function analysis has shown a weak physisorption of N2 in the Al-based catalysts. Projected Density of States (PDOS) illustrates the enhancement of aluminium electron density in Al5@N4-DVG led to enhanced orbital densities overlap of Alp and Np electrons. The Bader charge analysis and electronic analysis of the intermediates show efficient electron gain on the N atoms, leading to formation of NH3 from the NxHy intermediates in Al5@N4-DVG catalyst.

Tech Support

Section titled ā€œTech Supportā€

Original Source

Section titled ā€œOriginal Sourceā€

References

Section titled ā€œReferencesā€
  1. 2015 - A review of the existing and alternative methods for greener nitrogen fixation [Crossref]
  2. 2014 - Challenges in reduction of dinitrogen by proton and electron transfer [Crossref]
  3. 2021 - Development of Electrocatalysts for Efficient Nitrogen Reduction Reaction under Ambient Condition
  4. 2021 - Electrochemical nitrogen reduction: recent progress and prospects [Crossref]
  5. 2018 - Ambient ammonia synthesis via palladium-catalyzed electrohydrogenation of dinitrogen at low overpotential
  6. 2018 - Electrochemical synthesis of ammonia from N2 and H2O under ambient conditions using pore-size-controlled hollow gold nanocatalysts with tunable plasmonic properties [Crossref]
  7. 2018 - Achieving a record-high yield Rate of 120.9 Ī¼g NH3mgcat.āˆ’1hāˆ’1 for N2 electrochemical reduction over Ru single-atom catalysts
  8. 2018 - MoO3 nanosheets for efficient electrocatalytic N2 fixation to NH3 [Crossref]
  9. 2019 - Over 56.55% Faradaic efficiency of ambient ammonia synthesis enabled by positively shifting the reaction potential
  10. 2018 - Hierarchical cobalt phosphide hollow nanocages toward electrocatalytic ammonia synthesis under ambient pressure and room temperature, Small

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