Suppression of Hydrogen Evolution Reaction in Electrochemical N2 Reduction Using Single-Atom Catalysts: A Computational Guideline

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We studied electrochemical nitrogen reduction reactions (NRR) to ammonia on single atom catalysts (SACs) anchored on defective graphene derivatives by density functional calculations. We find significantly improved NRR selectivity on SACs compared to that on the existing bulk metal surface due to the great suppression of the hydrogen evolution reaction (HER) on SACs with the help of the ensemble effect. In addition, several SACs, including Ti@N-4 (0.69 eV) and V@N-4 (0.87 eV), are shown to exhibit lower free energy for NRR than that of the Ru(0001) stepped surface (0.98 eV) due to a strong back-bonding between the hybridized d-orbital metal atom in SAC and pi* orbital in *N-2. Formation energies as a function of nitrogen chemical potential suggest that Ti@N-4 and V@N-4 are also synthesizable under experimental conditions.
Publisher
AMER CHEMICAL SOC
Issue Date
2018-08
Language
English
Article Type
Article
Keywords

AMMONIA-SYNTHESIS; CO2 REDUCTION; ELECTROCATALYTIC REDUCTION; ORGANIC FRAMEWORKS; AMBIENT CONDITIONS; NITROGEN; ELECTROREDUCTION; NITRIDE; DFT; SELECTIVITY

Citation

ACS CATALYSIS, v.8, no.8, pp.7517 - 7525

ISSN
2155-5435
DOI
10.1021/acscatal.8b00905
URI
http://hdl.handle.net/10203/245929
Appears in Collection
NT-Journal Papers(저널논문)EEW-Journal Papers(저널논문)
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