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Theoretical Insights into the hydrogen evolution reaction on the Ni3N electrocatalyst

Cross, Russell W., Rondiya, Sachin R. and Dzade, Nelson Y. 2021. Theoretical Insights into the hydrogen evolution reaction on the Ni3N electrocatalyst. Catalysts 11 (6) , 716. 10.3390/catal11060716

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Ni-based catalysts are attractive alternatives to noble metal electrocatalysts for the hydrogen evolution reaction (HER). Herein, we present a dispersion-corrected density functional theory (DFT-D3) insight into HER activity on the (111), (110), (001), and (100) surfaces of metallic nickel nitride (Ni3N). A combination of water and hydrogen adsorption was used to model the electrode interactions within the water splitting cell. Surface energies were used to characterise the stabilities of the Ni3N surfaces, along with adsorption energies to determine preferable sites for adsorbate interactions. The surface stability order was found to be (111) < (100) < (001) < (110), with calculated surface energies of 2.10, 2.27, 2.37, and 2.38 Jm−2, respectively. Water adsorption was found to be exothermic at all surfaces, and most favourable on the (111) surface, with Eads = −0.79 eV, followed closely by the (100), (110), and (001) surfaces at −0.66, −0.65, and −0.56 eV, respectively. The water splitting reaction was investigated at each surface to determine the rate determining Volmer step and the activation energies (Ea) for alkaline HER, which has thus far not been studied in detail for Ni3N. The Ea values for water splitting on the Ni3N surfaces were predicted in the order (001) < (111) < (110) < (100), which were 0.17, 0.73, 1.11, and 1.60 eV, respectively, overall showing the (001) surface to be most active for the Volmer step of water dissociation. Active hydrogen adsorption sites are also presented for acidic HER, evaluated through the ΔGH descriptor. The (110) surface was shown to have an extremely active Ni–N bridging site with ΔGH = −0.05 eV.

Item Type: Article
Date Type: Publication
Status: Published
Schools: Chemistry
Publisher: MDPI
ISSN: 2073-4344
Funders: EPSRC
Date of First Compliant Deposit: 16 June 2021
Date of Acceptance: 5 June 2021
Last Modified: 26 Oct 2021 01:08

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