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A DFT plus U investigation of hydrogen adsorption on the LaFeO3(010) surface

Boateng, IW; Tia, R; Adei, E; Dzade, NY; Catlow, CRA; De Leeuw, NH; (2017) A DFT plus U investigation of hydrogen adsorption on the LaFeO3(010) surface. Physical Chemistry Chemical Physics , 19 (10) pp. 7399-7409. 10.1039/C6CP08698E. Green open access

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Abstract

The ABO3 perovskite lanthanum ferrite (LaFeO3) is a technologically important electrode material for nickel–metal hydride batteries, energy storage and catalysis. However, the electrochemical hydrogen adsorption mechanism on LaFeO3 surfaces remains under debate. In the present study, we have employed spin-polarized density functional theory calculations, with the Hubbard U correction (DFT+U), to unravel the adsorption mechanism of H2 on the LaFeO3(010) surface. We show from our calculated adsorption energies that the preferred site for H2 adsorption is the Fe–O bridge site, with an adsorption energy of −1.18 eV (including the zero point energy), which resulted in the formation of FeOH and FeH surface species. H2 adsorption at the surface oxygen resulted in the formation of a water molecule, which leaves the surface to create an oxygen vacancy. The H2 molecule is found to interact weakly with the Fe and La sites, where it is only physisorbed. The electronic structures of the surface–adsorption systems are discussed via projected density of state and Löwdin population analyses. The implications of the calculated adsorption strengths and structures are discussed in terms of the improved design of nickel–metal hydride (Ni–MH) battery prototypes based on LaFeO3.

Type: Article
Title: A DFT plus U investigation of hydrogen adsorption on the LaFeO3(010) surface
Open access status: An open access version is available from UCL Discovery
DOI: 10.1039/C6CP08698E
Publisher version: https://doi.org/10.1039/C6CP08698E
Language: English
Additional information: This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions.
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry
URI: https://discovery.ucl.ac.uk/id/eprint/10065217
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