Issue 20, 2023, Issue in Progress

Neutron diffraction and DFT studies of oxygen defect and transport in higher-order Ruddlesden–Popper phase materials

Abstract

A series of higher-order Ruddlesden–Popper phase materials – La3PrNi3O10−δ, La2Pr2Ni3O10−δ and LaPr3Ni3O10−δ – were synthesised and investigated by neutron powder diffraction to understand the oxygen defect structure and propose possible pathways for oxygen transport in these materials. Further complimentary DFT calculations of the materials were performed to support the experimental analysis. All of the phases were hypostoichiometric and it was observed that the majority of the oxygen vacancies were confined to the perovskite layers, with a preference for equatorial oxygen sites. A particular preference for vacancies in O(1) and O(5) sites at high temperatures was observed from neutron diffraction measurements which were further complimented by DFT calculations wherein the vacancy formation energy was found to be lowest at the O(1) site. Also, a preference for a curved oxygen transport pathway around the NiO6 octahedra was observed which agrees with the published literature for Ruddlesden–Popper phase materials. Lattice parameters for all three compositions showed a linear increase with increasing temperature, but the increase was greatest in the c parameter while the b parameter showed only a slight increase when compared to the a parameter. The thermal expansion coefficient was calculated for all compositions and was found to be in the range 13.0–13.4 × 10−6 °C−1, which is compatible with the commonly used electrolyte materials for solid oxide fuel cells.

Graphical abstract: Neutron diffraction and DFT studies of oxygen defect and transport in higher-order Ruddlesden–Popper phase materials

Supplementary files

Article information

Article type
Paper
Submitted
17 Mar 2023
Accepted
24 Apr 2023
First published
05 May 2023
This article is Open Access
Creative Commons BY license

RSC Adv., 2023,13, 13786-13797

Neutron diffraction and DFT studies of oxygen defect and transport in higher-order Ruddlesden–Popper phase materials

M. A. Yatoo, I. D. Seymour and S. J. Skinner, RSC Adv., 2023, 13, 13786 DOI: 10.1039/D3RA01772A

This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. You can use material from this article in other publications without requesting further permissions from the RSC, provided that the correct acknowledgement is given.

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