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Cation-doping strategies for tuning of zirconia acid-base properties

Delarmelina, Maicon; Catlow, C Richard A; (2022) Cation-doping strategies for tuning of zirconia acid-base properties. Royal Society Open Science , 9 (2) , Article 211423. 10.1098/rsos.211423. Green open access

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Abstract

The role of Y-, Ca- and Ce-doping of cubic zirconia (c-ZrO2) (111) surface on its acidity, basicity and the interplay between surface acid-base pairs is investigated by computational methods. The most stable surface structures for this investigation were initially determined based on previous studies of Y-doped c-ZrO2 (111) and by a detailed exploration of the most stable configuration for Ca-doped c-ZrO2 (111) and Ce-doped c-ZrO2 (111). Next, surface mapping by basic probe molecules (NH3 and pyridine) revealed a general reduction of the acidity of the surface sites, although a few exceptions were observed for zirconium ions at next nearest neighbour (NNN) positions to the oxygen vacancy and at the nearest neighbour (NN) position to the dopants. Adsorption of CO2 over basic sites revealed a cooperative interplay between acid-base groups. In this case, the overall effect observed was the decrease of the calculated adsorption energies when compared with the pristine surface. Moreover, spontaneous formation of η 3-CO2 systems from initial η 2-CO2 configurations indicates a decrease in the required energy for forming oxygen vacancies in the doped ZrO2 systems at NNN positions or further away from the existing vacancy site.

Type: Article
Title: Cation-doping strategies for tuning of zirconia acid-base properties
Location: England
Open access status: An open access version is available from UCL Discovery
DOI: 10.1098/rsos.211423
Publisher version: http://dx.doi.org/10.1098/rsos.211423
Language: English
Additional information: © 2022 The Authors. Published by the Royal Society under the terms of the Creative Commons Attribution License http://creativecommons.org/licenses/by/4.0/, which permits unrestricted use, provided the original author and source are credited.
Keywords: acid–base properties, biofuel upgrading, biofuels, deoxygenation reactions, zirconia
UCL classification: 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
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL
URI: https://discovery.ucl.ac.uk/id/eprint/10144941
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