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Understanding defect generation on CeO2 and its utilization for enhanced metal-support interactions in Ni/CeO2 catalysts for improved CO2 methanation performance

Chen, Sining; Costley-Wood, Lucy; Lezcano-Gonzalez, Ines; Campbell, Emma; Weng, Zhaoyue; Asunción Molina, M; Wu, Yani; (2025) Understanding defect generation on CeO2 and its utilization for enhanced metal-support interactions in Ni/CeO2 catalysts for improved CO2 methanation performance. Applied Catalysis B: Environment and Energy , 366 , Article 125029. 10.1016/j.apcatb.2025.125029. Green open access

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Abstract

A series of CeO2 supports were treated in an N2 plasma before being impregnated with Ni precursors to evaluate the impact this has on the metal-support interface and catalytic performance. This impact was determined using a suite of characterization methods including X-ray diffraction (XRD), H2 temperature-programmed reduction (H2-TPR), ex situ and in situ X-ray absorption spectroscopy (XAS) and in situ Kerr-gated Raman. The combined and self-consistent results indicated that plasma treatment of CeO2 can lead to the generation of an increasing number of oxygen vacancies, and a loss of long-range order in samples treated for 1 h, realizing a highly defective CeOx film at the interface between the Ni metal nanoparticles and bulk CeO2. However, this highly defective CeOx surface significantly enhances the Ni-CeOx interaction, resulting in a number of smaller Ni NPs in intimate contact with the support, leading to improved catalytic performance for CO2 methanation. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) revealed that the more defect-dense Ni−CeOx interface leads to the formation of more bidentate bridged carbonates (vs. bidentate chelate) and which are more readily consumed during reaction, suggesting the identification of an important parameter to effect low-temperature (< 300 °C) CH4 production.

Type: Article
Title: Understanding defect generation on CeO2 and its utilization for enhanced metal-support interactions in Ni/CeO2 catalysts for improved CO2 methanation performance
Open access status: An open access version is available from UCL Discovery
DOI: 10.1016/j.apcatb.2025.125029
Publisher version: https://doi.org/10.1016/j.apcatb.2025.125029
Language: English
Additional information: Copyright © 2025 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/).
Keywords: CO2 hydrogenation; Oxygen vacancies; Metal-support interface; Ni/CeO2; Non-thermal plasma
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/10204030
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