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Endogenous Nanoparticles Strain Perovskite Host Lattice Providing Oxygen Capacity and Driving Oxygen Exchange and CH4 Conversion to Syngas

Lookup NU author(s): Dr Kelly Kousi, Dr Dragos Neagu, Leonidas Bekris, Dr Evangelos Papaioannou, Professor Ian Metcalfe

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This is the authors' accepted manuscript of an article that has been published in its final definitive form by Wiley - VCH Verlag GmbH & Co. KGaA, 2020.

For re-use rights please refer to the publisher's terms and conditions.


Abstract

© 2020 Wiley-VCH Verlag GmbH & Co. KGaA, WeinheimParticles dispersed on the surface of oxide supports have enabled a wealth of applications in electrocatalysis, photocatalysis, and heterogeneous catalysis. Dispersing nanoparticles within the bulk of oxides is, however, synthetically much more challenging and therefore less explored, but could open new dimensions to control material properties analogous to substitutional doping of ions in crystal lattices. Here we demonstrate such a concept allowing extensive, controlled growth of metallic nanoparticles, at nanoscale proximity, within a perovskite oxide lattice as well as on its surface. By employing operando techniques, we show that in the emergent nanostructure, the endogenous nanoparticles and the perovskite lattice become reciprocally strained and seamlessly connected, enabling enhanced oxygen exchange. Additionally, even deeply embedded nanoparticles can reversibly exchange oxygen with a methane stream, driving its redox conversion to syngas with remarkable selectivity and long term cyclability while surface particles are present. These results not only exemplify the means to create extensive, self-strained nanoarchitectures with enhanced oxygen transport and storage capabilities, but also demonstrate that deeply submerged, redox-active nanoparticles could be entirely accessible to reaction environments, driving redox transformations and thus offering intriguing new alternatives to design materials underpinning several energy conversion technologies.


Publication metadata

Author(s): Kousi K, Neagu D, Bekris L, Papaioannou EI, Metcalfe IS

Publication type: Article

Publication status: Published

Journal: Angewandte Chemie - International Edition

Year: 2020

Volume: 59

Issue: 6

Pages: 2510-2519

Print publication date: 27/01/2020

Online publication date: 05/12/2019

Acceptance date: 05/12/2019

Date deposited: 27/01/2020

ISSN (print): 1433-7851

ISSN (electronic): 1521-3773

Publisher: Wiley - VCH Verlag GmbH & Co. KGaA

URL: https://doi.org/10.1002/anie.201915140

DOI: 10.1002/anie.201915140

Data Source Location: https://doi.org/10.25405/data.ncl.11302853


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