Volume 59, Issue 6 pp. 2510-2519
Research Article

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

Dr. Kalliopi Kousi

Corresponding Author

Dr. Kalliopi Kousi

School of Engineering, Newcastle University, Newcastle, Merz Court, NE1 7RU UK

These authors contributed equally to this work.

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Dr. Dragos Neagu

Corresponding Author

Dr. Dragos Neagu

School of Engineering, Newcastle University, Newcastle, Merz Court, NE1 7RU UK

These authors contributed equally to this work.

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Leonidas Bekris

Leonidas Bekris

School of Engineering, Newcastle University, Newcastle, Merz Court, NE1 7RU UK

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Dr. Evangelos I. Papaioannou

Dr. Evangelos I. Papaioannou

School of Engineering, Newcastle University, Newcastle, Merz Court, NE1 7RU UK

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Prof. Ian S. Metcalfe

Corresponding Author

Prof. Ian S. Metcalfe

School of Engineering, Newcastle University, Newcastle, Merz Court, NE1 7RU UK

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First published: 05 December 2019
Citations: 85

Graphical Abstract

Controlled growth of metallic nanoparticles at the surface and bulk of perovskite oxides induce strain and promote oxygen exchange with a methane stream leading to syngas production.

Abstract

Particles 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.

Conflict of interest

The authors declare no conflict of interest.

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