Endogenous nanoparticles strain perovskite host lattice providing oxygen capacity and driving oxygen exchange and CH4 conversion to syngas

Kalliopi Kousi, Dragos Neagu, Leonidas Bekris, Evangelos I. Papaioannou, Ian S. Metcalfe

Research output: Contribution to journalArticle

2 Citations (Scopus)

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.

Original languageEnglish
Pages (from-to)2510-2519
Number of pages10
JournalAngewandte Chemie - International Edition
Volume59
Issue number6
Early online date5 Dec 2019
DOIs
Publication statusPublished - 3 Feb 2020

Keywords

  • chemical looping
  • exsolution
  • methane conversion
  • oxygen exchange/capacity
  • strain

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