A high-entropy manganite in an ordered nanocomposite for long-term application in solid oxide cells

F. Baiutti, F. Chiabrera, Matias Acosta, D. Diercks, D. Parfitt, J. Santiso, Xuejing Wang, A. Cavallaro, A. Morata, H. Wang, A. Chroneos, J. MacManus-Driscoll, A. Tarancon

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Abstract

The implementation of nano-engineered composite oxides opens up the way towards the development of a novel class of functional materials with enhanced electrochemical properties. Here we report on the realization of vertically aligned nanocomposites of lanthanum strontium manganite and doped ceria with straight applicability as functional layers in high-temperature energy conversion devices. By a detailed analysis using complementary state-of-the-art techniques, which include atom-probe tomography combined with oxygen isotopic exchange, we assess the local structural and electrochemical functionalities and we allow direct observation of local fast oxygen diffusion pathways. The resulting ordered mesostructure, which is characterized by a coherent, dense array of vertical interfaces, shows high electrochemically activity and suppressed dopant segregation. The latter is ascribed to spontaneous cationic intermixing enabling lattice stabilization, according to density functional theory calculations. This work highlights the relevance of local disorder and long-range arrangements for functional oxides nano-engineering and introduces an advanced method for the local analysis of mass transport phenomena.

Original languageEnglish
Article number2660
Number of pages11
JournalNature Communications
Volume12
Issue number1
DOIs
Publication statusPublished - 11 May 2021

Bibliographical note

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Funding

J.S. acknowledges the support of ICN2 (funded by the CERCA programme/Generalitat de Catalunya and by the Severo Ochoa programme SEV-2017-0706) for the XRD measurements. M.A. acknowledges the support from the Feodor Lynen Research Fellowship Program of the Alexander von Humboldt Foundation and the Isaac Newton Trust, 17.25(a). M.A. and J.D. acknowledge the support from the EPSRC Centre of Advanced Materials for Integrated Energy Systems (CAM-IES) under EP/P007767/1. J.D. also acknowledge support from EPSRC grants EP/N004272/1, EP/T012218/1, the Royal Academy of Engineering-CIET1819_24, ERC POC grant 779444, Portapower. X.W. and H.W. acknowledge the funding support from the U.S. National Science Foundation for the TEM effort at Purdue University (DMR-1565822 and DMR-2016453). This project has received funding from the European Union\u2019s Horizon 2020 research and innovation program under grant agreement No 824072 (HARVESTORE), No 681146 (ULTRA-SOFC) and No 101017709 (EPISTORE) and was supported by an STSM Grant from the COST Action MP1308: Towards Oxide-Based Electronics (TO-BE), supported by COST (European Cooperation in Science and Technology). The authors thank A. Aguadero for the fruitful discussions and A. Kuzyk for support on graphics.

FundersFunder number
Royal Academy of Engineering, The
EPSRC Centre of Advanced Materials for Integrated Energy Systems
The COST Association
Alexander von Humboldt-Stiftung
Horizon Europe681146, 824072, 101017709
Horizon Europe
Isaac Newton Trust17.25
Isaac Newton Trust
CERCA programme/Generalitat de CatalunyaSEV-2017-0706
Engineering and Physical Sciences Research CouncilEP/T012218/1, EP/N004272/1
Engineering and Physical Sciences Research Council
Purdue UniversityDMR-2016453, DMR-1565822
Purdue University
EPSRC Centre of Advanced Materials for Integrated Energy SystemsEP/P007767/1
European Research Council779444
European Research Council
National Science Foundation2016453
National Science Foundation

ASJC Scopus subject areas

  • General Chemistry
  • General Biochemistry,Genetics and Molecular Biology
  • General Physics and Astronomy

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