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Redox engineering of strontium titanate-based thermoelectrics

Kovalevsky, Andrei V. and Zakharchuk, Kiryl V. and Aguirre, Myriam H. and Xie, Wenjie and Patrício, Sonia G. and Ferreira, Nuno M. and Lopes, Diogo and Sergiienko, Sergii A. and Constantinescu, Gabriel and Mikhalev, Sergey M. and Weidenkaff, Anke and Frade, Jorge R. (2020):
Redox engineering of strontium titanate-based thermoelectrics.
In: Journal of Materials Chemistry A, (15), 8. Royal Society of Chemistry, pp. 7317-7330, ISSN 2050-7488,
DOI: 10.1039/c9ta13824b,
[Article]

Abstract

The development of thermoelectrics for high-temperature applications imposes several essentialrequirements on the material properties. In some energy-conversion scenarios, the cost and thermalstability requirements may dominate over efficiency issues, making abundant, high-temperature-stableand low-toxic oxides attractive alternative thermoelectric materials. As compared to“traditional”thermoelectrics, oxides possess unique redoxflexibility and defect chemistry, which can be preciselytuned by external temperature and oxygen partial pressure conditions. This work aims to demonstratehow, by redox-sensitive substitutions, the thermoelectric properties of oxides can be tuned andenhanced. The proposed strategy is exemplified by considering molybdenum-containing strontiumtitanate within nominally single-substituted and nanocomposite concepts. The involved materials designallows us to proceed from an in-depth understanding of the redox-promoted effects to thedemonstration of the enhanced thermoelectric performance attained by redox engineering. Synergisticenhancement of the Seebeck coefficient and suppression of the thermal conductivity due to combinedcarrierfiltering effects and efficient phonon scattering at redox-induced interfaces provided up to 25%increase in the thermoelectric performance. The results demonstrate extraordinaryflexibility of theperovskite lattice towards retaining a rich combination of the molybdenum redox states and shifting theirratio by tuning the A-site stoichiometry, and the prospects for developing new materials combiningthermoelectric and (electro)catalytic functionalities.

Item Type: Article
Erschienen: 2020
Creators: Kovalevsky, Andrei V. and Zakharchuk, Kiryl V. and Aguirre, Myriam H. and Xie, Wenjie and Patrício, Sonia G. and Ferreira, Nuno M. and Lopes, Diogo and Sergiienko, Sergii A. and Constantinescu, Gabriel and Mikhalev, Sergey M. and Weidenkaff, Anke and Frade, Jorge R.
Title: Redox engineering of strontium titanate-based thermoelectrics
Language: English
Abstract:

The development of thermoelectrics for high-temperature applications imposes several essentialrequirements on the material properties. In some energy-conversion scenarios, the cost and thermalstability requirements may dominate over efficiency issues, making abundant, high-temperature-stableand low-toxic oxides attractive alternative thermoelectric materials. As compared to“traditional”thermoelectrics, oxides possess unique redoxflexibility and defect chemistry, which can be preciselytuned by external temperature and oxygen partial pressure conditions. This work aims to demonstratehow, by redox-sensitive substitutions, the thermoelectric properties of oxides can be tuned andenhanced. The proposed strategy is exemplified by considering molybdenum-containing strontiumtitanate within nominally single-substituted and nanocomposite concepts. The involved materials designallows us to proceed from an in-depth understanding of the redox-promoted effects to thedemonstration of the enhanced thermoelectric performance attained by redox engineering. Synergisticenhancement of the Seebeck coefficient and suppression of the thermal conductivity due to combinedcarrierfiltering effects and efficient phonon scattering at redox-induced interfaces provided up to 25%increase in the thermoelectric performance. The results demonstrate extraordinaryflexibility of theperovskite lattice towards retaining a rich combination of the molybdenum redox states and shifting theirratio by tuning the A-site stoichiometry, and the prospects for developing new materials combiningthermoelectric and (electro)catalytic functionalities.

Journal or Publication Title: Journal of Materials Chemistry A
Journal volume: 8
Number: 15
Publisher: Royal Society of Chemistry
Divisions: 11 Department of Materials and Earth Sciences
11 Department of Materials and Earth Sciences > Material Science
11 Department of Materials and Earth Sciences > Material Science > Materials and Resources
Date Deposited: 22 May 2020 08:01
DOI: 10.1039/c9ta13824b
Projects: This work was supported by the project CICECO-Aveiro Instituteof Materials (ref. UIDB/50011/2020 & UIDP/50011/2020) and theproject POCI-01-0145-FEDER-031875,, nanced by COMPETE2020 Program and National Funds through the FCT/MEC andwhen applicable co-nanced by FEDER under the PT2020Partnership Agreement,, y the project UID/EMS/00481/2019-FCT and by Centro 2020, through the European RegionalDevelopment Fund (ERDF),, in the scope of the project CENTRO-01-0145-FEDER-022083.
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