resumo
Inspired by recent research results that have demonstrated appealing thermoelectric performance of A-site cation-deficient titanates, this work focuses on detailed analysis of the changes in performance promoted by altering the defect chemistry mechanisms. The series of cation-stoichiometric SrTi1-xTaxO3 +/-delta and A-site deficient Sr1-x/2Ti1-xTaxO3-delta compositions (0.05 <= x <= 0.30) with cubic perovskite-like structure were selected to demonstrate the defect chemistry engineering approaches, which result in promising electric and thermal properties. High power factors were observed in compositions where appropriate concentration of the charge carriers and their mobility were attained by the presence of strontium- and oxygen vacancies and suppressed formation of the oxygen-rich layers. Noticeable deviations from stoichiometric oxygen content were found to decrease the lattice thermal conductivity, suggesting good phonon scattering ability for oxygen vacancies, vacant A-sites, and oxygen-excessive defects, while the effect from donor substitution on the thermal transport was less pronounced. The obtained guidelines for the defect chemistry engineering in donor-substituted strontium titanates open new possibilities for boosting the thermoelectric performance, especially if followed by complementary microstructural design to further promote electrical and thermal transport.
palavras-chave
NB-DOPED SRTIO3; LATTICE THERMAL-CONDUCTIVITY; TRANSPORT-PROPERTIES; POWER-GENERATION; SYSTEM; PROGRESS; OXIDES
categoria
Chemistry; Materials Science
autores
Yaremchenko, AA; Populoh, S; Patricio, SG; Macias, J; Thiel, P; Fagg, DP; Weidenkaff, A; Frade, JR; Kovalevsky, AV
nossos autores
Aleksey Yaremchenko
Investigador Principal
Andrei Kavaleuski
Investigador principal
Javier Macias Montiel
Estudante de doutoramento
Jorge Ribeiro Frade
Professor(a) Jubilado(a)
Sónia Gonçalves Patrício
Investigador AuxiliarGrupos
G3 - Materiais Eletroquímicos, Interfaces e Revestimentos
G5 - Materiais Biomiméticos, Biológicos e Vivos
agradecimentos
This work was supported by the FCT Investigador program (grants IF/00302/2012 and IF/01072/2013) and was developed within the scope of projects BPD/75943/2011, SFRH/BD/91675/2012, and project CICECO-Aveiro Institute of Materials (ref UID/CTM/50011/2013), financed by national funds through the FCT/MEC and when applicable cofinanced by FEDER under the PT2020 Partnership Agreement. Financial support from the Competence Centre Energy and Mobility (CCEM), the Swiss Federal Office of Energy (BfE) within the HITTEC project is also greatly acknowledged. The authors are thankful to Prof. Carlos Sa (CEMUP) for performing XPS studies and helpful discussion of the results, M. J. de Pinho Bastos (UA) for her assistance with XRD analysis, and to Dr. S. M. Mikhalev for his technical support.