Competing dopants grain boundary segregation and resultant seebeck coefficient and power factor enhancement of thermoelectric calcium cobaltite ceramics

Boyle, Cullen; Liang, Liang; Chen, Yun; Prucz, Jacky; Cakmak, Ercan; Watkins, Thomas R.; Lara-Curzio, Edgar; Song, Xueyan

doi:10.1016/j.ceramint.2017.06.029

Title: Competing dopants grain boundary segregation and resultant seebeck coefficient and power factor enhancement of thermoelectric calcium cobaltite ceramics

Journal Article · Tue Jun 06 00:00:00 EDT 2017 · Ceramics International

DOI:https://doi.org/10.1016/j.ceramint.2017.06.029· OSTI ID:1436959

Boyle, Cullen ^[1]; Liang, Liang ^[1]; Chen, Yun ^[1]; Prucz, Jacky ^[1];

^[2];

^[2]; Song, Xueyan ^[1]

West Virginia Univ., Morgantown, WV (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Here, the present work demonstrates the feasibility of increasing the values of Seebeck coefficient S and power factor of calcium cobaltite Ca₃Co₄O₉ ceramics through competing dopant grain boundary segregation. The nominal chemistry of the polycrystalline material system investigated is Ca_3–xBi_xBa_yCo₄O₉ with simultaneous stoichiometric substitution of Bi for Ca and non-stoichiometric addition of minute amounts of Ba. There is continuous increase of S due to Bi substitution and Ba addition. The electrical resistivity also changes upon doping. Overall, the power factor of best performing Bi and Ba co-doped sample is about 0.93 mW m^–1 K^–2, which is one of the highest power factor values ever reported for Ca₃Co₄O₉, and corresponds to a factor of 3 increase compared to that of the baseline composition Ca₃Co₄O₉. Systematic nanostructure and chemistry characterization was performed on the samples with different nominal compositions. When Bi is the only dopant in Ca₃Co₄O₉, it can be found at both the grain interior and the grain boundaries GBs as a result of segregation. When Bi and Ba are added simultaneously as dopants, competing processes lead to the segregation of Ba and depletion of Bi at the GBs, with Bi present only in the grain interior. Bi substitution in the lattice increases the S at both the low and high temperature regimes, while the segregation of Ba at the GBs dramatically increase the S at low temperature regime.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Revolutionary Materials for Solid State Energy Conversion (RMSSEC); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725; SC0001054

OSTI ID:: 1436959

Alternate ID(s):: OSTI ID: 1550159

Journal Information:: Ceramics International, Vol. 43, Issue 14; ISSN 0272-8842

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 13 works

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Cited By (2)

Influence of pressure assisted sintering and reaction sintering on microstructure and thermoelectric properties of bi-doped and undoped calcium cobaltite Bresch, Sophie; Mieller, Bjoern; Schoenauer-Kamin, Daniela Journal of Applied Physics, Vol. 126, Issue 7 https://doi.org/10.1063/1.5107476	journal	August 2019
Role of oversized dopant potassium on the nanostructure and thermoelectric performance of calcium cobaltite ceramics Romo-De-La-Cruz, C.; Liang, L.; Navia, S. A. Paredes Sustainable Energy & Fuels, Vol. 2, Issue 4 https://doi.org/10.1039/c7se00612h	journal	January 2018

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Title: Competing dopants grain boundary segregation and resultant seebeck coefficient and power factor enhancement of thermoelectric calcium cobaltite ceramics

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