Mixed protonic-electronic conductivity in barium lanthanide cobaltites: from simple perovskites to high entropy materials.

Sebastian Wachowski^a, Hanna Kavaliuk^a, Iga Szpunar^b, Aleksandra Mielewczyk-Gryń^a, Tadeusz Miruszewski^a, Ragnar Strandbakke^d^,^e, Maria Balaguer^c

^aInstitute of Nanotechnology and Materials Engineering, Faculty of Applied Physics and Mathematics, and Advanced Materials Centre, Gdańsk University of Technology, Narutowicza 11/12, 80-233 Gdańsk, Poland

^bGdańsk University of Technology, Faculty of Electronics, Telecommunications and Informatics

^cInstituto de Tecnología Química (Universitat Politècnica de València – Consejo Superior de Investigaciones Científicas), Av. Los Naranjos, s/n, 46022 Valencia, Spain

^dSINTEF Materials and Chemistry (NO)

^eDepartment of Chemistry, Centre for Materials Science and Nanotechnology, University of Oslo

Proceedings of 24th International Conference on Solid State Ionics (SSI24)

Emerging Materials for High-Performance Devices

London, United Kingdom, 2024 July 14th - 19th

Organizers: John Kilner and Stephen Skinner

Oral, Sebastian Wachowski, presentation 621
Publication date: 10th April 2024

Barium lanthanide cobaltites with perovskite structure have been studied as potential electrodes for electrochemical cells due to their mixed oxygen ionic – electronic conductivity[1]. More recently[2,3], protonic defect formation has been shown in some of these oxides. Moreover, our previous studies have shown that compositional complexity induces changes in both the structure and transport properties of this system[4]. Therefore, we decided to take a step further and leverage the emerging field of high entropy oxides. In these materials, compositional complexity is taken to the extreme by introducing up to a dozen (or even more) cations into one sublattice[5]. This approach allows for the discovery of new material properties and the enhancement of features such as electronic and/or ionic conductivities

This talk will focus on how structure, chemical composition and electronic states affect protonic defect formation and total conductivity of BaLnCo₂Fe_1-xO_6-δ. The study explores first simple compositions with one or two different lanthanides on the A-site and then introduces up to 12 different elements in one sublattice in equimolar proportions (e.g. BaLa_1/12Ce_1/12Pr_1/12 Nd_1/12 Sm_1/12 Eu_1/12 Gd_1/12Tb_1/12Dy_1/12Ho_1/12Er_1/12Tm_1/12Co₂O_6-δ). We evaluate changes in structure, total conductivity, Seebeck coefficient and water uptake occurring as an effect of introducing multiple elements in one sublattice. For selected compositions partial protonic conductivity is measured using a modified Hebb-Wagner DC polarization method.

References:

[1] R. Pelosato, G. Cordaro, D. Stucchi, C. Cristiani, G. Dotelli, Cobalt based layered perovskites as cathode material for intermediate temperature Solid Oxide Fuel Cells: A brief review, J. Power Sources. 298 (2015) 46–67.

[2] S.L. Wachowski, I. Szpunar, M.H. Sørby, A. Mielewczyk–Gryń, M. Balaguer, C. Ghica, M.C. Istrate, M. Gazda, A.E. Gunnæs, J.M. Serra, T. Norby, R. Strandbakke, Structure and water uptake in BaLnCo2O6−δ (Ln =La, Pr, Nd, Sm, Gd, Tb and Dy), Acta Mater. 199 (2020) 297–310.

[3] S. Choi, C.J. Kucharczyk, Y. Liang, X. Zhang, I. Takeuchi, H.-I. Ji, S.M. Haile, Exceptional power density and stability at intermediate temperatures in protonic ceramic fuel cells, Nat. Energy. 3 (2018) 202–210.

[4] R. Strandbakke, D.S. Wragg, M.H. Sørby, M.N. Guzik, A.E. Gunnæs, I. Szpunar, S.L. Wachowski, M. Balaguer, P.A. Carvalho, A. Mielewczyk-Gryń, J.M. Serra, T. Norby, Structural properties of mixed conductor Ba 1− x Gd 1− y La x + y Co 2 O 6− δ, Dalt. Trans. 51 (2022) 18667–18677

[5] M. Gazda, T. Miruszewski, D. Jaworski, A. Mielewczyk-Gryń, W. Skubida, S. Wachowski, P. Winiarz, K. Dzierzgowski, M. Łapiński, I. Szpunar, E. Dzik, Novel Class of Proton Conducting Materials - High Entropy Oxides, ACS Mater. Lett. 2 (2020)

Acknowledgements:

Project FunKeyCat is supported by the National Science Centre, Poland under the M-ERA.NET 2, which has received funding from the European Union’s Horizon 2020 research and innovation program under grant agreement no 685451.

Financial support of these studies from Gdańsk University of Technology by the DEC-3/1/2023/IDUB/III grant under the RADIUM- ‘Excellence Initiative - Research University’ program is gratefully acknowledged. Financial support of these studies from Gdańsk University of Technology by the DEC-1/1/2024/IDUB/III.4c/Tc grant under the Technetium - ‘Excellence Initiative - Research University’ program is gratefully acknowledged. This research was financially supported by the National Science Centre (NCN), Poland, within the project 2019/35/B/ST5/00888.

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