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Surface Chemistry of La0.99Sr0.01NbO4-d and Its Implication for Proton Conduction

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    Research Article

    Surface Chemistry of La0.99Sr0.01NbO4-d and Its Implication for Proton Conduction
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    Department of Materials, Imperial College London, Prince Consort Road, London SW7 2BP, United Kingdom
    *E-mail: [email protected], tel.: +44 (0)20 7594 6782.
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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2017, 9, 35, 29633–29642
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    https://doi.org/10.1021/acsami.7b04856
    Published August 18, 2017
    Copyright © 2017 American Chemical Society
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    Abstract

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    Acceptor-doped LaNbO4 is a promising electrolyte material for proton-conducting fuel cell (PCFC) applications. As charge transfer processes govern device performance, the outermost surface of acceptor-doped LaNbO4 will play an important role in determining the overall cell performance. However, the surface composition is poorly characterized, and the understanding of its impact on the proton exchange process is rudimentary. In this work, the surface chemistry of 1 atom % Sr-doped LaNbO4 (La0.99Sr0.01NbO4-d, denoted as LSNO) proton conductor is characterized using LEIS and SIMS. The implication of a surface layer on proton transport is studied using the isotopic exchange technique. It has shown that a Sr-enriched but La-deficient surface layer of about 6–7 nm thick forms after annealing the sample under static air at 1000 °C for 10 h. The onset of segregation is found to be between 600 and 800 °C, and an equilibrium surface layer forms after 10 h annealing. A phase separation mechanism, due to the low solubility of Sr in LaNbO4, has been proposed to explain the observed segregation behavior. The surface layer was concluded to impede the water incorporation process, leading to a reduced isotopic fraction after the D216O wet exchange process, highlighting the impact of surface chemistry on the proton exchange process.

    Copyright © 2017 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acsami.7b04856.

    • Calibration curves for XRF analysis, details of the deuterium exchange and associated SIMS data, analysis of SIMS crater depths as both a figure and tabulated data, details of the LEIS data analysis procedure, SIMS depth profiles at 450 °C, conductivity data (PDF)

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    This article is cited by 7 publications.

    1. Alessandro Chiara, Francesco Giannici, Candida Pipitone, Alessandro Longo, Chiara Aliotta, Marianna Gambino, Antonino Martorana. Solid–Solid Interfaces in Protonic Ceramic Devices: A Critical Review. ACS Applied Materials & Interfaces 2020, 12 (50) , 55537-55553. https://doi.org/10.1021/acsami.0c13092
    2. S. Balasundari, S. Jayasubramaniyan, M. Vithiya, P. A. Rayjada, N. Satyanarayana, T. Rani, P. Muralidharan. Enhanced proton conductivity in low-temperature sintered pristine and Ca-doped LaNbO4 nanocrystals synthesized via microwave hydrothermal method. Journal of Materials Science: Materials in Electronics 2025, 36 (7) https://doi.org/10.1007/s10854-025-14512-9
    3. Nai Shi, Yun Xie, Moses Oludayo Tadé, Zongping Shao. Evolution and Reconstruction of Air‐Electrode Surface Composition in Reversible Protonic Ceramic Cells: Mechanisms, Impacts on Catalytic Performance, and Optimization Strategies – A Review. Advanced Materials 2025, 37 (11) https://doi.org/10.1002/adma.202416528
    4. Aleksandra Mielewczyk‐Gryń, Sebastian Wachowski, Kacper Dzierzgowski, Iga Szpunar, Judyta Strychalska‐Nowak, Tomasz Klimczuk, Mirosław Sawczak, Maria Gazda. Vibrational Properties of LaNb 0.8 M 0.2 O 4‐δ (M=As, Sb, V, and Ta). ChemPhysChem 2023, 24 (1) https://doi.org/10.1002/cphc.202200368
    5. Aleksandra Mielewczyk-Gryń, Sebastian Wachowski, Marta Prześniak-Welenc, Kacper Dzierzgowski, Anna Regoutz, David J. Payne, Maria Gazda. Water uptake analysis of acceptor-doped lanthanum orthoniobates. Journal of Thermal Analysis and Calorimetry 2019, 138 (1) , 225-232. https://doi.org/10.1007/s10973-019-08208-6
    6. Jiajia Cui, Junkai Wang, Xiongwen Zhang, Guojun Li, Kai Wu, Yonghong Cheng, Jun Zhou. Enhanced oxygen reduction reaction through Ca and Co Co-doped YFeO3 as cathode for protonic ceramic fuel cells. Journal of Power Sources 2019, 413 , 148-157. https://doi.org/10.1016/j.jpowsour.2018.12.030
    7. Natalia M. Porotnikova, Vadim A. Eremin, Andrey S. Farlenkov, Edhem Kh. Kurumchin, Elena A. Sherstobitova, Dmitry I. Kochubey, Maxim V. Ananyev. Effect of AO Segregation on Catalytical Activity of La0.7A0.3MnO3±δ (A = Ca, Sr, Ba) Regarding Oxygen Reduction Reaction. Catalysis Letters 2018, 148 (9) , 2839-2847. https://doi.org/10.1007/s10562-018-2456-7
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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2017, 9, 35, 29633–29642
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsami.7b04856
    Published August 18, 2017
    Copyright © 2017 American Chemical Society
    Request reuse permissions

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