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An Unprecedented Vapor-Phase Sintering Activator for Highly Refractory Proton-Conducting Oxides

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    An Unprecedented Vapor-Phase Sintering Activator for Highly Refractory Proton-Conducting Oxides
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    • Hyegsoon An
      Hyegsoon An
      Center for Energy Materials Research, Korea Institute of Science and Technology (KIST), Seoul02792, Republic of Korea
      More by Hyegsoon An
    • Seunghyeok Im
      Seunghyeok Im
      Center for Energy Materials Research, Korea Institute of Science and Technology (KIST), Seoul02792, Republic of Korea
      Nanoscience and Technology, KIST School, Korea University of Science and Technology (UST)Seoul02792, Republic of Korea
      More by Seunghyeok Im
    • Junseok Kim
      Junseok Kim
      Center for Energy Materials Research, Korea Institute of Science and Technology (KIST), Seoul02792, Republic of Korea
      Department of Materials Science and Engineering, Korea University, Seoul02841, Republic of Korea
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    • Byung-Kook Kim
      Byung-Kook Kim
      Center for Energy Materials Research, Korea Institute of Science and Technology (KIST), Seoul02792, Republic of Korea
      More by Byung-Kook Kim
    • Ji-Won Son
      Ji-Won Son
      Center for Energy Materials Research, Korea Institute of Science and Technology (KIST), Seoul02792, Republic of Korea
      Graduate School of Energy and Environment (KU-KIST Green School), Korea University, Seoul02841, Republic of Korea
      More by Ji-Won Son
      Orcidhttps://orcid.org/0000-0002-5310-0633
    • Kyung Joong Yoon
      Kyung Joong Yoon
      Center for Energy Materials Research, Korea Institute of Science and Technology (KIST), Seoul02792, Republic of Korea
      Yonsei-KIST Convergence Research Institute, Yonsei University, Seoul03722, Republic of Korea
      More by Kyung Joong Yoon
      Orcidhttps://orcid.org/0000-0002-4161-5111
    • Hyoungchul Kim
      Hyoungchul Kim
      Center for Energy Materials Research, Korea Institute of Science and Technology (KIST), Seoul02792, Republic of Korea
      More by Hyoungchul Kim
      Orcidhttps://orcid.org/0000-0003-3109-660X
    • Sungeun Yang
      Sungeun Yang
      Center for Energy Materials Research, Korea Institute of Science and Technology (KIST), Seoul02792, Republic of Korea
      Nanoscience and Technology, KIST School, Korea University of Science and Technology (UST)Seoul02792, Republic of Korea
      More by Sungeun Yang
      Orcidhttps://orcid.org/0000-0001-9202-930X
    • Hyungmook Kang*
      Hyungmook Kang
      Center for Energy Materials Research, Korea Institute of Science and Technology (KIST), Seoul02792, Republic of Korea
      *[email protected]
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    • Jong-Ho Lee*
      Jong-Ho Lee
      Center for Energy Materials Research, Korea Institute of Science and Technology (KIST), Seoul02792, Republic of Korea
      Nanoscience and Technology, KIST School, Korea University of Science and Technology (UST)Seoul02792, Republic of Korea
      *[email protected]
      More by Jong-Ho Lee
      Orcidhttps://orcid.org/0000-0003-4481-6258
    • Ho-Il Ji*
      Ho-Il Ji
      Center for Energy Materials Research, Korea Institute of Science and Technology (KIST), Seoul02792, Republic of Korea
      Nanoscience and Technology, KIST School, Korea University of Science and Technology (UST)Seoul02792, Republic of Korea
      *[email protected]
      More by Ho-Il Ji
      Orcidhttps://orcid.org/0000-0002-6194-991X
    Other Access OptionsSupporting Information (3)

    ACS Energy Letters

    Cite this: ACS Energy Lett. 2022, 7, 11, 4036–4044
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    https://doi.org/10.1021/acsenergylett.2c02059
    Published October 21, 2022
    Copyright © 2022 American Chemical Society
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    Abstract

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    Proton-conducting oxides provide opportunities to boost the electrochemical characteristics of various energy conversion devices owing to their high ionic conductivity. While these oxides alone require high-temperature sintering above 1600 °C to gain full density, surprisingly, their thin membrane on Ni-based electrodes can be readily densified even below 1400 °C. However, the underlying mechanism is still unclear despite their widespread use, thereby hindering reliable fabrication of electrochemical devices. Here we reveal the mechanism by which an unprecedented type of sintering activator, vapor-phase BaNiOx, released from the transient phase in the electrode, is responsible for the accelerated sintering of refractory proton-conducting oxides. In contrast to conventional solid-phase sintering additives, the vapor-phase sintering activator is naturally supplied with an optimally small amount, which minimizes the residue but achieves sufficient enhancement of the sinterability, leading to negligible degradation of the electrical properties of the membrane. These findings establish a platform for fabrication of protonic ceramic electrochemical devices.

    Copyright © 2022 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsenergylett.2c02059.

    • Compositional analysis, dilatometery results, SEM images, XRD results, TG profile, APT 3D reconstruction images, conductivity results, and snapshots of MD simulation, including Tables S1–S4 and Figures S1–S12 (PDF)

    • Movie 1: barium oxide evaporation observed in MD simulation (MP4)

    • Movie 2: barium nickel oxide evaporation observed in MD simulation (MP4)

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    Electronic Supporting Information files are available without a subscription to ACS Web Editions. The American Chemical Society holds a copyright ownership interest in any copyrightable Supporting Information. Files available from the ACS website may be downloaded for personal use only. Users are not otherwise permitted to reproduce, republish, redistribute, or sell any Supporting Information from the ACS website, either in whole or in part, in either machine-readable form or any other form without permission from the American Chemical Society. For permission to reproduce, republish and redistribute this material, requesters must process their own requests via the RightsLink permission system. Information about how to use the RightsLink permission system can be found at http://pubs.acs.org/page/copyright/permissions.html.

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    This article is cited by 15 publications.

    1. Junseok Kim, Subrina Islam, Yue Bao, Hanping Ding, Chuancheng Duan. Two-Step Sintering for Dual Enhancement of Electrolyte and Hydrogen Electrode in Protonic Ceramic Electrochemical Cells. ACS Applied Materials & Interfaces 2025, 17 (23) , 34277-34283. https://doi.org/10.1021/acsami.5c06739
    2. Kyung Joong Yoon, Sanghoon Lee, Sun-Young Park, Nguyen Q. Minh. Advances in high-temperature solid oxide electrolysis technology for clean hydrogen and chemical production: materials, cells, stacks, systems and economics. Progress in Materials Science 2025, 154 , 101520. https://doi.org/10.1016/j.pmatsci.2025.101520
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    4. Charlie Meisel, Jake D. Huang, You‐Dong Kim, Sophia Stockburger, Ryan O'Hayre, Neal P. Sullivan. Insights on proton‐conducting ceramic electrochemical cell fabrication. Journal of the American Ceramic Society 2025, 108 (4) https://doi.org/10.1111/jace.20321
    5. Meng Li, Fan Liu, Dong Ding. Critical insights into the steam electrolysis electrode in protonic ceramic cells for hydrogen production. Nature Catalysis 2025, 8 (4) , 293-300. https://doi.org/10.1038/s41929-025-01313-w
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    7. You-Dong Kim, Charlie Meisel, In-Ho Kim, Carolina Herradón, Peter Rand, Jayoon Yang, Neal P. Sullivan, Ryan O'Hayre. Tuning barium release from sacrificial powders to optimize sintering and enhance the performance of reversible large-scale tubular protonic ceramic electrochemical cells. Journal of Power Sources 2025, 625 , 235700. https://doi.org/10.1016/j.jpowsour.2024.235700
    8. Charlie Meisel, Jake Huang, You-Dong Kim, Ryan O’Hayre, Neal P. Sullivan. Towards improved stability in proton-conducting ceramic fuel cells. Journal of Power Sources 2024, 615 , 235021. https://doi.org/10.1016/j.jpowsour.2024.235021
    9. Junseok Kim, Jiwon Yun, Wanjae Lee, Do‐Hyeong Kim, Puspendu Guha, Jin‐Ha Hwang, Deok‐Hwang Kwon, Sungeun Yang, Jong‐Ho Lee, Kyung Joong Yoon, Ji‐Won Son, Sahn Nahm, Sihyuk Choi, Ho‐Il Ji. Dual‐Phase Reaction Sintering for Overcoming the Inherent Sintering Ability of Refractory Electrolytes in Protonic Ceramic Cells. Advanced Energy Materials 2024, 14 (26) https://doi.org/10.1002/aenm.202400787
    10. Amina Lahrichi, Youness El Issmaeli, Shankara S. Kalanur, Bruno G. Pollet. Advancements, strategies, and prospects of solid oxide electrolysis cells (SOECs): Towards enhanced performance and large-scale sustainable hydrogen production. Journal of Energy Chemistry 2024, 94 , 688-715. https://doi.org/10.1016/j.jechem.2024.03.020
    11. Jianqiu Zhu, Yuxuan Zhang, Ze Liu, Jingzeng Cui, Ziting Xia, Jingyuan Ma, Jing Zhou, Zhiwei Hu, Jian-Qiang Wang, Xiangyong Zhao, Linjuan Zhang. Micro-beam XAFS reveals in-situ 3D exsolution of transition metal nanoparticles in accelerating hydrogen separation. The Innovation Materials 2024, 2 (<![CDATA[1]]>) , 100054. https://doi.org/10.59717/j.xinn-mater.2024.100054
    12. Donguk Kim, Tae Kyeong Lee, Seungwoo Han, Yuhan Jung, Dong Gyu Lee, Mingi Choi, Wonyoung Lee. Advances and challenges in developing protonic ceramic cells. Materials Today Energy 2023, 36 , 101365. https://doi.org/10.1016/j.mtener.2023.101365
    13. Jianqiu Zhu, Jingzeng Cui, Yuxuan Zhang, Ze Liu, Chuan Zhou, Susu Bi, Jingyuan Ma, Jing Zhou, Zhiwei Hu, Tao Liu, Zhi Li, Xiangyong Zhao, Jian-Qiang Wang, Linjuan Zhang. Enhanced H2 permeation and CO2 tolerance of self-assembled ceramic-metal-ceramic BZCYYb-Ni-CeO2 hybrid membrane for hydrogen separation. Journal of Energy Chemistry 2023, 82 , 47-55. https://doi.org/10.1016/j.jechem.2023.03.027
    14. Muhammad Bilal Hanif, Sajid Rauf, Zain ul Abadeen, Kashif Khan, Zuhra Tayyab, Sana Qayyum, Michał Mosiałek, Zongping Shao, Cheng-Xin Li, Martin Motola. Proton-conducting solid oxide electrolysis cells: Relationship of composition-structure-property, their challenges, and prospects. Matter 2023, 6 (6) , 1782-1830. https://doi.org/10.1016/j.matt.2023.04.013
    15. Donguk Kim, Tae Kyeong Lee, Seungwoo Han, Mingi Choi, Wonyoung Lee. Advances in developing protonic ceramic cells. Ceramist 2023, 26 (1) , 47-63. https://doi.org/10.31613/ceramist.2023.26.1.04
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    ACS Energy Letters

    Cite this: ACS Energy Lett. 2022, 7, 11, 4036–4044
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsenergylett.2c02059
    Published October 21, 2022
    Copyright © 2022 American Chemical Society
    Request reuse permissions

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