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Chemical Stability and Degradation Mechanism of Solid Electrolytes/Aqueous Media at a Steady State for Long-Lasting Sodium Batteries

  • Tae-Ung Wi
    Tae-Ung Wi
    Department of Energy Engineering, School of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea
    More by Tae-Ung Wi
  • Chanhee Lee
    Chanhee Lee
    Department of Energy Engineering, School of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea
    More by Chanhee Lee
  • M. Fahmi Rahman
    M. Fahmi Rahman
    Department of Energy Engineering, School of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea
  • Wooseok Go
    Wooseok Go
    Department of Energy Engineering, School of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea
    More by Wooseok Go
  • Su Hwan Kim
    Su Hwan Kim
    Department of Energy Engineering, School of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea
    More by Su Hwan Kim
  • Dae Yeon Hwang
    Dae Yeon Hwang
    Department of Energy Engineering, School of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea
  • Sang Kyu Kwak*
    Sang Kyu Kwak
    Department of Energy Engineering, School of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea
    *Email: [email protected]
  • Youngsik Kim*
    Youngsik Kim
    Department of Energy Engineering, School of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea
    *Email: [email protected]
    More by Youngsik Kim
  • , and 
  • Hyun-Wook Lee*
    Hyun-Wook Lee
    Department of Energy Engineering, School of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea
    *Email: [email protected]
Cite this: Chem. Mater. 2021, 33, 1, 126–135
Publication Date (Web):December 29, 2020
https://doi.org/10.1021/acs.chemmater.0c03022
Copyright © 2020 American Chemical Society

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    Abstract

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    Research on the interface between solid electrolytes and electrode materials or catholyte is important to effectively and safely use their high energy densities. However, compared to interfaces with electrode materials, the interface between solid electrolytes and liquid media lacks research. Herein, the stability of NA superionic conductor (NASICON) pellets is studied in various aqueous solutions, including deionized (DI) water and a marine environment, associated with different degradation mechanisms. A representative detrimental hydronium exchange reaction between solid electrolytes and aqueous media is suppressed with increasing concentration and ion types dissolved in the solutions. Results of density functional theory calculation and electron energy loss spectroscopy reveal the different activation energies and chemical bonding states of solid electrolytes based on the aqueous solutions’ conditions. NASICON’s ionic conductivity decreases to ∼10–6 S/cm because of severe changes in aqueous solutions with insufficient dissolved ions resulting in inferior chemical stability. Furthermore, chemical stability variations at a steady state can severely affect battery performance. Seawater batteries fabricated with NASICON in immersed DI water for 1 year exhibit a large resistance region from the first cycle; this system breaks down before 200 h, unlike a cell fabricated using NASICON immersed for 1 year in a marine environment.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.chemmater.0c03022.

    • Structure of seawater battery coin cell; SEM and TEM images of NASICON pellet including EDS results; additional ICP data about minor phase dissolution; XRD results of NASICON in diverse aqueous media; detailed experimental procedure of EIS test for NASICON pellet and EIS results of polished NASICON pellet; and results of 1H MAS NMR of immersed NASICONs and related DFT calculations (PDF)

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    Cited By

    This article is cited by 14 publications.

    1. Emily E. Morgan, Hayden A. Evans, Kartik Pilar, Craig M. Brown, Raphaële J. Clément, Ryo Maezono, Ram Seshadri, Bartomeu Monserrat, Anthony K. Cheetham. Lattice Dynamics in the NASICON NaZr2(PO4)3 Solid Electrolyte from Temperature-Dependent Neutron Diffraction, NMR, and Ab Initio Computational Studies. Chemistry of Materials 2022, 34 (9) , 4029-4038. https://doi.org/10.1021/acs.chemmater.2c00212
    2. Wooseok Go, Jongwoo Kim, Jinho Pyo, Jeffrey B. Wolfenstine, Youngsik Kim. Investigation on the Structure and Properties of Na3.1Zr1.55Si2.3P0.7O11 as a Solid Electrolyte and Its Application in a Seawater Battery. ACS Applied Materials & Interfaces 2021, 13 (44) , 52727-52735. https://doi.org/10.1021/acsami.1c17338
    3. Chanhee Lee, Ji Young Kim, Ki Yoon Bae, Taewon Kim, Soon-Jae Jung, Samick Son, Hyun-Wook Lee. Enhancing electrochemomechanics: How stack pressure regulation affects all-solid-state batteries. Energy Storage Materials 2024, 66 , 103196. https://doi.org/10.1016/j.ensm.2024.103196
    4. Vithiya Muralidharan, S. Jayasubramaniyan, Hyun-Wook Lee. Surpassing water-splitting potential in aqueous redox flow batteries: insights from kinetics and thermodynamics. EES Catalysis 2024, 7 https://doi.org/10.1039/D3EY00231D
    5. Namhyeok Kim, Chang-Min Kim, Sanghoon Park, Jiyoung Park, Kyung Hwa Cho, Youngsik Kim. Continuous desalination and high-density energy storage: Na metal hybrid redox flow desalination battery. Chemical Engineering Journal 2024, 479 , 147628. https://doi.org/10.1016/j.cej.2023.147628
    6. Namhyeok Kim, Seohae Kim, Seongwoo Jeong, Hyo Jin, Hyeonseok Lee, Youngsik Kim, Wang-Geun Lee, Jeong-Sun Park. Seawater to resource technologies with NASICON solid electrolyte: a review. Frontiers in Batteries and Electrochemistry 2023, 2 https://doi.org/10.3389/fbael.2023.1301806
    7. Taewon Kim, Sang Hyeok Ahn, You‐Yeob Song, Beom Jin Park, Chanhee Lee, Ahreum Choi, Min‐Ho Kim, Dong‐Hwa Seo, Sung‐Kyun Jung, Hyun‐Wook Lee. Prussian Blue‐Type Sodium‐ion Conducting Solid Electrolytes for All Solid‐State Batteries. Angewandte Chemie 2023, 135 (42) https://doi.org/10.1002/ange.202309852
    8. Taewon Kim, Sang Hyeok Ahn, You‐Yeob Song, Beom Jin Park, Chanhee Lee, Ahreum Choi, Min‐Ho Kim, Dong‐Hwa Seo, Sung‐Kyun Jung, Hyun‐Wook Lee. Prussian Blue‐Type Sodium‐ion Conducting Solid Electrolytes for All Solid‐State Batteries. Angewandte Chemie International Edition 2023, 62 (42) https://doi.org/10.1002/anie.202309852
    9. A.J. Pelczarska, D. Stefańska, A. Kabański, M. Ptak, R. Lisiecki, I. Szczygieł, J. Hanuza. Structural and optical properties of a new structural modification of Na3+3xYb2−x(PO4)3:1% Eu phosphate, where x = 0,1-0,5 and prospective thermometric applications of the compound. Journal of Alloys and Compounds 2023, 944 , 169228. https://doi.org/10.1016/j.jallcom.2023.169228
    10. S. Jayasubramaniyan, Chanhee Lee, Hyun-Wook Lee. Progress and perspectives of space charge limited current models in all-solid-state batteries. Journal of Materials Research 2022, 37 (23) , 4017-4034. https://doi.org/10.1557/s43578-022-00806-9
    11. Stefanie Arnold, Lei Wang, Volker Presser. Dual‐Use of Seawater Batteries for Energy Storage and Water Desalination. Small 2022, 18 (43) https://doi.org/10.1002/smll.202107913
    12. Myung-Jin Baek, Jieun Choi, Tae-Ung Wi, Hyeong Yong Lim, Min Hoon Myung, Chanoong Lim, Jinsu Sung, Jeong-Sun Park, Ju Hyun Park, Yul Hui Shim, Jaehyun Park, Seok Ju Kang, Youngsik Kim, So Youn Kim, Sang Kyu Kwak, Hyun-Wook Lee, Dong Woog Lee. Strong interfacial energetics between catalysts and current collectors in aqueous sodium–air batteries. Journal of Materials Chemistry A 2022, 10 (9) , 4601-4610. https://doi.org/10.1039/D2TA00329E
    13. Youngsik Kim, Wang-geun Lee. Secondary Seawater Batteries. 2022, 91-293. https://doi.org/10.1007/978-981-19-0797-5_3
    14. Jeonghoon Cho, Myeong Woo Kim, Youngjin Kim, Jeong-Sun Park, Do-Hee Lee, Youngsik Kim, Jae Joon Kim. Seawater Battery-Based Wireless Marine Buoy System With Battery Degradation Prediction and Multiple Power Optimization Capabilities. IEEE Access 2021, 9 , 104104-104114. https://doi.org/10.1109/ACCESS.2021.3098846

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