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Ion-Selective Graphene Oxide/Polyvinyl Alcohol Composite Membranes for Rechargeable Alkaline Zinc Manganese Dioxide Batteries
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    Ion-Selective Graphene Oxide/Polyvinyl Alcohol Composite Membranes for Rechargeable Alkaline Zinc Manganese Dioxide Batteries
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    • Jinchao Huang*
      Jinchao Huang
      Department of Chemical Engineering, CUNY Energy Institute, The City College of New York, Steinman Hall, 160 Convent Avenue, New York, New York 10031, United States
      Urban Electric Power, 401 N Middletown Road, Bldg 155, Pearl River, New York 10965, United States
      *Email: jinchao@urbanelectricpower.com
      More by Jinchao Huang
      Orcidhttps://orcid.org/0000-0002-5009-8144
    • Gautam Yadav
      Gautam Yadav
      Department of Chemical Engineering, CUNY Energy Institute, The City College of New York, Steinman Hall, 160 Convent Avenue, New York, New York 10031, United States
      Urban Electric Power, 401 N Middletown Road, Bldg 155, Pearl River, New York 10965, United States
      More by Gautam Yadav
    • Damon E. Turney
      Damon E. Turney
      Department of Chemical Engineering, CUNY Energy Institute, The City College of New York, Steinman Hall, 160 Convent Avenue, New York, New York 10031, United States
      More by Damon E. Turney
    • Jungsang Cho
      Jungsang Cho
      Department of Chemical Engineering, CUNY Energy Institute, The City College of New York, Steinman Hall, 160 Convent Avenue, New York, New York 10031, United States
      More by Jungsang Cho
    • Michael Nyce
      Michael Nyce
      Department of Chemical Engineering, CUNY Energy Institute, The City College of New York, Steinman Hall, 160 Convent Avenue, New York, New York 10031, United States
      More by Michael Nyce
    • Bryan R. Wygant
      Bryan R. Wygant
      Department of Photovoltaics and Materials Technology, Sandia National Laboratories, Albuquerque, New Mexico 87185, United States
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    • Timothy N. Lambert
      Timothy N. Lambert
      Department of Photovoltaics and Materials Technology, Sandia National Laboratories, Albuquerque, New Mexico 87185, United States
      More by Timothy N. Lambert
      Orcidhttps://orcid.org/0000-0002-2359-2876
    • Sanjoy Banerjee
      Sanjoy Banerjee
      Department of Chemical Engineering, CUNY Energy Institute, The City College of New York, Steinman Hall, 160 Convent Avenue, New York, New York 10031, United States
      Urban Electric Power, 401 N Middletown Road, Bldg 155, Pearl River, New York 10965, United States
      More by Sanjoy Banerjee
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    ACS Applied Energy Materials

    Cite this: ACS Appl. Energy Mater. 2022, 5, 8, 9952–9961
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    https://doi.org/10.1021/acsaem.2c01605
    Published July 18, 2022
    Copyright © 2022 American Chemical Society
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    Abstract

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    Blocking the zincate ion ([Zn(OH)4]2–) and limiting its reaction with the cathode material are key requirements for improving the energy density and rechargeability of alkaline zinc manganese dioxide (Zn|MnO2) batteries. Zincate is the soluble anode discharge product, which undergoes a side reaction with the reduced cathode material to form a resistive and irreversible spinel material. Such a side reaction prevents deeper discharge of MnO2, reduces the battery’s achievable energy, and prevents it from further cycling. In this article, we report the design and fabrication of an ion-selective graphene oxide/poly(vinyl alcohol) composite membrane and demonstrate its superiority in suppressing zincate ion crossover while minimally impairing the conduction of hydroxyl ions (OH–). With this advanced separator, near full utilization of the MnO2 electrode’s two-electron capacity (∼617 mA h/g-MnO2) with a high areal capacity of 20 mA h/cm2 is reported for both primary and secondary cells. In the primary cell, the energy density is almost doubled, and in the rechargeable cell, a cycle life of 300 cycles is achieved, which is more than 3 times better than the case with no zincate blocking separator.

    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/acsaem.2c01605.

    • Illustrations of the experimental setup and detailed descriptions of experimental procedures; detailed calculation of zincate permeability; illustration of cell assembly; photographs of fabricated membranes; property summaries of the membranes tested; Nyquist plots of different membranes; voltage profiles of zincate-free cells with sintered Ni counter electrodes and Hg/HgO reference electrodes; capacity curve and voltage profiles of a type-II cell with c-PVA; direct voltage profile comparison of type II cells with cellophane and c-PVA(GO); photograph of a post-cycling type-II cathode; and post-cycling characterization of the c-PVA(GO) membranes including ionic conductivity change, EDS mapping, and XPS of the surface (PDF)

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    This article is cited by 10 publications.

    1. Nirajan Paudel, Birendra Ale Magar, Krishna Acharya, Timothy N. Lambert, Igor Vasiliev. Influence of Defects and Surfaces on the Electrochemical Performance of MnO2 Cathodes in Rechargeable Alkaline Zn/MnO2 Batteries: A First-Principles Study. ACS Applied Energy Materials 2024, 7 (7) , 2767-2778. https://doi.org/10.1021/acsaem.3c03200
      View
    2. Vinod Mathew, Noah B. Schorr, Balaji Sambandam, Timothy N. Lambert, Jaekook Kim. A Critical Comparison of Mildly Acidic versus Alkaline Zinc Batteries. Accounts of Materials Research 2023, 4 (4) , 299-306. https://doi.org/10.1021/accountsmr.2c00221
      View
    3. Nan Li, Jiaming Li, Jiaqi Li, Changfu Ma, Zhiqing Luo, Yini Long, Xiao Yu, Junyi Han, Shaoyu Zhang, Hedong Gu, Zhanhong Yang, Xiaowei Liu. Zeolite-coated separator suppresses manganese dissolution by selective ion trapping for long-cycling alkaline batteries. Chemical Engineering Science 2026, 319 , 122256. https://doi.org/10.1016/j.ces.2025.122256
      View
    4. Yimin LIN, Akari IWASAKI, Yuto MIYAHARA, Hirofumi TAKAMI, Yoshitatsu MISU, Kaori TAKANO, Tomomi NAGATSUKA, Koji MATSUOKA, Changhee LEE, Ryo SAKAMOTO, Shota TSUJIMOTO, Kohei MIYAZAKI, Takeshi ABE. Understanding Separator Properties Governing Zincate Crossover in Rechargeable Alkaline Zn–MnO2 Batteries. Electrochemistry 2026, https://doi.org/10.5796/electrochemistry.25-73172
      View
    5. Xing Wei, Tian-Nian Zhang, Yu-Hao Yao, Si-Yuan Xuan, Yi-Nan Wu, Han Xu, Ye-Xing Wang, Song-Lin Zhou, Zhenlei Zou, Shi-Chao Xing, Wenqiang Zhao, Yang-Yi Liu. Recent Progress on Constructing Artificial Interfacial Layers for Zinc-Anodes-Stabilizing. Electrochemical Energy Reviews 2025, 8 (1) https://doi.org/10.1007/s41918-025-00271-y
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    6. Gautam G. Yadav, Malesa Sammy, Jungsang Cho, Megan N. Booth, Michael Nyce, Jinchao Huang, Timothy N. Lambert, Damon E. Turney, Xia Wei, Sanjoy Banerjee. Performance of Low-Cost Energy Dense Mixed Material MnO2-Cu2O Cathodes for Commercially Scalable Aqueous Zinc Batteries. Batteries 2025, 11 (8) , 291. https://doi.org/10.3390/batteries11080291
      View
    7. T. Rodrigues-Marinho, D. Miranda, J. C. Barbosa, R. Gonçalves, S. Lanceros-Méndez, C. M. Costa. Separator membranes for aqueous zinc–manganese oxide batteries: a comprehensive review on experimental results and theoretical simulations. Sustainable Energy & Fuels 2025, 9 (6) , 1432-1446. https://doi.org/10.1039/D4SE01817F
      View
    8. Yong Wen Chek, Pui Kee Lee, Jia nan Yu, Bin Wang, Desmond Teck-Chye Ang. Review—Separators for Rechargeable Alkaline Zinc Batteries: Challenges and Progress. Journal of The Electrochemical Society 2025, 172 (2) , 020509. https://doi.org/10.1149/1945-7111/adada8
      View
    9. Feifan Zhang, Gege Wang, Jing Wu, Xiaowei Chi, Yu Liu. An Organic Coordination Manganese Complex as Cathode for High‐Voltage Aqueous Zinc‐metal Battery. Angewandte Chemie 2023, 135 (45) https://doi.org/10.1002/ange.202309430
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    10. Feifan Zhang, Gege Wang, Jing Wu, Xiaowei Chi, Yu Liu. An Organic Coordination Manganese Complex as Cathode for High‐Voltage Aqueous Zinc‐metal Battery. Angewandte Chemie International Edition 2023, 62 (45) https://doi.org/10.1002/anie.202309430
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    ACS Applied Energy Materials

    Cite this: ACS Appl. Energy Mater. 2022, 5, 8, 9952–9961
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsaem.2c01605
    Published July 18, 2022
    Copyright © 2022 American Chemical Society
    Request reuse permissions

    Article Views

    1228

    Altmetric

    2

    Citations

    10
    Learn about these metrics

    Article Views are the COUNTER-compliant sum of full text article downloads since November 2008 (both PDF and HTML) across all institutions and individuals. These metrics are regularly updated to reflect usage leading up to the last few days.

    Citations are the number of other articles citing this article, calculated by Crossref and updated daily. Find more information about Crossref citation counts.

    The Altmetric Attention Score is a quantitative measure of the attention that a research article has received online. Clicking on the donut icon will load a page at altmetric.com with additional details about the score and the social media presence for the given article. Find more information on the Altmetric Attention Score and how the score is calculated.

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