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Cationic Covalent Organic Framework-Based Membranes for High-Performance Zn/Br2 Redox Flow Batteries.

Dabin Han1, Lamia Abuawwad2, Minji Kim1

  • 1Department of Energy Science & Engineering, Daegu Gyeongbuk Institute of Science & Technology (DGIST), Daegu, 42988, Republic of Korea.

Small (Weinheim an Der Bergstrasse, Germany)
|December 22, 2025
PubMed
Summary

A novel composite membrane using ethidium bromide-based COF in Nafion enhances zinc-bromine flow battery performance. This design boosts ion conductivity and suppresses polybromide shuttle, achieving 89.1% energy efficiency.

Keywords:
Bi‐ionic mobilitycovalent organic frameworkspolybromide shuttleredox flow batteriesseparator membrane

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Energy Storage

Background:

  • Zinc-bromine redox flow batteries (Zn/Br$_{2}$ RFBs) are promising for large-scale energy storage due to safety and efficiency.
  • Membrane design is crucial for Zn/Br$_{2}$ RFBs, balancing ion transport (Zn$^{2+}$, Br$^{-}$) with suppressing undesirable side reactions like polybromide (Br$_{n}$$^{-}$) shuttling.
  • Existing membranes face a trade-off between high ionic conductivity and effective blocking of Br$_{n}$$^{-}$ migration, limiting battery performance.

Purpose of the Study:

  • To develop a novel composite membrane for Zn/Br$_{2}$ RFBs that overcomes the ionic conductivity vs. Br$_{n}$$^{-}$ shuttle trade-off.
  • To enhance anion conduction while simultaneously suppressing Br$_{n}$$^{-}$ migration through strategic material incorporation.
  • To evaluate the performance of the new membrane in Zn/Br$_{2}$ RFBs.

Main Methods:

  • Incorporation of a cationic covalent organic framework (COF) derived from ethidium bromide and triformylphloroglucinol (EB-COF) into a Nafion (NF) matrix.
  • Characterization of the composite membrane's structure, water network formation, and functional groups (-CHO, -NH$_{2}$, N$^{+}$).
  • Assembly and testing of Zn/Br$_{2}$ RFBs using the NF/EB-COF composite membrane, specifically NF/EB-COF(0.3).

Main Results:

  • The EB-COF within the Nafion matrix facilitated abundant water networks, significantly enhancing ion conductivity.
  • The quaternary amine groups (N$^{+}$) in EB-COF effectively absorbed Br$_{2}$ and mitigated the Br$_{n}$$^{-}$ shuttle effect.
  • The NF/EB-COF(0.3) composite membrane demonstrated superior performance, enabling Zn/Br$_{2}$ RFBs to achieve 89.1% energy efficiency at 40 mA cm$^{-2}$.

Conclusions:

  • The proposed membrane design strategy effectively addresses the critical trade-off in Zn/Br$_{2}$ RFB membranes.
  • The NF/EB-COF composite membrane offers enhanced ion transport and suppressed polybromide crossover, leading to improved battery performance.
  • This work presents a viable pathway for developing advanced membranes for efficient and safe large-scale energy storage systems.