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Highly Proton-Conductive Solid-State Electrolyte Based on Covalent Organic Framework for Proton Battery Application.

Bing Tang1,2, Sheng-Ting Liu3, Xin-Rui Ma3

  • 1International Chinese-Belorussian Scientific Laboratory on Vacuum-Plasma Technology, Nanjing University of Science and Technology, Nanjing 210094, P. R. China.

ACS Applied Materials & Interfaces
|July 11, 2025
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Summary

Researchers developed a new solid-state proton battery electrolyte using a covalent organic framework (COF) composite. This advanced material, H₃PO₄@COF-SO₃H, shows high proton conductivity and stability for efficient energy storage.

Keywords:
covalent organic frameworkshigh specific capacityprotonic electrolytesolid-state proton batterysuperior proton conduction

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Energy Storage

Background:

  • Solid-state proton batteries offer a safer alternative for energy storage compared to liquid-electrolyte systems.
  • Development of efficient solid-state protonic electrolytes is crucial for advancing this technology.
  • Current electrolytes face challenges in achieving high conductivity and long-term stability.

Purpose of the Study:

  • To prepare and evaluate a novel covalent organic framework (COF)-based composite as a solid-state protonic electrolyte.
  • To investigate the proton conductivity, stability, and electrochemical performance of the new electrolyte.
  • To demonstrate the potential of COF-based electrolytes in solid-state proton batteries.

Main Methods:

  • A sulfonated COF (COF-SO₃H) was synthesized.
  • Phosphoric acid (H₃PO₄) was incorporated into the COF channels via a mechanochemical method to form the H₃PO₄@COF-SO₃H composite electrolyte.
  • The composite material was characterized using powder X-ray diffraction, NMR spectroscopy, XPS, and gas adsorption.
  • Electrochemical performance was assessed using impedance spectroscopy and by assembling a solid-state proton battery.

Main Results:

  • The H₃PO₄@COF-SO₃H composite exhibited superprotonic conductivity >10⁻² S cm⁻¹ under ambient conditions.
  • The electrolyte demonstrated excellent long-term stability and a wide electrochemical stability window.
  • The assembled solid-state proton battery showed a high specific capacity (101.8 mAh g⁻¹ at 1.0 A g⁻¹), excellent rate capability, and good cycling stability (80.6% retention after 1000 cycles).

Conclusions:

  • COF-based composite solid-state electrolytes, specifically H₃PO₄@COF-SO₃H, offer a promising pathway for high-performance solid-state proton batteries.
  • The developed electrolyte surpasses the performance of previously reported solid-state proton batteries.
  • This work highlights the potential of tailored COF structures for advanced energy storage applications.