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High-Performance Quasi-Solid-State Calcium-Ion Batteries from Redox-Active Covalent Organic Framework Electrolytes.

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Redox covalent organic frameworks (COFs) function as quasi-solid-state electrolytes, enhancing calcium ion battery performance. PT-COFs demonstrate improved ionic conductivity and stable cycling, paving the way for advanced energy storage solutions.

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Energy Storage

Background:

  • Calcium ion batteries (CIBs) offer high volumetric capacity and earth abundance, but face challenges from sluggish ion transport and anode passivation.
  • Developing stable and efficient electrolytes is crucial for high-performance CIBs.

Purpose of the Study:

  • To synthesize redox covalent organic frameworks (COFs) as quasi-solid-state electrolytes (QSSEs) for CIBs.
  • To address challenges of ion transport and cycling stability in CIBs.

Main Methods:

  • Preparation of two types of redox COFs (PT-COFs and PQ-COFs) with varying carbonyl group densities.
  • Characterization of ionic conductivity, Ca2+ transference number, and electrochemical performance in full calcium ion cells.

Main Results:

  • PT-COFs exhibited ionic conductivity of 0.46 mS cm-1 at room temperature and 5.05 mS cm-1 at 80 °C, with a Ca2+ transference number of 0.532.
  • The full calcium ion cell using PT-COFs achieved a reversible specific capacity of 155.9 mAh g-1 at 0.15 A g-1 and maintained over 74.6% capacity after 1000 cycles at 1 A g-1.

Conclusions:

  • Redox COFs, particularly PT-COFs, are effective QSSEs for high-performance CIBs.
  • This study highlights the potential of redox COFs in advancing solid-state electrolyte technology for next-generation energy storage.