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Two-Dimensional Imide-Based Covalent Organic Frameworks with Tailored Pore Functionality as Separators for

Jiangwei Shi1, Mengfei Su1, Hang Li1

  • 1State Key Laboratory of Coordination Chemistry, Coordination Chemistry Institute, Collaborative Innovation Center of Advanced Microstructures, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, P. R. China.

ACS Applied Materials & Interfaces
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PubMed
Summary

Researchers developed a novel separator for lithium-sulfur batteries (LSBs) using functionalized covalent organic frameworks (COFs) on reduced graphene oxide (rGO). This design effectively suppresses polysulfide shuttling, enhancing battery performance and cycle life.

Keywords:
Li−sulfur batterycovalent organic frameworkmorphology controlseparatorsurface tailoring

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Nanotechnology

Background:

  • The polysulfide shuttle effect is a major limitation in lithium-sulfur batteries (LSBs).
  • Developing stable, lightweight, and effective separators is crucial for advancing LSB technology.
  • Covalent organic frameworks (COFs) offer tunable properties for energy storage applications.

Purpose of the Study:

  • To design and fabricate a functionalized separator for LSBs to mitigate the polysulfide shuttle effect.
  • To explore the use of imide-based COFs integrated with reduced graphene oxide (rGO) for enhanced separator performance.
  • To investigate the impact of specific functional groups within COFs on polysulfide adsorption and battery cycling.

Main Methods:

  • Fabrication of imide-based COF-TpPa on rGO films via an oxygen-free solvothermal technique.
  • Modification of COF-TpPa with functional groups (-SO3H and -Cl) to tailor pore characteristics.
  • Characterization of the modified rGO/COF films as separators in LSBs.

Main Results:

  • Successfully constructed 2D COF nanosheets with tailored functionalities on rGO films.
  • The functional groups and narrowed pores within the COF effectively adsorbed and confined Li2S, weakening the shuttle effect.
  • The COF-SO3H-modified separator demonstrated a high specific capacity (1163.4 mAh/g at 0.2 C) and excellent cyclic stability (60.2% retention after 1000 cycles at 2.0 C).

Conclusions:

  • The developed rGO/COF composite separator is a promising strategy for improving LSB performance.
  • Rational design of functional COFs offers a feasible approach for advanced energy storage systems.
  • This work highlights the potential of COF-modified separators in boosting the efficiency and longevity of LSBs.