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Synergistic Dual-Polar-Functionalized Metal-Organic Framework-Modified Separator for Stable and High-Performance

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A novel multifunctional separator, UFS2@GF, enhances sodium metal batteries (SMBs) by promoting uniform sodium deposition and improving ion transport. This leads to significantly improved cycling stability and performance in high-energy-density devices.

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Energy Storage

Background:

  • Sodium metal anodes are ideal for high-energy-density rechargeable sodium metal batteries (SMBs).
  • Key challenges include sluggish sodium ion (Na+) transport kinetics and uncontrolled dendritic growth, limiting cycling stability.
  • Existing separators often fail to adequately address these limitations for practical applications.

Purpose of the Study:

  • To develop a multifunctional separator (UFS2@GF) to overcome the limitations of sodium metal anodes in SMBs.
  • To enhance Na+ deposition kinetics and uniformity.
  • To improve overall cycling stability and performance of SMBs.

Main Methods:

  • Fabrication of a UFS2@GF separator using metal-organic frameworks functionalized with fluorinated (-F) and sulfonic acid (-SO3H) groups.
  • Structural characterization and density functional theory (DFT) calculations.
  • Electrochemical testing of symmetric cells and full cells (Na∥Na3V2(PO4)3).

Main Results:

  • The UFS2@GF separator provides abundant nucleation sites, reducing overpotential and enabling uniform Na+ deposition.
  • It induces an inorganic-rich solid electrolyte interphase, facilitating uniform Na+ flux and enhancing charge transfer.
  • Synergistic effects of -F and -SO3H groups significantly accelerate Na+ transport kinetics, evidenced by higher transference number and ionic conductivity.
  • Stable cycling over 2500 h at 0.25 mA cm-2 in symmetric cells and excellent specific capacity in full cells.

Conclusions:

  • The UFS2@GF separator effectively addresses Na+ transport kinetics and dendritic growth issues in SMBs.
  • Synergistic functional group strategies are crucial for developing advanced separators for high-performance SMBs.
  • This work demonstrates a promising approach for realizing stable and high-energy-density sodium metal batteries.