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Area of Science:

  • Materials Science
  • Electrochemistry
  • Energy Storage

Background:

  • Metal-organic frameworks (MOFs) are promising for electrochemical energy storage but lack explored chemical principles for electroactivity.
  • Synthesizing anionic MOFs with lithium cation reservoirs and reversible redox capabilities remains a significant challenge.

Purpose of the Study:

  • To design and synthesize electrically conducting Li-ion MOF cathodes with tunable chemical and structural properties.
  • To investigate the relationship between MOF composition, secondary building unit (SBU) topology, and electrochemical performance.

Main Methods:

  • Rational control of ligand-to-transition metal stoichiometry and SBU topology in the CPO-27 archetypal MOF.
  • Synthesis of Li₂-M-DOBDC (M = Mg²⁺ or Mn²⁺) materials.
  • Electrochemical characterization including redox potential, conductivity measurements, and cycling stability tests.

Main Results:

  • Achieved electrically conducting Li-ion MOF cathodes (Li₂-M-DOBDC) with a million-fold increase in conductivity (up to 10⁻⁷ S/cm for Li₂-Mn-DOBDC).
  • Augmented the redox potential of the DOBDC⁴⁻ linker to 3.2 V vs Li⁺/Li⁰.
  • Demonstrated excellent capacity retention over 100 cycles and fast cycling rates for Li₂-Mn-DOBDC as a cathode material.

Conclusions:

  • Validated the concept of reversible redox activity and electronic conductivity in MOFs through precise composition and SBU design.
  • Li₂-M-DOBDC materials represent a significant advancement in MOF-based electrochemical energy storage.
  • The developed MOFs offer practical advantages for Li-ion battery assembly and performance.