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Area of Science:

  • Materials Science
  • Chemistry
  • Physics

Background:

  • Metal-organic frameworks (MOFs) are widely used as electronic or ionic conductors.
  • Mixed electron-ion conductivity in MOFs is an underexplored area with significant potential.

Purpose of the Study:

  • To develop a new methodology for designing mixed ionic-electronic conductors (MIECs) based on conductive MOFs (cMOFs).
  • To orthogonally tune electronic and ionic transport properties through side chain engineering.

Main Methods:

  • Synthesized a series of MOFs (M-R) by tethering ethylene glycol (EG) functional groups onto a cMOF core.
  • Systematically varied side chain functionalities (nBu, 1EG, 2EG) to modify the pore microenvironment.
  • Incorporated LiTFSI salt to evaluate ionic conductivity and measured electronic conductivity.

Main Results:

  • Ni-1EG exhibited the highest room-temperature ionic conductivity (1.1 × 10⁻⁴ S/cm), significantly higher than the hydrophobic Ni-nBu.
  • Electronic conductivity was preserved in Ni-1EG (∼5 × 10⁻⁴ S/cm).
  • Ni-2EG showed reduced ionic conductivity (2.58 × 10⁻⁶ S/cm) likely due to pore blockage, despite increased polarity.

Conclusions:

  • Side chain engineering provides a powerful strategy for decoupled control of ionic and electronic transport in cMOFs.
  • This work unlocks the potential of cMOFs as tunable platforms for single-phase porous crystalline MIECs.
  • The findings open new design possibilities for materials in chemistry, physics, and materials science.