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A Quinoidal Two-Dimensional Metal-Organic Framework for High-Performance Micro-Supercapacitors and Solid-State

Ziman Chen1,2, Nana Li3, Yilong Yang4

  • 1State Key Laboratory of Organic-Inorganic Composites, National Energy R&D Center for Biorefinery, International Joint Bioenergy Laboratory of Ministry of Education, Beijing Key Laboratory of Green Chemicals Biomanufacturing, Beijing Synthetic Bio-Manufacturing Technology Innovation Center, College of Life Science and Technology, Beijing University of Chemical Technology, Beijing, China.

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Summary

We developed novel 2D metal-organic frameworks (MOFs) with redox-active quinoidal linkers for advanced microscale energy storage. These materials demonstrate high capacitance and improved solid-state battery performance.

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microsupercapacitorsquinoidal metal–organic frameworksredox‐active ligandssolid‐state lithium batteriestwo‐dimensional nanosheets

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Nanotechnology

Background:

  • Two-dimensional (2D) metal-organic frameworks (MOFs) are crucial for energy storage due to their tunable structures.
  • Integrating redox-active linkers in 2D MOFs enhances charge storage and ion transport.
  • Existing MOFs often face limitations in processability and energy density for practical applications.

Purpose of the Study:

  • To synthesize and characterize novel 2D MOFs using a quinoidal dicarboxylate ligand for microscale energy storage.
  • To investigate the electrochemical properties and performance of these MOFs in energy storage devices.
  • To demonstrate the potential of these MOFs as components in miniature and solid-state energy storage systems.

Main Methods:

  • Synthesis of a quinoidal dicarboxylate ligand (AQM-H2L) and its coordination with Cu2+ and Zn2+ ions.
  • Characterization of the resulting crystalline MOFs and exfoliated nanosheets using techniques like X-ray diffraction and electron microscopy.
  • Fabrication of energy storage devices, including supercapacitors integrated with graphene and solid-state batteries utilizing MOFs as electrolyte additives.

Main Results:

  • The copper-based MOF (AQM-AQM-H2L-Cu) showed layered structures with significant pseudocapacitance from Cu2+/Cu+ redox activity.
  • Exfoliated MOF nanosheets (approx. 5 nm) maintained crystallinity and processability.
  • Supercapacitors achieved high areal and volumetric capacitances (29.6 mF cm-2 and 18.1 F cm-3), with an energy density of 2.6 mWh cm-3.
  • In solid-state batteries, 1 wt% MOF nanosheets enhanced LiFePO4 cell performance, delivering 169.8 mAh g-1 at 0.2 C with 93% capacity retention over 400 cycles.

Conclusions:

  • Quinoidal linkers are effective in creating ionically active 2D frameworks for energy storage.
  • The developed MOFs offer a promising design for high-performance miniature and solid-state energy devices.
  • This research paves the way for next-generation energy storage solutions using advanced MOF materials.