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Pillared-Layer Metal-Organic Frameworks for Improved Lithium-Ion Storage Performance.

Teng Gong1, Xiaobing Lou2, En-Qing Gao1

  • 1Shanghai Key Laboratory of Green Chemistry and Chemical Processes, College of Chemistry and Molecular Engineering, East China Normal University , Shanghai 200062, China.

ACS Applied Materials & Interfaces
|June 15, 2017
PubMed
Summary

A new pillared-layer strategy enhances metal-organic frameworks (MOFs) for lithium-ion batteries. This design offers high capacity and stable cycling by retaining structure during operation.

Keywords:
MOFsanodic materialslithium-ion batterypillared layerstructure−property

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Nanotechnology

Background:

  • Metal-organic frameworks (MOFs) are increasingly explored as advanced anodic materials for lithium-ion batteries.
  • Optimizing MOF structure for superior lithium storage performance remains a significant challenge due to limited structure-property relationship understanding.

Purpose of the Study:

  • To introduce and validate a "pillared-layer" design strategy for enhancing MOF performance in lithium-ion battery anodes.
  • To investigate the structural and electrochemical properties of four novel Mn(II) and Co(II) MOFs with mixed azide and carboxylate ligands.

Main Methods:

  • Synthesis and characterization of four 3D metal-organic frameworks (MOFs) with pillared-layer and chain architectures.
  • Electrochemical testing of MOFs as anodes in lithium-ion batteries, including initial lithiation capacity, rate capability, and cycling stability.
  • Post-cycling structural analysis (XRD) and electrochemical impedance spectroscopy (EIS) to understand performance variations.

Main Results:

  • All studied MOFs exhibited high initial lithiation capacities (1170-1400 mA h g⁻¹), attributed to abundant insertion sites from azide ions and aromatic ligands.
  • Pillared-layer MOFs (1, 3, 4) demonstrated excellent reversible capacities (580-595 mA h g⁻¹) and stable cycling, unlike the chain-based MOF (2) which showed rapid capacity decay.
  • Amorphization occurred in all MOFs after the first cycle; however, the amorphous phases of pillared-layer MOFs maintained accessible structures for lithium-ion storage, unlike the chain-based MOF.

Conclusions:

  • The pillared-layer strategy is effective for designing MOFs with high-performance lithium-ion storage capabilities.
  • Structural integrity and accessible amorphous phases post-lithiation are crucial for sustained electrochemical performance in MOF anodes.
  • The observed performance is primarily due to ion insertion/diffusion rather than metal conversion, as indicated by spectroscopy and comparisons between isomorphous MOFs.