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Solid-state Graft Copolymer Electrolytes for Lithium Battery Applications
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Air-Stable High-Voltage Li-Ion Organic Cathode Enabled by Localized High-Concentration Electrolyte.

Alae Eddine Lakraychi1,2, Ifeanyi Emmanuel Udom1, Wen Ren3

  • 1Department of Electrical and Computer Engineering, University of Houston, Houston, TX, 77204, USA.

Chemsuschem
|March 27, 2025
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Summary

Dithiin-fused dilithium naphthazarin (DNP-Li) shows promise as a stable, high-voltage organic cathode for lithium-ion batteries. Its performance is significantly enhanced by localized high-concentration electrolytes (LHCE), improving cycling stability.

Keywords:
high‐voltage Li‐ion organic cathodeslocalized high‐concentration electrolytesmultielectron small‐molecule organic cathodessolute–electrolyte interactions

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Sustainable Energy

Background:

  • Lithium-ion batteries rely on critical minerals, posing supply chain risks.
  • Organic cathodes offer a sustainable alternative to traditional metal-based cathodes.
  • Dithiin-fused dilithium naphthazarin (DNP-Li) is explored as a high-voltage organic cathode material.

Purpose of the Study:

  • To evaluate the performance of DNP-Li as a Li-ion organic cathode.
  • To investigate the impact of localized high-concentration electrolyte (LHCE) on DNP-Li's electrochemical behavior.
  • To understand solute-electrolyte interactions in multielectron small-molecule organic cathodes.

Main Methods:

  • Electrochemical performance testing of DNP-Li with different electrolytes (carbonate-based vs. LHCE).
  • Analysis of voltage profiles and phase transitions under varying electrolyte conditions.
  • Cycling stability assessment at different charge/discharge rates (0.1C and 0.5C).

Main Results:

  • DNP-Li demonstrates high operating potential (3.55 V vs. Li+/Li) and specific capacity (232 mAh g-1).
  • LHCE significantly improves cycling stability, retaining 85% capacity after 50 cycles at 0.1C and 75% after 160 cycles at 0.5C.
  • Electrolyte composition dictates voltage profiles and phase transition reversibility.

Conclusions:

  • DNP-Li is a promising, stable, high-voltage organic cathode material.
  • LHCE enhances DNP-Li performance by reducing redox intermediate solubility and improving cycling stability.
  • Solute-electrolyte interactions are crucial for optimizing multielectron organic cathode performance for sustainable energy storage.