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Lean electrolytes in lithium-sulfur (Li-S) batteries hinder performance. This study identifies activation polarization during sulfur nucleation as the key limit, offering insights for improved Li-S battery design.

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Energy Storage

Background:

  • Lithium-sulfur (Li-S) batteries offer high energy density potential beyond lithium-ion technology.
  • Achieving high energy density requires lean electrolyte conditions, which paradoxically degrade battery performance, particularly sulfur cathode kinetics.

Purpose of the Study:

  • To systematically decouple and identify the primary kinetic limiting factor in sulfur cathodes under lean electrolyte conditions in Li-S batteries.
  • To provide guidance for developing effective strategies to enhance Li-S battery performance.

Main Methods:

  • Developed a combined electrochemical impedance spectroscopy (EIS) and galvanostatic intermittent titration technique (GITT) method.
  • Decoupled cathodic polarizations into activation, concentration, and ohmic components.

Main Results:

  • Identified activation polarization during lithium sulfide nucleation as the dominant factor limiting performance as the electrolyte-to-sulfur (E/S) ratio decreases.
  • Sluggish interfacial charge transfer kinetics was confirmed as the main reason for performance degradation in lean electrolytes.
  • A novel lithium bis(fluorosulfonyl)imide electrolyte reduced activation polarization, enabling Li-S batteries to achieve 985 mAh g-1 at a low E/S ratio of 4 μL mg-1 (0.2 C).

Conclusions:

  • Activation polarization during lithium sulfide nucleation is the critical bottleneck in lean-electrolyte Li-S batteries.
  • The findings guide the design of targeted strategies, such as electrolyte modification, to overcome kinetic limitations and advance Li-S battery technology.