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Superior Low-Temperature All-Solid-State Battery Enabled by High-Ionic-Conductivity and Low-Energy-Barrier Interface.

Pushun Lu1,2, Sheng Gong3, Chuhong Wang3

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Summary

Developing stable interfaces is key for all-solid-state batteries (ASSBs) to operate at low temperatures. This study identifies critical interface features for cryogenic conditions, improving capacity retention in ASSBs.

Keywords:
all-solid-state batteryinterface energy barrierkinetic processlow-temperature performancesulfide solid electrolyte

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Energy Storage

Background:

  • All-solid-state batteries (ASSBs) show promise for energy storage but face challenges at low temperatures.
  • The kinetic properties of interfaces in ASSBs at subzero temperatures are not well understood, hindering low-temperature design.
  • Unstable interfaces, like that between LiNi0.90Co0.05Mn0.05O2 (Ni90) and Li6PS5Cl (LPSC) solid electrolyte, lead to poor performance.

Purpose of the Study:

  • To investigate and unlock critical interface features for cryogenic temperature operation in ASSBs.
  • To understand the impact of interface modification on lithium-ion transport and activation energy at low temperatures.
  • To guide the design of robust cathode/solid electrolyte interfaces for enhanced low-temperature performance.

Main Methods:

  • Constructing and analyzing various cathode interfaces for ASSBs.
  • Utilizing Li2ZrO3 (LZO) coating to modify the Ni90/LPSC interface and reduce activation energy.
  • Replacing LPSC with Li3InCl6 (LIC) halide solid electrolyte to achieve a stable interface and low activation energy.
  • Conducting theoretical evaluations of interface properties for Li+ conduction.

Main Results:

  • Inserting an LZO coating layer reduced the activation energy of the Ni90/LPSC interface from 60.19 kJ mol-1 to 41.39 kJ mol-1.
  • Replacing LPSC with LIC halide solid electrolyte and using an LZO coating resulted in a low activation energy of 25.79 kJ mol-1.
  • The modified Ni90/LIC/LPSC/Li-In ASSB demonstrated improved capacity retention of 26.9% at -30 °C.
  • Theoretical analysis confirmed that high ionic conductivity and low energy barriers at cathode/SE interfaces are crucial for efficient Li+ transport.

Conclusions:

  • Interface stability and low activation energy are critical for effective low-temperature operation of ASSBs.
  • Li2ZrO3 coating and Li3InCl6 halide solid electrolyte are promising strategies for enhancing low-temperature performance.
  • Understanding interfacial kinetics provides essential guidance for designing next-generation cryogenic ASSBs.