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Interfacial and Electronic Modulation via Localized Sulfurization for Boosting Lithium Storage Kinetics.

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Summary

This study introduces a novel 3D crumpled S-functionalized MXene integrated with iron oxide/sulfide heterostructures for advanced lithium storage. The resulting electrode exhibits remarkable cycling stability and rate capability, offering a new strategy for high-performance energy storage devices.

Keywords:
MXenesheterostructuresinterfacial and electronic propertieslithiation/delithiation pathwayslithium-ion batteries

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Nanotechnology

Background:

  • Structural modulation is key for advanced electrochemical energy storage.
  • Developing effective nanoscale tuning strategies for MXene materials remains a challenge.

Purpose of the Study:

  • To design and synthesize a novel 3D crumpled S-functionalized Ti3C2Tx substrate integrated with Fe3O4/FeS heterostructures.
  • To investigate the structural, electronic, and electrochemical properties of the hybrid electrode for lithium storage applications.

Main Methods:

  • Coprecipitation and partial sulfurization for heterostructure formation.
  • Electrochemical testing (cycling stability, rate capability).
  • Operando X-ray diffraction, in situ electroanalytical techniques, and first-principles calculations for mechanism elucidation.

Main Results:

  • The optimized hybrid electrode demonstrated excellent long-term cycling stability (913.9 mAh g⁻¹ after 1000 cycles at 1 A g⁻¹) and superior rate capability (490.4 mAh g⁻¹ at 10 A g⁻¹).
  • Surface S-terminations on MXene enhanced pseudocapacitive lithium storage.
  • Asymmetric conversion mechanism with stepwise phase transformations during discharge and uniform reconversion during charge was identified.

Conclusions:

  • The developed hybrid electrode offers a highly active and stable architecture for lithium storage.
  • This work provides a novel strategy for designing high-performance MXene-based hybrids.
  • The study deepens the understanding of complex lithium intercalation and conversion reactions in hybrid electrodes.