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Schottky defects arise when some lattice points in a crystal, such as those in NaCl, remain unoccupied, creating lattice vacancies without disturbing the overall electrical neutrality of the crystal. This defect is common in ionic crystals where the positive and negative ions are similar in size, as seen in sodium chloride and cesium chloride. The presence of Schottky defects enables the crystal to conduct electricity to a small extent through an ionic mechanism. Electric fields cause nearby...
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The Debye-Hückel-Onsager equation is a cornerstone of physical chemistry, providing a method to determine the molar conductance (Λm) and molar conductance at infinite dilution (Λ°m) for uni-univalent electrolytes.Uni-univalent electrolytes are electrolytes that dissociate in solution to produce one cation with a +1 charge and one anion with a –1 charge per formula unit.This equation addresses two crucial phenomena: the asymmetry effect and the electrophoretic effect.
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Preparation of Graphene Liquid Cells for the Observation of Lithium-ion Battery Material
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Defect evolution in graphene upon electrochemical lithiation.

Laila Jaber-Ansari1, Kanan P Puntambekar, Hadi Tavassol

  • 1Department of Materials Science and Engineering, Northwestern University , Evanston, Illinois 60208, United States.

ACS Applied Materials & Interfaces
|September 30, 2014
PubMed
Summary

Graphene defect formation accelerates during lithium-ion battery cycling due to lithiation. Defects act as active sites, leading to degradation until lithium can diffuse freely, minimizing further changes.

Keywords:
Raman spectroscopydefectsdensity functional theorygraphenelithium ion batterysilicon

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Nanotechnology

Background:

  • Graphene is of significant interest for lithium-ion batteries.
  • Understanding graphene's interaction with lithium ions and electrolyte species during cycling is crucial but not fully understood.

Purpose of the Study:

  • To investigate graphene defect formation during lithiation using a model system.
  • To elucidate the mechanisms of graphene degradation in lithium-ion battery environments.

Main Methods:

  • Utilized Raman spectroscopy on monolayer graphene on a Si(111) substrate.
  • Employed density functional theory (DFT) calculations to model defect formation and chemical interactions.
  • Performed ex situ and Ar-atmosphere Raman spectroscopy to track defect evolution.

Main Results:

  • Observed a rapid increase in graphene defect levels (I(D)/I(G) ratio) with initial lithiation/delithiation cycles.
  • Detected a significant drop in 2D peak intensity in Raman spectra, indicating structural changes.
  • DFT revealed that defects act as active sites for Li, O, and F, accelerating degradation via a positive feedback loop.

Conclusions:

  • Graphene degradation accelerates initially due to lithiation-induced defect formation and chemical functionalization.
  • Degradation stabilizes once sufficient defects allow unimpeded lithium diffusion.
  • Mechanistic insights inform the use of graphene in advanced lithium-ion battery technologies.