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Ions are atoms or molecules bearing an electrical charge. A cation (a positive ion) forms when a neutral atom loses one or more electrons from its valence shell, and an anion (a negative ion) forms when a neutral atom gains one or more electrons in its valence shell. Compounds composed of ions are called ionic compounds (or salts), and their constituent ions are held together by ionic bonds: electrostatic forces of attraction between oppositely charged cations and anions. 
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A type of Lewis acid-base chemistry involves the formation of a complex ion (or a coordination complex) comprising a central atom, typically a transition metal cation, surrounded by ions or molecules called ligands. These ligands can be neutral molecules like H2O or NH3, or ions such as CN− or OH−. Often, the ligands act as Lewis bases, donating a pair of electrons to the central atom. These types of Lewis acid-base reactions are examples of a broad subdiscipline called coordination...
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Initial SEI formation in LiBOB-, LiDFOB- and LiBF4-containing PEO electrolytes.

Edvin K W Andersson1, Liang-Ting Wu2, Luca Bertoli3

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|April 18, 2024
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Summary
This summary is machine-generated.

Understanding the solid polymer electrolyte (SPE) decomposition layer in lithium batteries is key. PEO:LiDFOB shows superior performance due to minimal interface decomposition, forming a more effective protective layer.

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Battery Technology

Background:

  • Solid polymer electrolytes (SPEs) are crucial for Li-battery safety and performance.
  • The electrolyte decomposition layer at the Li metal anode interface significantly impacts battery functionality.
  • Improving this layer is essential for advancing Li-battery technology.

Purpose of the Study:

  • To investigate the electrolyte decomposition layer in three different SPEs: PEO:LiBF4, PEO:LiBOB, and PEO:LiDFOB.
  • To correlate cell performance with the initial SPE decomposition at the anode interface.
  • To understand the formation and impact of the solid electrolyte interphase (SEI).

Main Methods:

  • Electrochemical impedance spectroscopy (EIS) for interface analysis.
  • Galvanostatic cycling to evaluate cell performance and capacity retention.
  • In situ Li deposition photoelectron spectroscopy (PES) for surface characterization.
  • Ab initio molecular dynamics (AIMD) simulations for mechanistic insights.

Main Results:

  • PEO:LiDFOB demonstrated the highest capacity retention among the investigated SPEs.
  • Lower SPE decomposition at the interface correlated with better performance and a more effective protective layer.
  • PES and AIMD revealed polyethylene formation in the SEI, originating from ethylene free-radical polymerization.

Conclusions:

  • The PEO:LiDFOB electrolyte forms a more effective decomposition layer with less initial decomposition.
  • Reduced interface decomposition is key to enhanced Li-battery performance and longevity.
  • Polyethylene formation via ethylene polymerization is a significant pathway in PEO-based SPE SEI.