Silicon Anode SEI Layer Stability via Fluorinated Carbonate Additives

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Solution Overview

Problem

Lithium-ion rechargeable battery cells with silicon anodes face challenges due to significant volume changes during charging and discharging, leading to mechanical degradation and reduced cycle life, along with issues in forming a stable Solid Electrolyte Interface (SEI) layer, which affects charge/discharge efficiency and cycle life.

Innovation Solution

The use of structured silicon materials with specific additives such as vinylene carbonate (VC) and halogenated cyclic carbonates like fluoroethylene carbonate (FEC) in the electrolyte, which help in forming a stable and flexible SEI layer, and maintaining anode performance and longevity by controlling the SEI formation and expansion during lithiation.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Quantity of substance

If silicon is used as anode material instead of graphite, then capacity is significantly increased, but volume change during charging/discharging causes mechanical degradation

Engineering Contradiction:
ImprovecapacityVSAvoidcycle life
Core Design Contradiction:
Quantity of substanceVSReliability

Solution Approach 1:

A flexible coating layer comprising fluorinated cyclic carbonate is applied to the silicon-based anode material. This coating acts as a protective shell that accommodates the volume expansion and contraction of silicon during lithiation and delithiation, preventing mechanical degradation and maintaining structural integrity over multiple cycles.

Inventive Principle:
Principle #30Flexible shells and thin films

Solution Approach 2:

The patent modifies the chemical composition and physical properties of the coating layer by using fluorinated cyclic carbonate with specific fluorine substitution patterns. This changes the coating's flexibility, adhesion, and stability parameters to match the dynamic volume changes of silicon, enabling it to withstand expansion/contraction cycles while maintaining protection.

Inventive Principle:
Principle #35Parameter changes

2Quantity of substance

If silicon anode material is charged to full lithiation, then maximum capacity is achieved, but crystalline phase formation causes additional mechanical stresses

Engineering Contradiction:
Improvecharge capacityVSAvoidanode material stability
Core Design Contradiction:
Quantity of substanceVSStrength

Solution Approach 1:

The flexible coating layer is formed on the silicon anode material before full lithiation occurs. This pre-formed coating prevents the formation of crystalline Li15Si4 phase by accommodating volume expansion at lower lithiation levels, thereby avoiding the mechanical stresses associated with crystalline-amorphous transitions while still achieving high capacity.

Inventive Principle:
Principle #10Preliminary action

3Ease of operation

If conventional electrolyte is used with silicon anode, then basic battery operation is achieved, but SEI layer formation is unstable affecting efficiency

Engineering Contradiction:
Improvebattery operationVSAvoidSEI layer stability
Core Design Contradiction:
Ease of operationVSReliability

Solution Approach 1:

The patent changes the chemical parameters of the electrolyte by introducing fluorinated cyclic carbonate additives with specific molecular structures and fluorine substitution patterns. This modification alters the SEI layer formation process, creating a more stable and flexible interface that accommodates silicon volume changes while maintaining ionic conductivity for basic battery operation.

Inventive Principle:
Principle #35Parameter changes

Applied Scientific Principles

This section explains which scientific principles are used to turn an abstract innovation direction into a practical engineering solution.

Function Achieved in This Case

This approach enhances the cycle performance and efficiency of lithium-ion cells by maintaining a stable SEI layer, reducing mechanical stress, and extending the cycle life of silicon anode materials, thereby improving the overall performance and longevity of the battery.

Implementation Method 1

the electrolyte including as an additive at least 5wt% of a halogenated cyclic carbonate... forming a stable and flexible SEI layer

Methodology Applied
Scientific EffectSEI layer formation: Electrolysis

Implementation Method 2

the volume of a fully lithiated Li-Si alloy can be 3-4 times larger than the unalloyed silicon volume... associated with the insertion and removal of lithium ions

Methodology Applied
Scientific EffectLithiation-induced expansion: Absorption (physical)

Data Source

PatentEP2922119B1A lithium ion rechargeable battery cell
Publication Date: 2020.07.22 NEXEON LTD
  • EP2922119B1 patent drawingFigure 1~2
  • EP2922119B1 patent drawingFigure 3~4
  • EP2922119B1 patent drawingFigure 5~6

AI summary

The present invention claims the addition of vinylene carbonate (VC) and optionally also fluoroethylene carbonate to the electrolyte of lithium ion cells having a structural silicon composite anode, i.e. an anode containing fibres or particles of silicon. The additive significantly improves the cycling performance of the cells. A VC content in the range 3.5 - 8 wt% based on the weight of the electrolyte has been found to be optimum.