Lithium Metal Anode Interfacial Layer for Stable Cycling

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Solution Overview

Problem

Lithium metal negative electrodes in secondary lithium metal batteries experience large volumetric changes during cycling, leading to inadequate mechanical stability and flexibility of the native Solid Electrolyte Interphase (SEI) layer, which results in direct exposure to the electrolyte, side reactions, and lithium consumption.

Innovation Solution

A protective interfacial layer is formed on the lithium metal negative electrode using a precursor solution containing a dioxolane and a fluorinated organosilane, creating a composite structure with a polymeric matrix and a lithium-containing dispersed component, which enhances mechanical stability and prevents undesirable side reactions.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Reliability

If a native SEI layer is formed on the lithium metal negative electrode, then direct exposure to the electrolyte is prevented and uniform plating/stripping is promoted, but the mechanical stability and flexibility are inadequate to accommodate large volumetric changes during cycling

Engineering Contradiction:
Improveprotection against electrolyte exposureVSAvoidmechanical stability
Core Design Contradiction:
ReliabilityVSStrength

Solution Approach 1:

The patent applies composite materials by combining polymeric components with inorganic lithium-containing components to form a protective interfacial layer. This composite structure provides both the flexibility needed to accommodate volumetric changes during cycling and the mechanical stability required to prevent cracking and maintain protection throughout battery operation.

Inventive Principle:
Principle #40Composite materials

Solution Approach 2:

The patent changes the physical and chemical parameters of the protective layer by controlling the composition ratios of dioxolane (10-50 wt%), fluorinated organosilane (5-40 wt%), and other components. This parameter optimization ensures the layer has appropriate flexibility and mechanical properties to withstand volumetric expansion and contraction during battery cycling.

Inventive Principle:
Principle #35Parameter changes

2Reliability

If a native SEI layer is formed on the lithium metal negative electrode, then uniform plating and stripping of lithium ions is promoted, but the layer cracks or damages over time due to inadequate flexibility

Engineering Contradiction:
Improveuniform plating and strippingVSAvoidcycle life
Core Design Contradiction:
ReliabilityVSDuration of action of moving object

Solution Approach 1:

The patent employs a flexible protective interfacial layer with thickness of 1-20 micrometers that can accommodate the volumetric changes of lithium metal during cycling. The flexible polymer matrix combined with inorganic components creates a layer that bends and expands/contricts with the lithium metal without cracking, thereby maintaining protection throughout the battery's operational life.

Inventive Principle:
Principle #30Flexible shells and thin films

Solution Approach 2:

The composite structure of polymeric and inorganic components provides both flexibility for accommodating volumetric changes and mechanical strength to prevent cracking. This composite approach ensures the protective layer remains intact over extended cycling, preventing electrolyte exposure and maintaining uniform plating/stripping behavior.

Inventive Principle:
Principle #40Composite materials

3Reliability

If the SEI layer cracks or damages during cycling, then direct exposure of the electrolyte to lithium metal occurs, but this leads to additional SEI formation and consumption of active lithium

Engineering Contradiction:
Improveprotection functionVSAvoidactive lithium consumption
Core Design Contradiction:
ReliabilityVSLoss of substance

Solution Approach 1:

The patent applies beforehand cushioning by forming a robust, flexible protective interfacial layer before battery operation begins. This pre-formed layer is designed to accommodate volumetric changes during cycling without cracking, thereby preventing electrolyte exposure and the subsequent formation of additional SEI material that would consume active lithium. The layer acts as a cushion against the mechanical stresses of cycling.

Inventive Principle:
Principle #11Beforehand cushioning (Prior cushioning)

Solution Approach 2:

The patent converts the potentially harmful effect of volumetric changes into a benefit by designing a protective layer that flexes and expands/contricts with the lithium metal during cycling. This flexibility, which might seem to compromise mechanical stability, actually prevents cracking and maintains the protective function, thereby preventing electrolyte decomposition and active lithium loss.

Inventive Principle:
Principle #22Blessing in disguise (Convert harm into benefit)

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

The protective interfacial layer provides exceptional flexibility and mechanical stability, accommodating volumetric changes during battery cycling while preventing direct contact with the electrolyte, thus improving coulombic efficiency and cycling stability without decomposing the electrolyte or consuming active lithium.

Implementation Method 1

The polymeric matrix component may be chemically bonded to the major surface of the lithium metal substrate via a plurality of silicon-oxygen bonds and/or alkoxide bonds

Methodology Applied
Scientific EffectChemical Bonding: Chemical Bonding

Implementation Method 2

The fluorinated organosilane may have the formula: R′R′′nSiX4-n, wherein n=0, 1, or 2, and wherein R′ is a polyfluorinated C1-C8 alkyl group, R′′ is a methyl group, and X is a methoxy group or a chlorine atom

Methodology Applied
Scientific EffectHydrolysis: Hydrolysis

Implementation Method 3

The protective interfacial layer exhibits a composite structure including a polymeric matrix component and a lithium-containing dispersed component embedded in the polymeric matrix component

Methodology Applied
Scientific EffectCondensation: Condensation

Data Source

PatentUS12334561B2Lithium metal negative electrode and method of manufacturing the same
Publication Date: 2025.06.17 GM GLOBAL TECHNOLOGY OPERATIONS LLC
  • US12334561B2 patent drawing
  • US12334561B2 patent drawing

AI summary

A negative electrode for an electrochemical cell of a secondary lithium metal battery is manufactured by a method in which a precursor solution is applied to a major surface of a lithium metal substrate to form a protective interfacial layer thereon. The precursor solution includes a first organic solvent mixture, a dioxolane, and a fluorinated organosilane. The protective interfacial layer exhibits a composite structure including a polymeric matrix component and a lithium-containing dispersed component embedded in the polymeric matrix component.