Polyanion Coated Positive Electrode for Solid-State Battery Interface

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Solution Overview

Problem

All solid-state batteries face a persistent issue of increasing interfacial resistance over time due to reactions between the positive electrode active material and the solid electrolyte, which affects the battery's performance and durability, especially when transition metals are involved.

Innovation Solution

A composite positive electrode active material is developed, featuring a transition metal-containing positive electrode active material coated with a reaction suppressor made of a polyanion structure-containing compound. This suppressor, with a cation moiety and a center atom covalently bonded to multiple oxygen atoms, forms a thin transition metal-reducing layer on the surface, reducing interfacial resistance and enhancing electrochemical stability.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Reliability

If LiNbO3 is coated onto the surface of LiCoO2 to reduce interfacial resistance, then initial interfacial resistance is reduced, but interfacial resistance rises over time due to reactions with solid electrolyte material

Engineering Contradiction:
Improveinterfacial resistanceVSAvoidtime stability
Core Design Contradiction:
ReliabilityVSDuration of action of stationary object

Solution Approach 1:

The patent introduces a reaction suppressor layer as an intermediary substance between the positive electrode active material and the solid electrolyte material. This reaction suppressor, composed of a polyanion structure-containing compound, mediates the interface to prevent harmful reactions while maintaining low interfacial resistance over time.

Inventive Principle:
Principle #24Intermediary (Mediator)

Solution Approach 2:

The patent creates a composite structure consisting of the positive electrode active material (containing transition metal) combined with a reaction suppressor layer. This composite material approach allows the system to benefit from both the electrochemical activity of the transition metal and the stability of the polyanion structure.

Inventive Principle:
Principle #40Composite materials

2Stability of the object's composition

If a compound with polyanion structural moiety is used to suppress reactions, then electrochemical stability is improved, but interfacial resistance may still rise when transition metal is present

Engineering Contradiction:
Improveelectrochemical stabilityVSAvoidinterfacial resistance
Core Design Contradiction:
Stability of the object's compositionVSReliability

Solution Approach 1:

The patent optimizes specific parameters of the polyanion structure-containing compound, including the electronegativity of the center atom (1.74 or more) and the thickness of the reaction suppressor layer (1 nm to 500 nm). These parameter changes ensure both electrochemical stability and low interfacial resistance.

Inventive Principle:
Principle #35Parameter changes

3Power

If transition metal is used in positive electrode active material, then battery performance is improved, but interfacial resistance rises due to reactions with solid electrolyte

Engineering Contradiction:
Improvebattery performanceVSAvoidinterfacial resistance
Core Design Contradiction:
PowerVSReliability

Solution Approach 1:

The patent applies local quality by creating a reaction suppressor layer specifically at the interface region where the positive electrode active material contacts the solid electrolyte. This localized treatment preserves the bulk properties of the transition metal-containing material while protecting the critical interface region.

Inventive Principle:
Principle #3Local quality

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 composite positive electrode active material effectively decreases interfacial resistance and suppresses the formation of high-resistance layers, leading to improved battery performance and durability by maintaining low resistance over time, even when used with high-resistance layer-forming solid electrolytes.

Implementation Method 1

a transition metal-reducing layer which has self-assembled on the surface of the positive electrode active material in contact with the reaction suppressor owing to reaction of the transition metal with the polyanion structure-containing compound

Methodology Applied
Scientific EffectChemical reaction: Chemical Bonding

Implementation Method 2

when a compound having a polyanion structural moiety with covalent bonds is used instead of LiNbO3, such a compound substantially does not react with the positive electrode active material and the solid electrolyte material

Methodology Applied
Scientific EffectChemical stability: Chemical Bonding

Data Source

PatentUS9391328B2Composite positive electrode active material, all solid-state battery, and methods for manufacture thereof
Publication Date: 2016.07.12 TOYOTA JIDOSHA KK
  • US9391328B2 patent drawing
  • US9391328B2 patent drawing
  • US9391328B2 patent drawing

AI summary

A composite positive electrode active material includes: a positive electrode active material which includes a transition metal; and a reaction suppressor which is formed so as to cover a surface of the positive electrode active material, and which is made of a polyanion structure-containing compound having a cation moiety composed of a metal atom that becomes a conducting ion and having a polyanion structural moiety composed of a center atom that is covalently bonded to a plurality of oxygen atoms. A transition metal-reducing layer which has self-assembled on the surface of the positive electrode active material in contact with the reaction suppressor owing to reaction of the transition metal with the polyanion structure-containing compound, has a thickness of 10 nm or less.