All-Solid Battery Grain Boundary Coating for Ionic Conduction

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Solution Overview

Problem

All-solid lithium ion batteries face challenges in achieving high current charge and discharge efficiency due to chemical compounds that inhibit ionic conduction at the interface between the electrode and solid electrolyte layers, and low electrical conductivity of electrode active materials, leading to insufficient reaction during calcination.

Innovation Solution

A coating layer with a thickness of 1 to 200 nm is applied to at least 30% of the grain boundary surrounding electrode active material particles, using materials like C, Au, Ag, Cu, Pd, Ru, Ni, Fe, Co, Mn, Ti, Sn, Al, and Si, to reduce reaction inhibition and enhance electrical conductivity, allowing for high current charge and discharge capabilities.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Ease of manufacture

If electrode precursor and solid electrolyte precursor are calcined at the same time, then manufacturing cost is reduced and interface joining is improved, but chemical compounds that inhibit ionic conduction are generated at the interface

Engineering Contradiction:
Improvemanufacturing process simplicityVSAvoidionic conduction capability
Core Design Contradiction:
Ease of manufactureVSReliability

Solution Approach 1:

A coating layer is formed on the electrode precursor before calcination to prevent harmful reactions during the subsequent high-temperature treatment. This preliminary protective action allows the electrode and solid electrolyte to be calcined together without generating ionic conduction inhibitors at the interface.

Inventive Principle:
Principle #10Preliminary action

Solution Approach 2:

A coating layer acts as an intermediary substance between the electrode and solid electrolyte during calcination. This intermediate layer prevents direct harmful chemical reactions while allowing ionic conduction to proceed, thus enabling simultaneous calcination without compromising ionic conduction capability.

Inventive Principle:
Principle #24Intermediary (Mediator)

2Strength

If high calcination temperature is used, then sintering of electrode and solid electrolyte is improved, but chemical compounds that inhibit ionic conduction are generated

Engineering Contradiction:
Improvesintering qualityVSAvoidionic conduction capability
Core Design Contradiction:
StrengthVSReliability

Solution Approach 1:

The coating layer is applied to the electrode precursor before calcination to protect against harmful reactions at high temperatures. This preliminary protection enables the use of high calcination temperatures for improved sintering without generating ionic conduction inhibitors.

Inventive Principle:
Principle #10Preliminary action

Solution Approach 2:

The coating layer serves as a protective intermediary that allows high-temperature calcination to proceed without generating harmful chemical compounds. It mediates between the high temperature environment and the electrode-solid electrolyte interface to prevent ionic conduction inhibition.

Inventive Principle:
Principle #24Intermediary (Mediator)

3Reliability

If low calcination temperature is used, then harmful chemical reactions are reduced, but sintering of electrode and solid electrolyte is insufficient

Engineering Contradiction:
Improveionic conduction capabilityVSAvoidsintering quality
Core Design Contradiction:
ReliabilityVSStrength

Solution Approach 1:

The coating layer is applied before calcination to enable low-temperature processing. This preliminary protection allows sufficient sintering to occur at lower temperatures without generating harmful chemical compounds that would inhibit ionic conduction.

Inventive Principle:
Principle #10Preliminary action

4Power

If electrode active material with high reducing power is used, then electromotive force is increased, but reaction with solid electrolyte during calcination generates ionic conduction inhibitors

Engineering Contradiction:
Improveelectromotive forceVSAvoidionic conduction capability
Core Design Contradiction:
PowerVSReliability

Solution Approach 1:

A coating layer is applied to the electrode active material with high reducing power before calcination to protect it from reacting with the solid electrolyte. This preliminary protection allows high electromotive force materials to be used without generating ionic conduction inhibitors at the interface.

Inventive Principle:
Principle #10Preliminary action

Solution Approach 2:

The coating layer acts as an intermediary that prevents direct contact and harmful reactions between the high reducing power electrode active material and the solid electrolyte during calcination, while still allowing the high electromotive force characteristics to be maintained.

Inventive Principle:
Principle #24Intermediary (Mediator)

5Reliability

If coating layer is applied to grain boundary, then ionic conduction is improved, but manufacturing complexity increases

Engineering Contradiction:
Improveionic conduction capabilityVSAvoidmanufacturing process complexity
Core Design Contradiction:
ReliabilityVSDevice complexity

Solution Approach 1:

The coating layer is applied to the electrode precursor before calcination in a single integrated process step. This preliminary action forms the coating on grain boundaries during the normal calcination process, improving ionic conduction without adding significant manufacturing complexity.

Inventive Principle:
Principle #10Preliminary action

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 solution enables high charge and discharge efficiency at large operation currents while reducing manufacturing costs by minimizing materials that inhibit ionic conduction and improving electron supply and emission in the electrode active material.

Implementation Method 1

a portion of at least 30% by area of a grain boundary surrounding the electrode active material particles has a coating layer with a thickness of 1 to 200 nm... there are extremely few materials that inhibit ionic conduction in an interface between an electrode layer and a solid electrolyte layer

Methodology Applied
Scientific EffectChemical reaction inhibition:

Implementation Method 2

even in a case in which electrical conductivity of an electrode active material itself is low, supply and emission of electrons are performed well in the electrode active material

Methodology Applied
Scientific EffectElectrical conduction: Conduction (electrical)

Implementation Method 3

in the interface between a solid electrolyte layer and an electrode layer, a reaction between the two layers would generate chemical compounds that inhibit ionic conduction

Methodology Applied
Scientific EffectIonic conduction: Conduction (electrical)

Data Source

PatentUS9159989B2All-solid battery and method of manufacturing the same
Publication Date: 2015.10.13 OHARA INC
  • US9159989B2 patent drawing
  • US9159989B2 patent drawing
  • US9159989B2 patent drawing

AI summary

The all-solid battery has two electrode layers of a positive electrode and a negative electrode interposing a solid electrolyte layer therebetween, in which at least one of the electrode layers is composed of a sintered body of a mixed material including at least one or more types of electrode active material particles comprising electrode active material and solid electrolyte particles comprising solid electrolyte, and a portion of at least 30% by area of a grain boundary surrounding the electrode active material particles has a coating layer with a thickness of 1 to 200 nm.