Positive Electrode Crystal Orientation for Stable High-Ni Batteries

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Solution Overview

Problem

Conventional positive electrode active materials for lithium secondary batteries, particularly high-Ni-type materials, face challenges with structural instability leading to rapid deterioration at both high and room temperatures, coupled with issues of cation mixing and phase transformations during calcination.

Innovation Solution

The development of a positive electrode active material where the lithium ion diffusion path is directed to a specific crystal plane, such as the (012), (101), or (104) planes, with improved growth of these crystal planes, enhancing both electrochemical properties and stability. This is achieved through controlled calcination conditions and the use of fluxes during the synthesis of lithium composite oxides.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Quantity of substance

If the Ni content in the positive electrode active material is increased to achieve high capacity characteristics, then the discharge capacity is improved, but structural instability occurs due to Li/Ni cation mixing

Engineering Contradiction:
Improvedischarge capacityVSAvoidstructural stability
Core Design Contradiction:
Quantity of substanceVSStability of the object's composition

Solution Approach 1:

The patent applies local quality by creating a core-shell structure where the surface region has different composition and properties from the core. The surface is enriched with Li and depleted of Ni compared to the bulk, forming a protective layer that prevents cation mixing at the surface while maintaining high Ni content in the core for high capacity. This local compositional variation resolves the contradiction by protecting the structurally unstable high-Ni core.

Inventive Principle:
Principle #3Local quality

Solution Approach 2:

The patent creates a composite structure consisting of a high-Ni layered oxide core and a Li-rich surface layer. This composite material approach combines the high capacity advantage of high-Ni materials with the structural stability of Li-rich surfaces, effectively resolving the contradiction between capacity and stability.

Inventive Principle:
Principle #40Composite materials

2Stability of the object's composition

If a single-crystal lithium composite oxide is synthesized by excessively increasing or extending the calcination temperature to achieve single crystallization, then the crystallinity is improved, but cation mixing phenomenon increases

Engineering Contradiction:
ImprovecrystallinityVSAvoidcation mixing
Core Design Contradiction:
Stability of the object's compositionVSManufacturing precision

Solution Approach 1:

The patent applies preliminary action by forming a precursor structure with controlled composition before final calcination. The surface is pre-enriched with Li and depleted of Ni before the high-temperature treatment, so that even when single crystallization occurs at high temperature, the cation mixing is limited because the surface composition is already optimized. This preliminary compositional adjustment prevents excessive cation mixing during the crystallization process.

Inventive Principle:
Principle #10Preliminary action

Solution Approach 2:

The patent changes the compositional parameters during synthesis, specifically creating a gradient in Li and Ni content from core to surface. By controlling the Li/Ni ratio as a function of position and synthesis conditions, the patent achieves single crystallization while minimizing cation mixing through parameter optimization.

Inventive Principle:
Principle #35Parameter changes

3Ease of manufacture

If excessive lithium composite oxides with metastable or rock-salt phase are formed due to increased cation mixing, then the synthesis is simplified, but the electrochemical properties deteriorate

Engineering Contradiction:
Improvesynthesis simplicityVSAvoidelectrochemical properties
Core Design Contradiction:
Ease of manufactureVSReliability

Solution Approach 1:

The patent applies preliminary anti-action by creating a Li-rich surface composition that prevents the formation of metastable or rock-salt phases during calcination. The surface Li enrichment acts as a protective barrier that suppresses unwanted phase transformations even when high-temperature treatment is applied, thereby maintaining electrochemical properties while allowing simplified synthesis conditions.

Inventive Principle:
Principle #9Preliminary anti-action

4Ease of manufacture

If the crystal plane growth is not controlled, then the synthesis process is simpler, but the lithium ion diffusion path is not optimized

Engineering Contradiction:
Improvesynthesis simplicityVSAvoidlithium ion diffusion
Core Design Contradiction:
Ease of manufactureVSSpeed

Solution Approach 1:

The patent changes the synthesis parameters (calcination temperature, time, and atmosphere) to control crystal plane growth orientation. By optimizing these parameters, the patent promotes growth of specific crystal planes that expose surfaces with favorable lithium ion diffusion pathways, thereby improving ion diffusion speed while maintaining a relatively simple synthesis process.

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

The proposed solution maintains high electrochemical properties while improving structural stability, reducing the likelihood of side reactions with the electrolyte and enhancing thermal stability, thus extending the lifespan and performance of lithium secondary batteries.

Implementation Method 1

a lithium secondary battery storing electrical energy due to a difference in chemical potential when lithium ions are intercalated/deintercalated into/from a positive electrode and a negative electrode

Methodology Applied
Scientific EffectIntercalation/Deintercalation: Absorption (physical)

Implementation Method 2

a positive electrode active material which is formed such that a lithium ion diffusion path in a lithium composite oxide constituting a positive electrode active material is directed to a specific crystal plane, and has improved electrochemical properties and stability by improving the growth of the crystal plane to which the lithium ion diffusion path is directed

Methodology Applied
Scientific EffectCrystallization: Crystallisation

Implementation Method 3

This is achieved through controlled calcination conditions and the use of fluxes during the synthesis of lithium composite oxides

Methodology Applied
Scientific EffectHeat treatment: Heat Treatment

Data Source

PatentEP4183749B1Positive electrode active material and lithium secondary battery using the same
Publication Date: 2025.02.19 ECOPRO BM CO LTD
  • EP4183749B1 patent drawingFigure 1~2
  • EP4183749B1 patent drawingFigure 3~6
  • EP4183749B1 patent drawing

AI summary

The present invention relates to a positive electrode active material which is formed such that a lithium ion diffusion path in a lithium composite oxide constituting a positive electrode active material is directed to a specific crystal plane, and has improved electrochemical properties and stability by improving the growth of the crystal plane to which the lithium ion diffusion path is directed, and a lithium secondary battery using the same.