Fluorinated Nickel-Cobalt-Manganese Cathode for Gelation Control

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Solution Overview

Problem

Lithium-based composite oxides, such as LiNiO2, face issues with gelation when kneaded with binder resins and have poor capacitance characteristics, while lithium cobaltate is expensive and prone to reduced crystallinity and electrolyte decomposition, limiting their suitability for lithium secondary batteries.

Innovation Solution

A positive electrode active material is developed by mixing nickel, cobalt, and a transition metal with a lithium compound and a calcium compound, followed by firing, to incorporate calcium atoms on the surface and reduce residual Li2CO3, enhancing cycle characteristics and safety by suppressing gelation and improving coating properties.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Ease of manufacture

If LiNiO2 or lithium composite oxide with nickel replacement is used as positive electrode material, then cost is reduced compared to lithium cobaltate, but gelation occurs during kneading with binder resin causing poor coating properties

Engineering Contradiction:
ImprovecostVSAvoidcoating properties
Core Design Contradiction:
Ease of manufactureVSEase of operation

Solution Approach 1:

The patent applies fluorination treatment to the surface of LiNi0.8Co0.1Mn0.1O2 particles, changing the surface chemical composition by introducing fluorine atoms. This surface modification reduces residual Li2CO3 and improves wettability with binder resin, preventing gelation during kneading while maintaining the cost advantage of nickel-based materials

Inventive Principle:
Principle #35Parameter changes

Solution Approach 2:

The patent creates a composite structure with a LiNi0.8Co0.1Mn0.1O2 core and a fluorinated surface layer. This composite material combines the high capacity benefits of nickel-based oxides with the improved surface properties of fluorinated compounds, achieving both cost reduction and good coating properties

Inventive Principle:
Principle #40Composite materials

2Ease of manufacture

If LiNiO2 is used as positive electrode material, then cost is reduced, but residual Li2CO3 remains causing gelation during kneading

Engineering Contradiction:
ImprovecostVSAvoidstability during kneading
Core Design Contradiction:
Ease of manufactureVSReliability

Solution Approach 1:

The patent converts the harmful effect of residual Li2CO3 on the surface into a beneficial process by applying fluorination treatment. The fluorine reacts with residual Li2CO3 to form volatile LiF and CO2, eliminating the harmful residue and improving material stability during subsequent processing

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

Solution Approach 2:

The fluorination treatment changes the surface chemical parameters by introducing fluorine atoms and removing carbon-containing residues. This parameter change transforms the surface from a gelation-prone state to a stable, processable state while maintaining the cost benefits of nickel-based materials

Inventive Principle:
Principle #35Parameter changes

3Reliability

If lithium cobaltate is used as positive electrode material, then excellent electrical properties are achieved, but raw material cobalt is rare and expensive

Engineering Contradiction:
Improveelectrical propertiesVSAvoidcost
Core Design Contradiction:
ReliabilityVSEase of manufacture

Solution Approach 1:

The patent changes the compositional parameters by replacing 80% of cobalt with nickel in the LiNi0.8Co0.1Mn0.1O2 formula. This parameter change dramatically reduces cobalt content and cost while the fluorination treatment compensates for any electrical property degradation, achieving a balance between cost and performance

Inventive Principle:
Principle #35Parameter changes

Solution Approach 2:

The patent creates a composite material LiNi0.8Co0.1Mn0.1O2 that combines multiple transition metals. This composite approach reduces dependence on expensive cobalt while the fluorinated surface layer maintains good electrical properties by improving interfacial contact and reducing resistance

Inventive Principle:
Principle #40Composite materials

4Quantity of substance

If lithium cobaltate is charged with 0.7 electron or more, then capacity is increased, but crystallinity is reduced and electrolyte solution is decomposed

Engineering Contradiction:
ImprovecapacityVSAvoidcrystallinity
Core Design Contradiction:
Quantity of substanceVSReliability

Solution Approach 1:

The fluorination treatment changes the surface electrochemical parameters by introducing fluorine atoms that stabilize the surface structure. This allows the material to withstand higher charging levels (0.7 electron or more) without severe crystallinity loss or electrolyte decomposition, enabling higher capacity operation

Inventive Principle:
Principle #35Parameter changes

Solution Approach 2:

The fluorinated surface layer acts as a protective cushion before high-capacity charging occurs. This pre-applied surface modification prevents direct contact between the high-voltage charged state and the electrolyte, cushioning against decomposition reactions and maintaining crystallinity even at high charge levels

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

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 resulting lithium secondary battery exhibits excellent cycle characteristics and safety, with reduced gas generation and improved initial discharge capacity, maintaining capacity over multiple cycles.

Implementation Method 1

mixing a compound containing nickel, cobalt, a transition metal atom other than these and the like with a lithium compound and a calcium compound; and firing the resulting mixture

Methodology Applied
Scientific EffectChemical reaction: Chemical Bonding

Data Source

PatentEP2178138B1Positive electrode active material for lithium secondary battery, method for production thereof, and lithium secondary battery
Publication Date: 2013.04.17 NIPPON CHEMICAL IND CO LTD
  • EP2178138B1 patent drawingFigure 1
  • EP2178138B1 patent drawingFigure 2
  • EP2178138B1 patent drawingFigure 3

AI summary

There is provided a positive electrode active material for lithium secondary batteries which suppresses gelation when kneaded with a binder resin in producing a positive electrode material and provides excellent coating properties. The positive electrode active material for lithium secondary batteries comprises a lithium composite oxide represented by the following general formula (1) and a Ca atom contained in the lithium composite oxide. When the positive electrode active material is analyzed by X-ray diffraction using Cu- Kα radiation as a radiation source, the intensity ratio (b/a) of (b) the diffraction peak at 2θ = 18.7 ± 0.2° to (a) the diffraction peak at 2θ = 37.4 ± 0.2° derived from CaO is from 10 to 150. LixNi1-y-zCoyMezO2 (1) In the formula, Me represents a metal element having an atomic number of 11 or more other than Co and Ni; and x, y, and z are represented by the formulae 0.98 ≤ x ≤ 1.20, 0 < y ≤ 0.5, and 0 < z ≤ 0.5, respectively, provided that y + z < 1.