Si/C Precomposite Particles via Solvent-Free Granulation

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Solution Overview

Problem

Current methods for producing silicon-carbon (Si/C) composite particles for lithium-ion battery anodes face challenges such as solvent usage, particle aggregation, and inefficient energy transfer due to the need for solvent evaporation and inert gas atomization in spray drying processes, leading to suboptimal spherical structure and particle size distribution.

Innovation Solution

A solvent-free process involving dry mixing of silicon particles with polyacrylonitrile and carbon additives, followed by thermal treatment to create precomposite particles that convert into Si/C composite particles with minimal aggregation, using polyacrylonitrile to form a conductive carbon matrix around silicon particles.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Shape

If spray drying process is used to produce spherical Si/C composite particles, then spherical structure is achieved, but solvent usage and energy consumption increase

Engineering Contradiction:
Improvespherical structureVSAvoidenergy consumption
Core Design Contradiction:
ShapeVSLoss of energy

Solution Approach 1:

The invention extracts and removes the solvent evaporation step from the traditional spray drying process. By using a solvent-free granulation process followed by direct carbonization, the method eliminates the energy-intensive step of evaporating organic solvents while still achieving spherical particle morphology through mechanical granulation rather than aerosol drying.

Inventive Principle:
Principle #2Taking out (Extraction)

Solution Approach 2:

The invention replaces the thermal-mechanical spray drying system with a mechanical granulation system. Instead of using spray drying equipment that requires solvent evaporation, the method uses a granulator to mechanically form spherical particles from dry powder mixtures, substituting thermal energy with mechanical energy for particle formation.

Inventive Principle:
Principle #28Mechanics substitution (Replace mechanical system)

2Shape

If spray drying process is used to produce Si/C composite particles, then spherical particles are formed, but particle aggregation occurs

Engineering Contradiction:
Improvespherical particlesVSAvoidparticle size distribution
Core Design Contradiction:
ShapeVSManufacturing precision

Solution Approach 1:

The invention performs preliminary classification of particles after granulation and before carbonization. By separating oversized aggregates and undersized particles at the green particle stage, the method prevents aggregation issues from propagating through the carbonization process, ensuring better particle size distribution in the final product.

Inventive Principle:
Principle #10Preliminary action

Solution Approach 2:

The invention changes the processing parameters by operating the granulator at controlled speeds and using specific binder contents to optimize particle formation. By adjusting granulation parameters such as rotation speed, feed rate, and binder addition, the method achieves spherical particles with narrow size distribution without the aggregation problems associated with spray drying.

Inventive Principle:
Principle #35Parameter changes

3Stability of the object's composition

If inert gas atomization is used in spray drying, then dispersion is achieved, but device complexity and cost increase

Engineering Contradiction:
Improvehomogeneous distributionVSAvoidprocessing complexity
Core Design Contradiction:
Stability of the object's compositionVSDevice complexity

Solution Approach 1:

The invention extracts and removes the inert gas atomization system from the process. By using direct mechanical granulation of dry powders without solvent dispersion, the method eliminates the need for complex gas flow control systems, atomization nozzles, and inert gas handling equipment, significantly simplifying the overall process design.

Inventive Principle:
Principle #2Taking out (Extraction)

Solution Approach 2:

The invention allows the powder mixture to self-bind during granulation using minimal binder addition. The granulation process itself provides the mixing and distribution function that would otherwise require inert gas atomization, with the binder serving multiple functions of lubrication, binding, and homogeneous distribution without requiring external gas systems.

Inventive Principle:
Principle #25Self-service

4Shape

If solvent evaporation is used in spray drying, then particle formation is achieved, but processing time and energy consumption increase

Engineering Contradiction:
Improveparticle formationVSAvoidprocessing time
Core Design Contradiction:
ShapeVSLoss of time

Solution Approach 1:

The invention extracts the time-consuming solvent evaporation step from the particle formation process. By using solvent-free granulation where particles are formed directly from dry powder compaction and binding, the method eliminates the extended drying time required for solvent removal, significantly reducing overall processing time.

Inventive Principle:
Principle #2Taking out (Extraction)

Solution Approach 2:

The invention inverts the traditional approach by forming particles first through mechanical granulation and then applying carbon coating, rather than forming particles through solvent-based aerosol that requires subsequent drying. This reversal of the process sequence eliminates the evaporation step entirely and accelerates particle production.

Inventive Principle:
Principle #13The other way round (Inversion)

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 process produces Si/C composite particles with improved mechanical stability and homogeneous distribution of components, avoiding solvent-related issues and particle aggregation, resulting in enhanced electrochemical performance and reduced processing complexity.

Implementation Method 1

followed by thermal treatment to create precomposite particles that convert into Si/C composite particles

Methodology Applied
Scientific EffectPyrolysis: Pyrolysis

Data Source

PatentEP3497055B1Production of si/c precomposite particles
Publication Date: 2022.03.16 WACKER CHEMIE AG
  • EP3497055B1 patent drawingFigure 1~2
  • EP3497055B1 patent drawingFigure 3~4

AI summary

The invention provides processes for producing precomposite particles by mixing silicon particles, polyacrylonitrile and one or more carbon additives (C additives) based on one carbon polymorph, optionally one or more organic pore formers and optionally one or more inorganic additives, each in the form of a powder, wherein no solvent is added before and during the mixing, and the inorganic additives are selected from the group comprising halides of the alkali metals and alkaline earth metals, carbonates of the alkali metals, zinc oxide, magnesium carbonate and nickel sulfide, wherein the polyacrylonitrile, the silicon particles and/or the C additives are wholly or partly initially charged prior to the mixing or are wholly or partly metered in during the mixing, with the proviso that, without polyacrylonitrile in the initial charge, the silicon particles and/or the C additives are at least partly metered in together with polyacrylonitrile or after addition of polyacrylonitrile. The invention further provides processes for producing Si/C composite particles, characterized in that the aforementioned precomposite particles are subjected to thermal treatment.