Low-Defect Turbostratic Carbon Envelopes for Silicon Anode Cycling

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Solution Overview

Problem

Silicon-based anode materials in lithium-ion batteries face rapid cycle life degradation, poor charge-discharge rate capability, and low coulombic efficiency due to extreme volume changes during lithiation and delithiation, leading to electrical disconnection and unstable solid electrolyte interface (SEI) formation, which compromises energy and power density.

Innovation Solution

Incorporating low-defect turbostratic carbon materials with specific Raman spectrum characteristics into the anode active material, providing a conductive network that buffers volume expansion and maintains intimate contact with silicon particles, thereby stabilizing cycle life and enhancing rate performance.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Use of energy by moving object

If silicon-based anode materials are used to achieve high energy density, then the theoretical gravimetric capacity increases to about 4,200 mAh/g, but rapid cycle life degradation occurs due to extreme volume changes during lithiation and delithiation

Engineering Contradiction:
Improvegravimetric capacityVSAvoidcycle life
Core Design Contradiction:
Use of energy by moving objectVSReliability

Solution Approach 1:

The patent applies this principle by coating silicon particles with a flexible carbon-containing material that can accommodate the extreme volume changes (up to 400% expansion) during lithiation and delithiation. This flexible coating maintains structural integrity and prevents particle pulverization, thereby resolving the contradiction between high capacity and cycle life stability.

Inventive Principle:
Principle #30Flexible shells and thin films

Solution Approach 2:

The patent creates a composite structure where silicon particles are combined with a carbon-containing material. This composite approach allows the silicon to provide high theoretical capacity while the carbon component provides structural stability and conductivity, resolving the contradiction between energy density and cycling stability.

Inventive Principle:
Principle #40Composite materials

2Quantity of substance

If silicon particles undergo significant volume fluctuations during charge and discharge, then high lithium storage capacity is achieved, but electrical disconnection occurs due to pulverization and loss of electrical contact

Engineering Contradiction:
Improvelithium storage capacityVSAvoidelectrical contact
Core Design Contradiction:
Quantity of substanceVSReliability

Solution Approach 1:

The carbon-containing coating acts as a flexible shell that maintains electrical contact with the silicon particles even during significant volume fluctuations. This flexible coating prevents pulverization and ensures continuous electrical pathways, resolving the contradiction between high lithium storage capacity and maintaining electrical contact.

Inventive Principle:
Principle #30Flexible shells and thin films

Solution Approach 2:

The carbon-containing material serves as an intermediary between the silicon particles and the electrolyte, providing a stable conductive network that maintains electrical contact. This intermediary layer prevents direct exposure of silicon to electrolyte while ensuring electrical connectivity, resolving the contradiction between capacity and electrical contact reliability.

Inventive Principle:
Principle #24Intermediary (Mediator)

3Quantity of substance

If new Si surfaces are exposed to electrolyte solvents due to cracking and fracture, then SEI formation occurs leading to lithium ion consumption, but charge/discharge rate capability and coulombic efficiency are compromised

Engineering Contradiction:
Improvelithium ion capacityVSAvoidcharge/discharge rate capability
Core Design Contradiction:
Quantity of substanceVSProductivity

Solution Approach 1:

The carbon-containing coating is applied preliminarily to protect silicon surfaces from direct contact with electrolyte solvents. This preliminary protective layer prevents unwanted SEI formation on fresh silicon surfaces during cracking, thereby preventing lithium ion consumption and maintaining charge/discharge rate capability and coulombic efficiency.

Inventive Principle:
Principle #9Preliminary anti-action

Solution Approach 2:

The carbon-containing material acts as an intermediary barrier between silicon surfaces and electrolyte solvents. This intermediary layer controls SEI formation, preventing excessive lithium ion consumption while maintaining ionic and electronic transport, thus resolving the contradiction between lithium ion capacity and charge/discharge rate capability.

Inventive Principle:
Principle #24Intermediary (Mediator)

4Reliability

If the insulating SEI layer grows thicker during charge/discharge cycling, then lithium ion transport impedance increases, but capacity and cycling stability are degraded

Engineering Contradiction:
Improvecycling stabilityVSAvoidionic transport impedance
Core Design Contradiction:
ReliabilityVSObject-affected harmful factors

Solution Approach 1:

The carbon-containing coating serves as a stable intermediary layer that mediates between silicon and electrolyte. This intermediary layer provides a controlled interface that allows ionic transport while preventing uncontrolled SEI growth, thereby maintaining low ionic transport impedance and high cycling stability simultaneously.

Inventive Principle:
Principle #24Intermediary (Mediator)

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 use of low-defect turbostratic carbon improves cycling stability, energy density, and high-rate performance of lithium-ion batteries by reducing defects and maintaining electrical contact during volume changes, resulting in longer cycle life and higher capacity retention.

Implementation Method 1

providing a conductive network that buffers volume expansion and maintains intimate contact with silicon particles

Methodology Applied
Scientific EffectVolume expansion buffering: Elasticity

Implementation Method 2

maintains electrical contact during volume changes

Methodology Applied
Scientific EffectElectrical conduction: Conduction (electrical)

Data Source

PatentUS11929494B2Anode active material including low-defect turbostratic carbon
Publication Date: 2024.03.12 M2INNOVATIONS LLC
  • US11929494B2 patent drawing
  • US11929494B2 patent drawing
  • US11929494B2 patent drawing

AI summary

An electrode material for a lithium ion secondary battery and method of forming the same, the electrode material including composite particles, each composite particle including: a primary particle including an electrochemically active material; and an envelope disposed on the surface of the primary particle. The envelope includes turbostratic carbon having a Raman spectrum having: a D band having a peak intensity (ID) at wave number between 1330 cm-1 and 1360 cm-1; a G band having a peak intensity (IG) at wave number between 1530 cm-1 and 1580 cm-1; and a 2D band having a peak intensity (I2D) at wave number between 2650 cm-1 and 2750 cm-1. In one embodiment, a ratio of ID/IG ranges from greater than zero to about 1.1, and a ratio of I2D/IG ranges from about 0.4 to about 2.