Anhydride Electrolyte Additives for Stable Silicon Battery Interfaces

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Solution Overview

Problem

Lithium-ion batteries with silicon-based anodes and high-voltage nickel-rich cathodes face challenges such as unstable solid electrolyte interphase layers, oxidative instability, and poor cycling life due to volumetric expansion and transition metal ion dissolution, limiting their energy density and safety.

Innovation Solution

The development of anhydride-based electrolyte additives that form stable, electronically insulating but ionically conducting solid electrolyte interphase layers on silicon anodes and cathode electrolyte interphase films, enhancing mechanical strength, thermal stability, and reducing flammability to improve the electrochemical performance and safety of silicon-based lithium-ion batteries.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Quantity of substance

If silicon-based anodes are used to increase energy density, then capacity is improved, but volumetric expansion during lithiation causes disintegration and reduces cycling life

Engineering Contradiction:
ImprovecapacityVSAvoidcycling life
Core Design Contradiction:
Quantity of substanceVSReliability

Solution Approach 1:

The anhydride additive performs preliminary action by forming a stable SEI layer on the silicon anode surface before the electrolyte can decompose. This pre-formed protective layer prevents subsequent electrolyte reduction and maintains interface stability during silicon expansion and contraction cycles.

Inventive Principle:
Principle #10Preliminary action

Solution Approach 2:

The anhydride-derived SEI layer acts as an intermediary between the silicon anode and the liquid electrolyte. This intermediate layer mechanically accommodates silicon volumetric changes while chemically preventing direct contact between the electrolyte and silicon surface, thereby preventing electrolyte decomposition and maintaining cycling stability.

Inventive Principle:
Principle #24Intermediary (Mediator)

2Quantity of substance

If conventional electrolytes are used with high-voltage cathodes, then energy density is improved, but oxidative instability occurs beyond 4.5 V leading to accelerated decay

Engineering Contradiction:
Improveenergy densityVSAvoidelectrolyte stability
Core Design Contradiction:
Quantity of substanceVSStability of the object's composition

Solution Approach 1:

The anhydride additive performs preliminary oxidation at the cathode interface before the bulk electrolyte can undergo oxidative decomposition. By forming a CEI film on the high-voltage cathode surface first, it prevents subsequent electrolyte oxidation even at potentials beyond 4.5 V.

Inventive Principle:
Principle #10Preliminary action

Solution Approach 2:

The anhydride additive changes the electrochemical stability window parameters of the electrolyte system. By introducing this additive, the oxidation potential threshold is effectively extended beyond 4.5 V, allowing high-voltage cathodes to operate stably at elevated potentials without electrolyte decomposition.

Inventive Principle:
Principle #35Parameter changes

3Quantity of substance

If silicon anodes are used to achieve high capacity, then energy density is improved, but unstable SEI layer leads to endless electrolyte exposure and irreversible capacity loss

Engineering Contradiction:
ImprovecapacityVSAvoidirreversible capacity loss
Core Design Contradiction:
Quantity of substanceVSLoss of energy

Solution Approach 1:

The anhydride additive forms a stable SEI layer during initial cycles before the electrolyte can repeatedly decompose. This preliminary SEI formation prevents subsequent electrolyte reduction reactions that would otherwise cause continuous irreversible capacity loss.

Inventive Principle:
Principle #10Preliminary action

Solution Approach 2:

The anhydride-derived SEI layer serves as a stable intermediary that prevents direct electrolyte contact with the silicon anode surface. This intermediate layer eliminates the endless cycle of electrolyte decomposition and reformation, thereby preventing irreversible capacity loss while maintaining silicon's high capacity.

Inventive Principle:
Principle #24Intermediary (Mediator)

4Quantity of substance

If transition metal ions dissolve into electrolyte from NCM/NCA cathodes, then capacity is improved, but stability deteriorates due to surface layer exfoliation and continuous decomposition

Engineering Contradiction:
ImprovecapacityVSAvoidsurface layer stability
Core Design Contradiction:
Quantity of substanceVSStability of the object's composition

Solution Approach 1:

The anhydride-derived CEI film acts as an intermediary protective layer between the NCM/NCA cathode and the liquid electrolyte. This intermediate film prevents transition metal ion dissolution into the electrolyte and stops continuous electrolyte decomposition, thereby stabilizing the cathode surface layer while maintaining high capacity.

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 anhydride additives improves the cycle life, energy density, and safety of silicon-based lithium-ion batteries by stabilizing the electrolyte interface, reducing electrolyte decomposition, and enhancing thermal stability, leading to improved electrochemical performance and reduced risk of mechanical and electrical failure.

Implementation Method 1

anhydride-based electrolyte additives that form stable, electronically insulating but ionically conducting solid electrolyte interphase layers on silicon anodes

Methodology Applied
Scientific EffectSolid electrolyte interphase formation:

Implementation Method 2

formative of a stable cathode electrolyte interphase film on high voltage cathodes

Methodology Applied
Scientific EffectCathode electrolyte interphase formation:

Implementation Method 3

ionically conducting solid electrolyte interphase layers

Methodology Applied
Scientific EffectIonic conduction: Conduction (electrical)

Data Source

PatentUS11837711B2Silicon-based energy storage devices with anhydride containing electrolyte additives
Publication Date: 2023.12.05 ENEVATE CORP
  • US11837711B2 patent drawing
  • US11837711B2 patent drawing
  • US11837711B2 patent drawing

AI summary

Electrolytes and electrolyte additives for energy storage devices including an anhydride compound are provided. The energy storage device includes a first electrode and a second electrode, where at least one of the first electrode and the second electrode is a Si-based electrode, a separator between the first electrode and the second electrode, an electrolyte, and at least one electrolyte additive which is an anhydride compound.