Nitrogen Argyrodite Solid Electrolyte for High-Voltage Stability

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Solution Overview

Problem

Current lithium-ion batteries using liquid electrolytes pose safety risks due to flammable organic solvents, and sulfide-based solid electrolytes have weak stability at high voltages, necessitating an improved solid electrolyte for enhanced safety and performance.

Innovation Solution

A solid electrolyte with a nitrogen-containing compound having an argyrodite crystal structure, specifically represented by Formula (Li1-aMa)7-d+xPS6-d-x+kNxXd, is developed, which includes a mixture of lithium, sulfur, phosphorus, and nitrogen precursors, heat-treated at temperatures above 300°C to achieve improved ion conductivity and stability.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Reliability

If sulfide-based solid electrolyte is used, then ion conductivity is improved, but stability towards oxidation at high voltage deteriorates

Engineering Contradiction:
Improveion conductivityVSAvoidstability towards oxidation at high voltage
Core Design Contradiction:
ReliabilityVSStability of the object's composition

Solution Approach 1:

The patent applies composite materials by combining multiple elements (Li, P, S, Ge, and halogens) to form a complex argyrodite structure. This composite approach allows the electrolyte to achieve both high ion conductivity and improved oxidation stability at high voltages, resolving the contradiction between these two properties that plagues simpler sulfide-based electrolytes.

Inventive Principle:
Principle #40Composite materials

Solution Approach 2:

The patent utilizes parameter changes by systematically varying the composition ratios of Li, P, S, Ge, and halogen elements in the argyrodite structure. By optimizing these compositional parameters, the electrolyte achieves enhanced oxidation stability while maintaining high ion conductivity, thus resolving the contradiction between these two critical properties.

Inventive Principle:
Principle #35Parameter changes

2Ease of manufacture

If liquid electrolyte is used, then ease of manufacture is improved, but safety deteriorates due to flammable organic solvent

Engineering Contradiction:
Improveease of manufactureVSAvoidsafety
Core Design Contradiction:
Ease of manufactureVSObject-affected harmful factors

Solution Approach 1:

The patent applies parameter changes by transitioning from liquid to solid state electrolyte, fundamentally changing the physical state parameter. This solidification eliminates the flammability issue while the argyrodite crystal structure maintains good ion conductivity, thus improving safety without severely compromising manufacturability.

Inventive Principle:
Principle #35Parameter changes

Solution Approach 2:

The patent uses composite materials by creating a complex argyrodite structure with multiple elements (Li, P, S, Ge, halogens) that combines the advantages of solid electrolytes (safety) with high ion conductivity. This composite approach makes solid electrolytes more viable for practical applications compared to simple solid electrolytes.

Inventive Principle:
Principle #40Composite materials

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 nitrogen-containing solid electrolyte exhibits stabilized interfaces, increased ion conductivity, and enhanced high-voltage stability, leading to improved discharge capacity and cycle characteristics in electrochemical cells, making them safer and more efficient.

Implementation Method 1

heat-treating the solid electrolyte precursor at a temperature equal to or greater than about 300° C. to prepare the solid electrolyte including the compound of Formula 1

Methodology Applied
Scientific EffectHeat treatment: Heat Treatment

Implementation Method 2

a solid electrolyte with a nitrogen-containing compound having an argyrodite crystal structure

Methodology Applied
Scientific EffectCrystallization: Crystallisation

Data Source

PatentUS11908994B2Metal and nitrogen-including argyrodite solid electrolyte, electrochemical cell including solid electrolyte, and method of preparing solid electrolyte oxide
Publication Date: 2024.02.20 SAMSUNG SDI CO LTD
  • US11908994B2 patent drawing
  • US11908994B2 patent drawing
  • US11908994B2 patent drawing

AI summary

A solid electrolyte including a compound represented by Formula 1:(Li1-aMa)7-d+xPS6-d-x+kNxXd  Formula 1wherein, in Formula 1,M is Na, K, Ca, Fe, Mg, Ag, Cu, Zr, Zn, or a combination thereof;X is Cl, Br, F, I, a pseudohalogen, or a combination thereof; and0<x<1, 0≤a<1, 0<d≤1.8, and 0≤k<1, andwherein the compound has an argyrodite crystal structure.