High Entropy Composite Oxide Anode for Li-Ion Batteries
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Solution Overview
Problem
Conventional high-entropy alloy materials used in lithium-ion batteries require inactive components to stabilize the anode structure, which reduces specific capacitance and cycle stability, limiting their performance.
Innovation Solution
A high-entropy composite oxide with a spinel crystal structure, represented by the formula (M1pMnqFexCryNiz)3O4, is developed, where [M1] is Co or Ti, with a non-equal molar ratio design that disperses various valence states of cations, forming oxygen vacancies and enhancing lithium-ion conductivity and cycle stability.
Engineering Contradictions & Design Principles
Engineering Contradiction Analysis
1Stability of the object's composition
If inactive material (MgO) is added to stabilize the high-entropy alloy structure, then structural stability is improved, but specific capacitance decreases
Solution Approach 1:
The patent removes the inactive stabilizing material (MgO) from the high-entropy alloy composition and replaces it with active metal elements (Co, Ni, Cu, Zn, Mn) that can simultaneously provide both structural stability and electrochemical activity. This extraction of the harmful inactive component resolves the contradiction by eliminating the need for non-contributing stabilizers.
Solution Approach 2:
The patent creates a composite high-entropy alloy structure where multiple active metal elements (Co, Ni, Cu, Zn, Mn) are combined in a spinel oxide matrix. This composite approach allows the material to achieve structural stability through the synergistic interaction of multiple active elements rather than relying on inactive fillers, thereby maintaining both stability and specific capacitance.
2Ease of manufacture
If traditional alloy materials are used, then manufacturing simplicity is maintained, but performance and service life are limited
Solution Approach 1:
The patent changes the compositional parameters by introducing five or more metal elements in specific proportions (each between 5-40 at%) to create a high-entropy alloy with enhanced properties. This parameter change transforms the material from traditional low-entropy alloys with limited service life to high-entropy alloys with superior reliability while maintaining compatibility with existing manufacturing processes.
Solution Approach 2:
The patent utilizes the formation of a spinel oxide phase structure in the high-entropy alloy, which provides exceptional structural stability and resistance to degradation. The spinel phase transition and stabilization mechanism enables the material to maintain its integrity under electrochemical cycling, significantly extending service life compared to traditional alloy phases.
3Reliability
If high-entropy alloy materials are used to improve lithium-ion conductivity, then conductivity is enhanced, but cycle stability deteriorates without inactive stabilizers
Solution Approach 1:
The patent optimizes the compositional parameters by carefully controlling the ratios of Co, Ni, Cu, Zn, and Mn elements, along with oxygen content, to achieve the optimal balance between lithium-ion conductivity and structural stability. The specific composition ranges (5-40 at% for each element) are designed to maximize ionic conductivity pathways while maintaining phase stability during cycling.
Solution Approach 2:
The patent creates a composite spinel oxide structure where the high-entropy alloying of multiple metal elements generates a synergistic effect that simultaneously enhances lithium-ion conductivity and cycle stability. The spinel matrix provides stable ion transport pathways while the multi-element composition prevents structural degradation, eliminating the need for inactive stabilizers.
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 high-entropy composite oxide significantly increases lithium-ion conductivity, charge/discharge capability, and specific capacitance, while providing redox durability and excellent cycle stability, making it suitable for high-performance lithium-ion batteries.
Implementation Method 1
subjecting the reaction solution to a hydrothermal reaction, wherein the reaction solution includes a precursor salt, an oxidizer, and a surfactant dissolved therein
Implementation Method 2
the reaction solution includes a precursor salt, an oxidizer, and a surfactant dissolved therein
Data Source
AI summary
Provided is a high entropy composite oxide of formula ([M1]pMnqFexCryNiz)3O4 having a spinel crystal, wherein the [M1], p, q, x, y and z are as defined in the specification. A method for producing the high entropy composite oxide, and anode materials including the same are further provided. With the entropy stabilization effect and plenty of oxygen vacancies, the anode materials including the high entropy composite oxide show the advantage of high Li+ transport rate, high electric capacity, redox durability, and good cycling stability, thereby having a bright prospect for application.


