Si-Anode Battery Separator Structure for Hi-Pot Defect Reduction
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Solution Overview
Problem
The use of Si-based anode active materials in lithium secondary batteries leads to increased volume expansion, internal pressure, and local damage to the separator during lamination, resulting in Hi-pot defects and reduced capacity retention rates.
Innovation Solution
A lithium secondary battery with a separator substrate made of polyolefin resin having a specific polydispersity index (PDI) of 2.5 to 4.2, average pore size of 20 to 40 nm, and maximum pore size of 50 nm or less, exhibiting a strain of 25% or less under tensile stress, and a recovery rate of 70% within 200 seconds, along with an organic/inorganic composite coating layer for improved compression resistance.
Engineering Contradictions & Design Principles
Engineering Contradiction Analysis
1Quantity of substance
If Li4SiO4 is used as negative electrode active material, then battery capacity is improved, but charge-discharge rate capability deteriorates due to slow Li-ion diffusion
Solution Approach 1:
The Li4SiO4 particles are divided into fine particles with a maximum diameter of 10 μm, preferably 1-5 μm. This segmentation increases the surface area and shortens the Li-ion diffusion path length, thereby improving charge-discharge rate capability while maintaining high battery capacity.
Solution Approach 2:
A coating layer comprising at least one of Li2SiO3 and amorphous SiO2 is formed on the surface of the Li4SiO4 particles. This local modification at the particle surface improves Li-ion diffusion kinetics at the critical interface where Li-ion insertion/extraction occurs, enhancing rate capability without reducing overall capacity.
2Quantity of substance
If Si-based negative electrode active material is used, then battery capacity is improved, but volume expansion occurs during charging
Solution Approach 1:
The invention uses Li4SiO4 as the core active material, which is a composite material combining silicon (providing high capacity) with lithium oxide (providing structural stability). This composite structure allows the material to utilize silicon's high Li-ion storage capacity while the lithium oxide component constrains volume expansion during charging cycles.
Solution Approach 2:
The invention changes the crystal structure parameter by using the olivine structure of Li4SiO4, which has a stable framework that accommodates Li-ion insertion/extraction with minimal volume change. Additionally, the coating layer of Li2SiO3 or amorphous SiO2 further stabilizes the surface structure and prevents excessive volume expansion.
3Strength
If Li4SiO4 particles are sintered at high temperature, then particle strength is improved, but Li4SiO4 crystal structure transforms to harmful phase
Solution Approach 1:
The sintering temperature is optimized to 900°C or lower, preventing the phase transformation of Li4SiO4 from the olivine structure to the harmful Li3SiO3 phase. This parameter control maintains both particle strength and crystal structure stability simultaneously.
Solution Approach 2:
A coating layer comprising Li2SiO3 or amorphous SiO2 is formed on the Li4SiO4 particles before or during sintering. This coating layer acts as a protective barrier that prevents excessive grain growth and phase transformation at elevated temperatures, allowing sintering to proceed at lower temperatures while maintaining particle strength.
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 solution enhances the separator's compression resistance, reducing Hi-pot defects and improving capacity retention rates while allowing for faster processing speeds.
Implementation Method 1
it has come to light, however, that Li4SiO4 has a low charge-discharge rate capability due to slow diffusion of Li-ions
Implementation Method 2
a coating layer comprising at least one of Li2SiO3 and amorphous SiO2 is formed on the surface of the Li4SiO4 particles
Implementation Method 3
the Li4SiO4 particles after the sintering step have a maximum diameter of 10 μm or less, preferably 1 μm to 5 μm
Data Source
Figure 1~2
Figure 3
AI summary
Provided is a lithium secondary battery with reduced Hi-pot defects and improved capacity retention rate. According to one aspect of the present disclosure, there is provided a lithium secondary battery including an anode, a cathode, and a separator interposed between the anode and the cathode, in which the anode includes a Si-based anode active material, the separator includes a separator substrate having a plurality of pores and including a polyolefin resin, the polyolefin resin has a polydispersity index (PDI) of 2.5 to 4.2, an average pore size of 20 to 40 nm, and a maximum pore size of 50 nm or less.