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Organic-inorganic composite coating film on the surface of metal lithium negative electrode and preparation method thereof

An inorganic composite, metal lithium technology, applied in the direction of battery electrodes, structural parts, electrical components, etc., can solve the problems of electrolyte penetration into the coating film and lithium metal reaction, easy detachment, increase, etc., to improve the electrochemical stability window , improve cycle life, and high flexibility

Active Publication Date: 2021-01-05
UNIV OF SCI & TECH BEIJING
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

[0006] The present invention aims at the easy detachment between the inorganic phase and the organic phase in the coating film and the coating film and metal lithium in the use and coating technology of the lithium metal negative electrode, causing the electrolyte to penetrate into the coating film and react with lithium metal, and the To solve the problem of sharp increase in interface resistance, an organic-inorganic composite coating film on the surface of the metal lithium negative electrode and its preparation method are proposed, and the surface of the metal lithium negative electrode is coated with LiSi x o y The siloxane organic phase film formed by the condensation of inorganic particles and silane improves the cycle life of the lithium metal negative electrode and its battery system, and ensures the safety of the lithium metal negative electrode and its battery system in use

Method used

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  • Organic-inorganic composite coating film on the surface of metal lithium negative electrode and preparation method thereof
  • Organic-inorganic composite coating film on the surface of metal lithium negative electrode and preparation method thereof
  • Organic-inorganic composite coating film on the surface of metal lithium negative electrode and preparation method thereof

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Experimental program
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Effect test

Embodiment 1

[0032](1) Dissolve 0.4166g of ethyl orthosilicate in 1.25g of dimethyl sulfoxide, and stir magnetically at 60°C for 7 hours to obtain a silane solution.

[0033] (2) Float the lithium slice on 1000 μL silane solution and react for 5 minutes.

[0034] (3) Rinse with dimethyl carbonate to remove excess liquid, place it in an environment with water and oxygen content ≤ 5ppm for 5 minutes, take it out, and dry it at 35°C for 3.5 hours, and a brown-gray coating film is formed on the surface.

[0035] (4) Li / Li symmetric batteries were assembled using coated lithium sheets, using commercial separators and carbonate-based LiPF 6 electrolyte.

[0036] (5) After the battery cycled for one week, the organic coating film evolved in situ to form an organic-inorganic composite coating film in which inorganic particles were randomly embedded in the organic phase with a spatial network structure. The film was bonded to lithium metal through the hydroxyl formed by hydrolysis at one end. Amo...

Embodiment 2

[0039] (1) Dissolve 0.5568g of γ-glycidoxypropyltrimethoxysilane in 1.5626g of N-methylpyrrolidone, and stir magnetically at 50°C for 5h to obtain a silane solution.

[0040] (2) Spread 800 μL of silane solution evenly on the surface of the lithium sheet and react for 1 min.

[0041] (3) Rinse with dimethyl carbonate to remove excess liquid, place it in an environment with water and oxygen content ≤ 5ppm for 5 minutes, take it out, and dry it at 45°C for 3.5 hours, and a gray coating film is formed on the surface.

[0042] (4) A lithium / lithium symmetric battery was assembled using the coated lithium sheet, using a commercial separator and an ether-based LiTFSI electrolyte.

[0043] (5) After one cycle of the battery, the organic coating film evolves in situ to form an organic-inorganic composite coating film in which inorganic particles are randomly embedded in the organic phase with a spatial network structure. metal bonding. Among them, the particle size of inorganic part...

Embodiment 3

[0046] (1) Dissolve 0.7854g (3-mercaptopropyl)trimethoxysilane in 1.7558g N-methylpyrrolidone, and stir magnetically at 65°C for 5.5h to obtain a silane solution.

[0047] (2) Spread 1000 μL of silane solution evenly on the surface of the lithium sheet and react for 8 minutes.

[0048] (3) Rinse with dimethyl carbonate to remove excess liquid, place it in an environment with water and oxygen content ≤ 5ppm for 5 minutes, take it out, and dry it at 50°C for 3.5 hours, and an off-white coating film is formed on the surface.

[0049] (4) A lithium / lithium symmetric battery was assembled using the coated lithium sheet, using a commercial separator and a carbonate-based LiODFB electrolyte.

[0050] (5) After one cycle of the battery, the organic coating film evolves in situ to form an organic-inorganic composite coating film in which inorganic particles are randomly embedded in the organic phase with a spatial network structure. The film is formed by bonding the active sulfhydryl g...

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Abstract

The invention provides an organic-inorganic composite coating film on the surface of a metal lithium negative electrode. The film comprises a siloxane organic phase formed by condensation of LiSixOy inorganic particles and silane; and the film uniformly coats the surface of metal lithium, and has the characteristics of relatively high ionic conductivity, high young modulus, small interface resistance, improved long-term working stability of the metal lithium, and the like. Meanwhile, the invention also provides a preparation method of the organic-inorganic composite coating film on the surface of the metal lithium negative electrode. The silane which is distributed on the surface of the metal lithium is subjected to adaptive phase splitting along with a first-time deposition process of the lithium to form an organic-inorganic composite double-phase structure, and the metal lithium is guided to be uniformly deposited and stripped in a charging process, so that the growth of lithium dendrites is inhibited. The cycle lives of the metal lithium negative electrode and a battery system are remarkably prolonged, and the safety of the metal lithium negative electrode and the battery system during use is guaranteed.

Description

technical field [0001] The invention relates to the technical field of batteries and key materials thereof, in particular to an organic-inorganic composite coating film on the surface of a metal lithium negative electrode and a preparation method thereof. Background technique [0002] The lithium metal anode has an ultra-high energy density (3860mAh g -1 ) and extremely low electrochemical potential (-3.04V vs standard hydrogen electrode), becoming the most promising anode material for high energy density secondary batteries. However, lithium metal has very high reactivity, which causes electrolyte loss and interface failure, especially the lithium dendrites generated during the cycle, which lead to the loss of lithium metal active materials and serious safety hazards, which restrict lithium metal from being used as a secondary battery. Development and application of negative electrode materials. [0003] Coating lithium metal with a dense layer physically isolates it from...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): H01M4/62
CPCH01M4/62H01M4/624H01M4/628Y02E60/10
Inventor 连芳梁伟朱依欣薛杉杉
Owner UNIV OF SCI & TECH BEIJING
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