Composite lithium metal negative electrode material, preparation method thereof and metal lithium battery

A technology for lithium metal batteries and metal negative electrodes, which can be applied to lithium batteries, negative electrodes, battery electrodes, etc., and can solve the problems of poor wettability between LLZO and lithium

Pending Publication Date: 2022-06-24
CHONGQING UNIV
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Problems solved by technology

[0003] But the most critical problem is that the inorganic ceramic solid electrolyte will chemically react with air to form lithium carbonate, which will cover the surface of the solid electrolyte, resulting in poor wettability between LLZO and lithium.
Although these methods can improve the interfacial contact between the solid electrolyte and the lithium anode and reduce the interfacial impedance, however, these modification strategies are relatively strict, and there are still many limitations for practical applications, such as the high temperature or corrosive environment required to remove the impurity layer. and the expensive equipment needed to deposit the lithium-philic layer, etc.

Method used

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  • Composite lithium metal negative electrode material, preparation method thereof and metal lithium battery
  • Composite lithium metal negative electrode material, preparation method thereof and metal lithium battery
  • Composite lithium metal negative electrode material, preparation method thereof and metal lithium battery

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preparation example Construction

[0031] The present invention also provides a method for preparing a composite lithium metal negative electrode material, comprising the following steps:

[0032] A) mix the skeleton material with the nitrate solution, and obtain the additive material after drying;

[0033] B) Mixing the additive material with molten metal lithium, and cooling to obtain a composite lithium metal negative electrode material.

[0034] The present invention firstly configures a nitrate solution, and the nitrate is preferably one or more of aluminum nitrate, magnesium nitrate, lithium nitrate, zinc nitrate, copper nitrate, nickel nitrate, tin nitrate, bismuth nitrate, antimony nitrate and iron nitrate ; The concentration of the nitrate solution is preferably 0.05-0.2 mol / L, more preferably 0.1-0.15 mol / L.

[0035] Then, the framework material is added to the nitrate solution, sonicated, and dried to obtain the additive material.

[0036] In the present invention, the type of the skeleton material...

Embodiment 1

[0049] A 0.1 mol / L nitrate aqueous solution was prepared, then CNTs were added to the above solution according to the mass ratio of nitrate:CNT=1:20, ultrasonicated for 30 min, and finally the above solution was dried to obtain CNT / nitrate powder.

[0050] Lithium metal was heated to 200°C to a molten state, and then different mass ratios (0.5%, 1% and 5%) of additives (CNT / nitrate powder) were added to the molten lithium.

[0051] The nitrate additive and the molten lithium were stirred at a constant temperature for 5 min until the mixture was uniform, and then cooled to room temperature to obtain a modified lithium composite negative electrode material.

[0052] (1) The LLZO was placed in a glove box, and composite lithium was used as an electrode to assemble a composite lithium / / LLZTO / / composite lithium symmetrical lithium battery, and its interface impedance and cycle stability were evaluated.

[0053] The result is as figure 1 shown, by figure 1 It can be seen that when...

Embodiment 2

[0059] The carbon cloth (CC) was soaked in 0.1M nitrate solution to construct a three-dimensional composite negative electrode. During the soaking process, ultrasonication for 10 min can also improve the lithiophilicity of the carbon cloth. The lithium metal was heated to 200 °C, and the above three-dimensional composite electrode was immersed in the molten carbon cloth. In lithium, molten lithium can be automatically adsorbed into the carbon cloth and impregnated for 40s to obtain a composite negative electrode material.

[0060] Using carbon cloth and pure lithium sheet as electrodes, and using ester electrolyte without any additives, LNO-CC / / LE / / LNO-CC and Li / / LE / / Li symmetrical lithium batteries were assembled respectively. Cyclic Stability,

[0061] The result is as Image 6 As shown, the resulting LNO-CC / / LE / / LNO-CC symmetric cell can be operated at 1 mA cm -2 (1mAh cm -2 ) for 500 hours. In the comparison experiment, the overpotential fluctuation of the symmetric ba...

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Abstract

The invention provides a composite lithium metal negative electrode material. The composite lithium metal negative electrode material comprises a framework material, and Li3N, LiNOx and metal lithium which are compounded with the framework material, the framework material comprises one or more of a carbon nano tube, carbon cloth, a three-dimensional porous copper film, a three-dimensional porous aluminum film and a carbon nano tube film. A framework material, nitrate and molten metal lithium are mixed, the framework material, lithium nitride, nitrogen oxide and the like are generated through an in-situ chemical reaction, a CNT/Li3N/LiNOx/lithium dual-ion electronic conductive network is provided, and the composite lithium negative electrode with stable interface, high ionic conductivity and high electronic conductivity dual conductive network is obtained; meanwhile, the formation of interface holes in the battery circulation process can be inhibited, and the long circulation stability of the solid-state battery is realized. The invention also provides a preparation method of the composite lithium metal negative electrode material and a metal lithium battery.

Description

technical field [0001] The invention belongs to the technical field of metal lithium batteries, and in particular relates to a composite lithium metal negative electrode material, a preparation method thereof and a metal lithium battery. Background technique [0002] The lithium metal anode has a high specific capacity (3680mAh g -1 ), low electrode potential (-3.04V vs standard hydrogen electrode) and low density (0.59g cm -3 ) and other characteristics, inorganic solid-state electrolytes (LLZO) have the advantages of high ionic conductivity, wide electrochemical window, high thermal stability, high mechanical strength and chemical stability to lithium metal, so solid-state lithium metal batteries have become the research focus of next-generation lithium batteries. one. [0003] However, the most critical problem is that the inorganic ceramic solid electrolyte will chemically react with the air to generate lithium carbonate, and the lithium carbonate will cover the surfac...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): H01M4/62H01M4/36H01M4/38H01M4/58H01M10/052H01M10/0525H01M10/0562H01M10/0563H01M10/0566H01M12/06
CPCH01M4/362H01M4/382H01M4/58H01M4/625H01M4/626H01M4/628H01M10/052H01M10/0525H01M10/0566H01M10/0562H01M10/0563H01M12/06H01M2004/021H01M2004/027
Inventor 徐朝和逯贯杰王荣华
Owner CHONGQING UNIV
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