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Lithium ion all-solid all-battery and preparation method thereof

An all-solid-state, all-battery technology, used in lithium batteries, battery electrodes, secondary batteries, etc., can solve the problems of low lithium ion conductivity, loss of active materials, and decreased electrochemical cycle stability of silicon anodes, to avoid safety. The effect of avoiding hidden dangers, inhibiting volume expansion, and avoiding the shuttle effect

Active Publication Date: 2019-06-21
SHANDONG UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

The volume of the silicon negative electrode continues to expand and shrink during the charging and discharging process, which makes the liquid electrolyte and the new surface produced by the broken silicon continuously react to form an SEI film, resulting in the continuous loss of active materials, and the electrochemical cycle stability of the silicon negative electrode drops sharply.
Generally, the problem of volume expansion is solved by nanosizing, compounding or alloying silicon, but the inventors found that the compounded silicon composite has the disadvantage of low lithium ion conductivity

Method used

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  • Lithium ion all-solid all-battery and preparation method thereof
  • Lithium ion all-solid all-battery and preparation method thereof
  • Lithium ion all-solid all-battery and preparation method thereof

Examples

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preparation example Construction

[0043]A method for preparing a lithium sulfide / silicon solid-state full battery, comprising the steps of:

[0044] (1) Preparation of silicon / solid electrolyte composite anode material refers to the patent "A silicon anode material coated with sulfur-based solid electrolyte and its preparation method" to prepare the corresponding anode material";

[0045] (2) The lithium sulfide / carbon composite was prepared by ball milling or absolute ethanol dissolution.

[0046] (3) Sulfur-based solid electrolyte prepared by solution method or ball milling sintering method.

[0047] (4) Silicon / sulfur-based solid electrolyte composite anode material, sulfur-based solid electrolyte and carbon material are ball milled or ground with a mortar under certain conditions.

[0048] (5) Lithium sulfide / carbon composite material, sulfur-based solid electrolyte and carbon material are ball milled or ground with a mortar under certain conditions.

[0049] (6) Assemble the negative electrode obtained ...

Embodiment 1

[0063] Grind lithium sulfide and phosphorus pentasulfide in a mortar at a ratio of 1:1 (molar ratio), add silicon and ground sulfide to tetrahydrofuran at a ratio of 1:1 (mass ratio), stir magnetically at room temperature for 8 hours, and use rotary evaporation The organic solvent was removed by the method, and the heat treatment was performed at 50° C. for 24 hours to obtain a silicon / sulfur-based solid electrolyte composite negative electrode material.

[0064] Lithium sulfide and Ketjen black were mixed and ball-milled at a ratio of 3:1 (mass ratio) for 24 hours to obtain a lithium sulfide / carbon composite material. Preparation of solid electrolyte Li by solution method using lithium sulfide and phosphorus pentasulfide as raw materials 4 P 2 S 6 .

[0065] Preparation of solid electrolyte Li by solution method using lithium sulfide and phosphorus pentasulfide as raw materials 7 P 3 S 11 .

[0066] The silicon / sulfur-based solid electrolyte composite anode material, t...

Embodiment 2

[0068] Mill lithium sulfide, phosphorus pentasulfide, and aluminum sulfide in a ball mill for 12 hours at a ratio of 5:2:1 (molar ratio), and add silicon and mixed sulfide to dimethyl ether at a ratio of 1:5 (mass ratio), at 50°C Under magnetic stirring for 24 hours, the organic solvent was removed by suction filtration, and heat treated at 700° C. for 6 hours to obtain a silicon / sulfur-based solid electrolyte composite negative electrode material.

[0069] Dissolve lithium sulfide in absolute ethanol to obtain a solution with a mass fraction of 10%, add a certain amount of graphite solution, wherein the mass ratio of graphene to lithium sulfide is 1:1, evaporate the ethanol to dryness, and obtain the powder under argon atmosphere Heat treatment at 500°C for 8 hours to obtain a lithium sulfide / carbon composite material.

[0070] The silicon / sulfur-based solid-state electrolyte composite negative electrode material, the sulfur-based solid-state electrolyte, and the carbon mater...

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Abstract

The invention relates to lithium sulfide / silicon solid-state all-battery positive and negative electrode materials with high cycling performance and preparation method thereof. A silicon / sulfur-basedsolid-state electrolyte composite negative electrode material is prepared through a solution in-situ synthesis one-step method; and the method is simple and convenient to operate, and the electrochemical performance stability and the electrochemical cycling performance are improved through sulfur-based solid-state electrolyte coating. A lithium sulfide / carbon composite positive electrode materialis prepared, and the carbon material can effectively improve the electronic conductivity of a lithium sulfide material and inhibit the volume expansion of lithium sulfide in charging and discharging;meanwhile, the utilization rate of the active substances can be improved by lithium sulfide nano-crystallization, so that the electrochemical performance is improved. The assembled lithium sulfide / silicon solid-state all-battery has high electrochemical cycling performance, and meanwhile, the interface problem of a lithium-sulfur battery and a solid electrolyte can be effectively solved, and potential safety hazards caused by metal lithium are avoided.

Description

technical field [0001] The invention belongs to the technical field of new energy materials, and in particular relates to an electrode material for a lithium sulfide / silicon solid-state full battery, battery preparation and application. Background technique [0002] In order to meet the demand for energy storage devices for grid energy storage, electric vehicles, and consumer electronics, lithium-sulfur batteries have received widespread attention. Lithium-sulfur batteries have high specific capacity and energy density. At the same time, they are rich in sulfur storage, environmentally friendly, and basically have no pollution to the environment. Therefore, lithium-sulfur batteries are considered to be a very promising lithium battery. However, there are certain problems and shortcomings in lithium-sulfur batteries, such as the shuttle effect of polysulfur compounds, the low conductivity of sulfur and the volume expansion during the cycle, and the lithium metal produces lith...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): H01M10/0562H01M4/36H01M4/58H01M4/583H01M4/62H01M4/38H01M10/052
CPCY02E60/10
Inventor 慈立杰徐小燕
Owner SHANDONG UNIV
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