Method for preparing solid electrolytes using sonochemical process

Patent metadata

Field	Value
Publication number	US-2019067745-A1
Application number	US-201815991580-A
Country	US
Kind code	A1
Filing date	May 29, 2018
Priority date	Aug 30, 2017
Publication date	Feb 28, 2019
Grant date	—

Abstract

The present invention relates to a method for preparing a solid electrolyte using a sonochemical process, which includes a step of preparing a reaction vessel holding a solid electrolyte raw material in a solid or liquid form and a step of reacting the solid electrolyte raw material by applying energy into the reaction vessel by irradiating an ultrasound to the reaction vessel.

First claim

What is claimed is:

1 . A method for preparing a solid electrolyte using a sonochemical process, comprising:
preparing a reaction vessel holding a solid electrolyte raw material in a liquid form; and reacting the solid electrolyte raw material by applying energy into the reaction vessel by irradiating an ultrasound to the reaction vessel.

2 . The method for preparing a solid electrolyte using a sonochemical process according to claim 1 , wherein the solid electrolyte raw material comprises:
10-40 mol % of a sulfide-based raw material selected from a group consisting of P 2 S 3 , P 2 S 5 , P 4 S 3 , P 4 S 5 , P 4 S 7 , P 4 S 10 and a combination thereof; and 60-90 mol % of lithium sulfide (Li 2 S).

3 . The method for preparing a solid electrolyte using a sonochemical process according to claim 1 , wherein the solid electrolyte raw material is dissolved in a polar organic solvent selected from a group consisting of an ester-based solvent, a carbonate-based solvent, an ether-based solvent, a furan-based solvent and a combination thereof.

4 . The method for preparing a solid electrolyte using a sonochemical process according to claim 1 , wherein reacting the solid electrolyte raw material is conducted by irradiating an ultrasound with a frequency of 20-2,000 kHz to the reaction vessel for 1 minute to 6 hours.

5 . The method for preparing a solid electrolyte using a sonochemical process according to claim 1 , wherein reacting the solid electrolyte raw material is conducted at −50° C. to 200° C.

6 . The method for preparing a solid electrolyte using a sonochemical process according to claim 1 , wherein reacting the solid electrolyte raw material comprises sealing the reaction vessel, immersing the reaction vessel in a water bath equipped with an ultrasound generating apparatus and filled with a medium and then irradiating an ultrasound to the reaction vessel.

7 . The method for preparing a solid electrolyte using a sonochemical process according to claim 1 , which further comprises drying a product obtained by reacting the solid electrolyte raw material.

8 . The method for preparing a solid electrolyte using a sonochemical process according to claim 7 , which further comprises heat-treating the dried product at 250-800° C. for 1 minute to 100 hours.

9 . The method for preparing a solid electrolyte using a sonochemical process according to claim 1 , wherein the solid electrolyte has a shape selected from a group consisting of a sphere, a plate, a needle and a combination thereof.

10 . A continuous circulation reactor for preparing a solid electrolyte using a sonochemical process, comprising:
a storage reservoir holding a solid electrolyte raw material in a liquid form; an ultrasound generator comprising a reaction tube and an ultrasound irradiation means which is located outside the reaction tube and reacts the solid electrolyte raw material by applying energy into the reaction tube by irradiating an ultrasound to the reaction tube; a first transport pipe one end of which is inserted in the storage reservoir and contacts the solid electrolyte raw material and the other end of which is connected to a circulation pump; a second transport pipe one end of which is connected to the circulation pump and the other end of which is linked with one end of the reaction tube; and a third transport pipe one end of which is linked with other end of the reaction tube and the other end of which is inserted in the storage reservoir; and the circulation pump which allows the solid electrolyte raw material to flow from the storage reservoir through the reaction tube and again into the storage reservoir.

11 . The continuous circulation reactor for preparing a solid electrolyte using a sonochemical process according to claim 10 , wherein the solid electrolyte raw material comprises:
10-40 mol % of a sulfide-based raw material selected from a group consisting of P 2 S 3 , P 2 S 5 , P 4 S 3 , P 4 S 5 , P 4 S 7 , P 4 S 10 and a combination thereof; and 60-90 mol % of lithium sulfide (Li 2 S).

12 . The continuous circulation reactor for preparing a solid electrolyte using a sonochemical process according to claim 10 , wherein the solid electrolyte raw material is dissolved in a polar organic solvent selected from a group consisting of an ester-based solvent, a carbonate-based solvent, an ether-based solvent, a furan-based solvent and a combination thereof.

13 . The continuous circulation reactor for preparing a solid electrolyte using a sonochemical process according to claim 10 , wherein the flow rate of the solid electrolyte raw material passing through the cross section of the reaction tube is 0.01-50 m/min.

14 . The continuous circulation reactor for preparing a solid electrolyte using a sonochemical process according to claim 10 , wherein the ultrasound irradiation means irradiates an ultrasound with a frequency of 20-2,000 kHz.

15 . The continuous circulation reactor for preparing a solid electrolyte using a sonochemical process according to claim 10 , which further comprises a temperature controller controlling the temperature of the reaction tube to −50° C. to 200° C.

16 . A method for preparing a solid electrolyte using a sonochemical process, which uses the continuous circulation reactor according to claim 10 , comprises:
allowing the solid electrolyte raw material held in the storage reservoir to pass through a first transport pipe, the circulation pump and the second transport pipe and to flow into the reaction tube of the ultrasound generator; reacting the solid electrolyte raw material by irradiating an ultrasound to the solid electrolyte raw material flowing in the reaction tube; and flowing the solid electrolyte raw material discharged from the reaction tube through the third transport pipe into the storage reservoir, wherein the steps are repeated.

17 . The method for preparing a solid electrolyte using a sonochemical process according to claim 16 , wherein the steps are repeated for 1 minute to 6 hours.

18 . The method for preparing a solid electrolyte using a sonochemical process according to claim 16 , which further comprises drying a product obtained by repeating the steps.

19 . The method for preparing a solid electrolyte using a sonochemical process according to claim 18 , which further comprises heat-treating the dried product at 250-800° C. for 1 minute to 100 hours.

20 . The method for preparing a solid electrolyte using a sonochemical process according to claim 16 , wherein the solid electrolyte has a shape selected from a group consisting of a sphere, a plate, a needle and a combination thereof.

Assignees

• Korea Inst Sci & Tech

Inventors

• Kim Hyoungchul
• Lee Hae-Weon
• Kim Byung Kook
• Lee Jong Ho
• Son Ji-Won
• Jung Hun-Gi
• Choi Sung Jun
• Jung Eu Deum

Classifications

• H01M2300/0068

  inorganic · CPC title

• H01M10/052 Primary

  Li-accumulators · CPC title

• C01B25/14

  Sulfur, selenium, or tellurium compounds of phosphorus · CPC title

• H01M10/0562 Primary

  Solid materials · CPC title

• H01M10/0585 Primary

  of accumulators having only flat construction elements, i.e. flat positive electrodes, flat negative electrodes and flat separators · CPC title