Separation membrane coating agent composition, separation membrane made from coating agent composition, and battery using same

Patent metadata

Field	Value
Publication number	US-10050247-B2
Application number	US-201314418849-A
Country	US
Kind code	B2
Filing date	Jul 31, 2013
Priority date	Aug 1, 2012
Publication date	Aug 14, 2018
Grant date	Aug 14, 2018

Abstract

Disclosed herein is a coating composition having excellent thermal resistance and drying processability, utilizing polyamic acid having high thermal resistance and excellent solubility in a low boiling point solvent. Specifically, the coating composition includes polyamic acid and a low boiling point solvent having a boiling point less than 150° C. Also, disclosed herein a separator having improved thermal resistance by coating the coating composition on one or both surfaces of a polyolefin-based substrate film, and an electrochemical battery having improved thermal stability by using the separator.

First claim

The invention claimed is:

1. A composition for coating a separator, the composition comprising:
a polyamic acid having a weight average molecular weight (Mw) of 50,000 to 130,000;
a solvent having a boiling point less than 150° C.; and
inorganic particles, the inorganic particles being present in the composition in a greater weight than the polyamic acid, wherein:
the polyamic acid is represented by one of the following Chemical Formula 5 to 7:

wherein x is an integer of 30 to 10,000 in Chemical Formula 5,

wherein x and y are an integer of 15 to 5,000, respectively, in Chemical Formula 6,

wherein x and y are an integer of 15 to 5,000, respectively, in Chemical Formula 7.

2. The composition as claimed in claim 1 , wherein the solvent having a boiling point less than 150° C. is acetone.

3. The composition as claimed in claim 1 , further comprising a solvent having a boiling point of 150° C. or more, wherein:
a weight ratio of the solvent having a boiling point less than 150° C. : the solvent having a boiling point of 150° C. or more is 9:1 to 6:4,
a ratio x:y is 1:9 to 5:5 in Chemical Formula 6,
a ratio x:y is 1:9 to 5:5 in Chemical Formula 7, and
the polyamic acid is not imidized but is present in the form of the polyamic acid.

4. The composition as claimed in 3 , wherein the solvent having a boiling point of 150° C. or more includes one or more of dimethylformamide, dimethylsulfoxide, dimethylacetamide, dimethylcarbonate or N-methylpyrrolidone.

5. A separator, comprising:
a polyolefin-containing substrate film; and
a coating layer on at least one surface of the substrate film, wherein:
the coating layer includes a polyamic acid having a weight average molecular weight (Mw) of 50,000 to 130,000 and inorganic particles, the inorganic particles being present in the coating layer in a greater weight than the polyamic acid,
the coating layer has an organic solvent residual amount of 500 ppm or less therein, and
the polyamic acid is represented by one of the following Chemical Formula 5 to 7:

wherein x is an integer of 30 to 10,000 in Chemical Formula 5,

wherein x and y are an integer of 15 to 5,000, respectively, in Chemical Formula 6,

wherein x and y are an integer of 15 to 5,000, respectively, in Chemical Formula 7.

6. The separator as claimed in claim 5 , wherein the organic solvent has a boiling point higher than the melting point of the substrate film.

7. The separator as claimed in claim 5 , wherein the separator has thermal shrinkage of 20% or less in a machine direction and a transverse direction, respectively, after being left at 200° C. for 1 hour.

8. The separator as claimed in claim 5 , wherein the separator has thermal shrinkage of 5% or less in a machine direction and a transverse direction, respectively, after being left at 200° C. for 1 hour.

9. A method of preparing a coated separator, the method comprising:
applying a coating composition containing a polyamic acid having a weight average molecular weight (Mw) of 50,000 to 130,000, inorganic particles in a greater weight than the polyamic acid, a solvent having a boiling point less than 150° C., and a solvent having a boiling point of 150° C. or more on at least one surface of a polyolefin-containing substrate film, and
drying the applied coating composition to form a coating layer, wherein:
the polyamic acid is represented by one of the following Chemical Formula 5 to 7:

wherein x is an integer of 30 to 10,000 in Chemical Formula 5,

wherein x and y are an integer of 15 to 5,000, respectively, in Chemical Formula 6,

wherein x and y are an integer of 15 to 5,000, respectively, in Chemical Formula 7.

10. The method as claimed in claim 9 , wherein, after the drying, a residual amount of solvent in the coating layer is 500 ppm or less.

11. An electrochemical battery, comprising:
a cathode, an anode, the separator as claimed in claim 5 , and an electrolyte.

12. The electrochemical battery as claimed in claim 11 , wherein the electrochemical battery is a lithium secondary battery.

13. The composition as claimed in claim 1 , wherein each of the sulfone groups in the Chemical Formulae 5 to 7 is a substituent in an ortho-, meta- or para- position to an amine group.

14. The separator as claimed in claim 5 , wherein:
a ratio x:y in Chemical Formula 6 is 1:9 to 5:5,
a ratio x:y is 1:9 to 5:5 in Chemical Formula 7, and
the polyamic acid is not imidized in the coating layer but is present in the form of the polyamic acid.

15. The method as claimed in claim 9 , wherein:
a weight ratio of the solvent having a boiling point less than 150° C. : the solvent having a boiling point of 150° C. or more is 9:1 to 6:4,
a residual amount of the first and the second solvent in the coating layer is 500 ppm or less, and
the polyamic acid is not imidized in the coating layer but is present in the form of the polyamic acid.

Assignees

• Samsung Sdi Co Ltd

Inventors

• Jeon In Sik
• Park Jin Kyu
• Chung Jun Ho
• Hong Ki Chul
• Lim Geon Ja

Classifications

• C09D179/08 Primary

  Polyimides; Polyester-imides; Polyamide-imides; Polyamide acids or similar polyimide precursors · CPC title

• H01M50/423

  Polyamide resins · CPC title

• H01M50/417 Primary

  Polyolefins · CPC title

• H01M50/449

  having a layered structure · CPC title

• C08K5/20

  Carboxylic acid amides · CPC title