Carbon-sulfur composite, preparation method therefor, and lithium secondary battery comprising same

Patent metadata

Field	Value
Publication number	US-12113206-B2
Application number	US-202318490351-A
Country	US
Kind code	B2
Filing date	Oct 19, 2023
Priority date	Sep 28, 2017
Publication date	Oct 8, 2024
Grant date	Oct 8, 2024

Abstract

A carbon-sulfur composite including a carbonized metal-organic framework (MOF); and a sulfur compound introduced to at least a part of an outside surface and an inside of the carbonized metal-organic framework, wherein the carbonized metal-organic framework has a specific surface area of 1000 m 2 /g to 1500 m 2 /g, and the carbonized metal-organic framework has a pore volume of 0.1 cc/g to 10 cc/g, and a method for preparing the same.

First claim

The invention claimed is:

1. A carbon-sulfur composite comprising:
a carbonized metal-organic framework; and
a sulfur compound introduced to at least a part of an outside surface and an inside of the carbonized metal-organic framework,
wherein the carbonized metal-organic framework has a specific surface area of 1000 m 2 /g to 1500 m 2 /g according to BET analysis, and
the carbonized metal-organic framework has a pore volume of 2.2 cc/g to 3.0, cc/g.

2. The carbon-sulfur composite of claim 1 , wherein the carbonized metal-organic framework has a specific surface area of 1000 m 2 /g.

3. The carbon-sulfur composite of claim 1 , wherein the carbonized metal-organic framework has a specific surface area of 1500 m 2 /g.

4. The carbon-sulfur composite of claim 1 , wherein the metal-organic framework (MOF) includes a structural unit represented by the following Chemical Formula 1:
[M x (L) y ]  [Chemical Formula 1]

in Chemical Formula 1,
M is one or more types of metals selected from the group consisting of copper (Cu), zinc (Zn), iron (Fe), nickel (Ni), chromium (Cr), scandium (Sc), cobalt (Co), titanium (Ti), manganese (Mn), vanadium (V), aluminum (Al), magnesium (Mg), gallium (Ga) and indium (In);
L is one or more types of organic metal ligands selected from the group consisting of 1,4-benzenedicarboxylate (BDC), 1,3,5-benzenetricarboxlate (BTC), 1,1′-biphenyl-3,3′,5,5′-tetracarboxylate (BPTC) and 2-(N,N,N′,N′-tetrakis(4-carboxyphenyl)-biphenyl-4,4′-diamine (TCBTDA); and
x is an integer of 2 to 6, and y is an integer of 2 to 12.

5. The carbon-sulfur composite of claim 1 , comprising the carbonized metal-organic framework (MOF) and the sulfur compound in a weight ratio of 9:1 to 1:9.

6. A method for preparing a carbon-sulfur composite according to claim 1 , comprising:
(a) preparing a carbonized metal-organic framework (MOF) by carbonizing a metal-organic framework (MOF) to 950° C. or higher; and
(b) preparing a carbon-sulfur composite by mixing the metal-organic framework (MOF) carbonized in (a) with a sulfur compound.

7. The method for preparing a carbon-sulfur composite of claim 6 , wherein, in (a), the metal-organic framework (MOF) is carbonized to 950° C. to 2,000° C.

8. The method for preparing a carbon-sulfur composite of claim 6 , wherein, in (a), the metal-organic framework (MOF) is carbonized to 950° C. to 1,500° C.

9. The method for preparing a carbon-sulfur composite of claim 6 , wherein, in (a), the carbonized metal-organic framework has a specific surface area of 1000 m 2 /g.

10. The method for preparing a carbon-sulfur composite of claim 6 , wherein the metal-organic framework (MOF) includes a structural unit represented by the following Chemical Formula 1:
[M x (L) y ]  [Chemical Formula 1]

in Chemical Formula 1,
M is one or more types of metals selected from the group consisting of copper (Cu), zinc (Zn), iron (Fe), nickel (Ni), chromium (Cr), scandium (Sc), cobalt (Co), titanium (Ti), manganese (Mn), vanadium (V), aluminum (Al), magnesium (Mg), gallium (Ga) and indium (In);
L is one or more types of organic metal ligands selected from the group consisting of 1,4-benzenedicarboxylate (BDC), 1,3,5-benzenetricarboxlate (BTC), 1,1′-biphenyl-3,3′,5,5′-tetracarboxylate (BPTC) and 2-(N,N,N′,N′-tetrakis(4-carboxyphenyl)-biphenyl-4,4′-diamine (TCBTDA); and
x is an integer of 2 to 6, and y is an integer of 2 to 12.

11. The method for preparing a carbon-sulfur composite of claim 6 , wherein, in (b), the carbonized metal-organic framework (MOF) and the sulfur compound are mixed in a weight ratio of 9:1 to 1:9.

12. A positive electrode comprising the carbon-sulfur composite of claim 1 .

13. The positive electrode of claim 12 , which is for a lithium-sulfur battery.

14. A lithium secondary battery comprising:
the positive electrode of claim 12 ;
a negative electrode; and
an electrolyte.

Assignees

• Lg Energy Solution Ltd
• Univ Yonsei Iacf

Inventors

• Cho Eunkyung
• Han Suenghoon
• Song Myeong Jun
• Kim Il To
• Sohn Kwonnam
• Yang Doo Kyung
• Kim Jiwon
• Shin Moo Whan

Classifications

• H01M2004/028

  Positive electrodes · CPC title

• H01M10/0525

  Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries · CPC title

• H01M4/60

  of organic compounds · CPC title

• H01M4/587

  for inserting or intercalating light metals · CPC title

• H01M4/38

  of elements or alloys · CPC title