# US 12,113,206 B2 · Carbon-sulfur composite, preparation method therefor, and lithium secondary battery comprising same

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- Number: US 12,113,206 B2
- Document ID: US12113206B2
- Status: Granted
- Kind: B2
- Application number: 18/490,351
- Filed: 2023-10-19
- Published: 2024-02-08
- Granted: 2024-10-08
- Earliest claimed: 2017-09-28
- Assignees: LG Energy Solution, Ltd.; Industry-Academic Cooperation Foundation, Yonsei University
- Applicants: LG Energy Solution, Ltd.; Industry-Academic Cooperation Foundation, Yonsei University
- Inventors: Eunkyung Cho; Suenghoon Han; Myeong Jun Song; Il To Kim; Kwonnam Sohn; Doo Kyung Yang; Jiwon Kim; Moo Whan Shin
- Web page: https://patentgrep.com/patent/US12113206B2

## CPC

- H01M 4/13: Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M 4/364: {as mixtures}
- C01B 17/02: Preparation of sulfur; Purification
- C01B 32/05: Preparation or purification of carbon not covered by groups C01B32/15, C01B32/20, C01B32/25, C01B32/30
- H01M 4/139: Processes of manufacture
- H01M 4/38: of elements or alloys
- H01M 4/587: for inserting or intercalating light metals
- H01M 4/60: of organic compounds
- H01M 4/663: {containing carbon or carbonaceous materials as conductive part, e.g. graphite, carbon fibres}
- H01M 4/666: {in the form of mixed materials (H01M4/668 takes precedence)}
- H01M 10/0525: Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
- C01B 32/00: Carbon; Compounds thereof (C01B21/00, C01B23/00 take precedence; percarbonates C01B15/10; carbon black C09C1/48)
- C01P 2004/03: obtained by SEM
- C01P 2006/12: Surface area
- C01P 2006/14: Pore volume
- C01P 2006/40: Electric properties
- H01M 2004/028: {Positive electrodes}
- Y02E 60/10: Energy storage using batteries
- H01M: PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- C01B: NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; {METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C}
- C01P: INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
- Y02E: REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION

## 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 m2/g to 1500 m2/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.

## Claims

### Claim 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 m2/g to 1500 m2/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.

### Claim 2 (depends on 1)

The carbon-sulfur composite of claim 1, wherein the carbonized metal-organic framework has a specific surface area of 1000 m2/g.

### Claim 3 (depends on 1)

The carbon-sulfur composite of claim 1, wherein the carbonized metal-organic framework has a specific surface area of 1500 m2/g.

### Claim 4 (depends on 1)

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

### Claim 5 (depends on 1)

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.

### Claim 6 (depends on 1)

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.

### Claim 7 (depends on 6)

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.

### Claim 8 (depends on 6)

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.

### Claim 9 (depends on 6)

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 m2/g.

### Claim 10 (depends on 6)

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:
[Mx(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.

### Claim 11 (depends on 6)

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.

### Claim 12 (depends on 1)

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

### Claim 13 (depends on 12)

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

### Claim 14 (depends on 12)

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