IP Library Granted Patent US 10,586,979
Granted Patent B2
US 10,586,979 · App. 15/771,498 · Granted Mar 10, 2020

Sulfur-carbon composite comprising a highly graphitic carbon material for lithium-sulfur batteries and process for preparing the same

Inventors: Yunhua Chen (Shanghai, CN); Juan Zhang (Beijing, CN); NaHong Zhao (Shanghai, CN); Yaxia Yin (Beijing, CN); Yuguo Guo (Beijing, CN)
Assignees: Robert Bosch GmbH; Institute of Chemistry, Chinese Academy of Sciences
H01M4/366C01B17/00C01B32/174C01B32/198C01B32/205H01M4/13H01M4/139H01M4/364H01M4/38H01M4/587H01M4/625C01P2002/01C01P2002/82C01P2006/16C01P2006/40H01M10/052H01M2004/021H01M2004/028
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Quick Facts
Patent No.
US 10,586,979
App. No.
15/771,498
Granted
Mar 10, 2020
Kind
B2
Abstract

Provided is a sulfur-carbon composite comprising a highly graphitic carbon material and sulfur, wherein the carbon material has a high graphitization degree characterized by a ratio of the intensity of G band to the intensity of D band in Raman spectrum being more than 1.0, the material is either a graphitic microporous carbon substrate, or a core-shell material with a conductive core coated by a graphitic microporous carbon layer, and wherein sulfur is encapsulated into the porous structure of the carbon material. Also provided are an electrode and a lithium-sulfur battery comprising the sulfur-carbon composite, and a process for preparing the sulfur-carbon composite.

Claims (17)

1. A process for preparing a sulfur-carbon composite, wherein the sulfur-carbon composite comprises a highly graphitic carbon material and sulfur, wherein the highly graphitic carbon material has a porous structure and a high graphitization degree characterized by a ratio of the intensity of G band to the intensity of D band in Raman spectrum being more than 1.0, said material being a core-shell material with a conductive core coated by a graphitic microporous carbon layer, and wherein sulfur is encapsulated into the porous structure of the highly graphitic carbon material,

the process comprising:

mixing an aqueous suspension of the conductive core with an aqueous solution of transition metal-containing salt, keeping at 60-120° C. for 2-12 h, carrying out a hydrothermal reaction by adding carbon source to the obtained product, followed by centrifuging, washing and drying; or alternatively, mixing an aqueous suspension of the conductive core with an aqueous solution of transition metal-containing salt and carbon source at the same time, then carrying out a hydrothermal reaction, followed by centrifuging, washing and drying,

pyrolyzing the obtained material at a temperature of 500-900° C. for 1-12 h;

removing the transition metal oxide by an acid solution; and

loading of sulfur.

2. A process for preparing a sulfur-carbon composite, wherein the sulfur-carbon composite comprises a highly graphitic carbon material and sulfur, wherein the highly graphitic carbon material has a porous structure and a high graphitization degree characterized by a ratio of the intensity of G band to the intensity of D band in Raman spectrum being more than 1.0, said material being a graphitic microporous carbon substrate, and wherein sulfur is encapsulated into the porous structure of the highly graphitic carbon material,

the process comprising the steps of:

dispersing microporous carbon substrate in an aqueous solution of transition metal-containing salt, stirring and heating at 60-120° C. for 2-12 h;

pyrolyzing the obtained material at a temperature of 500-900° C. for 1-12 h to carbonize and graphitize the microporous carbon substrate;

removing the transition metal oxide by an acid solution; and

loading of sulfur.

3. The process according to claim 1 , wherein said carbon source is one or more selected from the group consisting of sucrose, D-glucose, fructose, polyaniline, polyacetylene, polythiophene, dopamine and sodium alginate.

4. The process according to claim 1 , wherein the transition metal-containing salt is selected from the group consisting of chloride, sulfate, nitrate, acetate, carbonate and phosphate of Fe, Co and Ni.

5. The process according to claim 1 , wherein the sulfur loading comprises mixing homogeneously the carbon material obtained after removing the transition metal oxide with a solution of sulfur dissolved in a non-polar solvent by ultrasonication, and then adding a polar solvent to precipitate sulfur particles from the solution and deposite into the carbon material, followed by drying.

6. The process according to claim 2 , wherein the transition metal-containing salt is selected from the group consisting of chloride, sulfate, nitrate, acetate, carbonate and phosphate of Fe, Co and Ni.

7. The process according to claim 2 , wherein the sulfur loading comprises mixing homogeneously the carbon material obtained after removing the transition metal oxide with a solution of sulfur dissolved in a non-polar solvent by ultrasonication, and then adding a polar solvent to precipitate sulfur particles from the solution and deposite into the carbon material, followed by drying.

Assignments (1)
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Apr 27, 2018
From: CHEN, YUNHUA; ZHANG, JUAN; ZHAO, NAHONG; YIN, YAXIA; GUO, YUGUO
To: ROBERT BOSCH GMBH; INSTITUTE OF CHEMISTRY, CHINESE ACADEMY OF SCIENCES
Reel/Frame 045651/0975 →
Continuity (1)
Related Publication 20180351166A1 · Dec 6, 2018