Novel methods for sol-gel polymerization in absence of solvent and creation of tunable carbon structure from same
US-2020148886-A1 · May 14, 2020 · US
US11492260B2 · US · B2
| Field | Value |
|---|---|
| Publication number | US-11492260-B2 |
| Application number | US-201816628191-A |
| Country | US |
| Kind code | B2 |
| Filing date | Jul 4, 2018 |
| Priority date | Jul 6, 2017 |
| Publication date | Nov 8, 2022 |
| Grant date | Nov 8, 2022 |
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A problem to be solved by the present invention is to provide a carbonaceous material suitable for a negative electrode active material for non-aqueous electrolyte secondary batteries (e.g., lithium ion secondary batteries, sodium ion secondary batteries, lithium sulfur batteries, lithium air batteries) having high charge/discharge capacities and preferably high charge/discharge efficiency as well as low resistance, a negative electrode comprising the carbonaceous material, a non-aqueous electrolyte secondary battery comprising the negative electrode, and a production method of the carbonaceous material. The present invention relates to a carbonaceous material having a nitrogen element content of 1.0 mass % or more and an oxygen content of 1.5 mass % or less obtained by elemental analysis, a ratio of nitrogen element content and hydrogen element content (RN/H) of 6 or more and 100 or less, a ratio of oxygen element content and nitrogen element content (RO/N) of 0.1 or more and 1.0 or less, and a carbon interplanar spacing (d002) observed by X-ray diffraction measurement of 3.70 Å or more.
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The invention claimed is: 1. A carbonaceous material having a nitrogen content of 1.0 mass % or more and an oxygen content of 1.5 mass % or less as measured by elemental analysis, a ratio of the nitrogen content and a hydrogen content (R N/H ) of 6 or more and 100 or less, a ratio of the oxygen content and the nitrogen content (R O/N ) of 0.1 or more and 1.0 or less, and a carbon interplanar spacing (d 002 ) observed by X-ray diffraction measurement of 3.70 Å or more. 2. The carbonaceous material according to claim 1 , wherein a value of half-value width of a peak near 1360 cm −1 of a Raman spectrum observed by laser Raman spectroscopy is 190 to 270 cm −1 . 3. The carbonaceous material according to claim 1 , wherein a value of half-value width of a peak near 1360 cm −1 of a Raman spectrum observed by laser Raman spectroscopy is 190 to 250 cm −1 . 4. The carbonaceous material according to claim 1 , wherein a value of half-value width of a peak near 1650 cm −1 of a Raman spectrum observed by laser Raman spectroscopy is 100 cm −1 or less. 5. The carbonaceous material according to claim 1 , wherein a half-value width of a peak near 1650 cm −1 of a Raman spectrum observed by laser Raman spectroscopy exceeds 100 cm −1 . 6. The carbonaceous material according to claim 1 , wherein a specific surface area measured by a BET method is 40 m 2 /g or more, and wherein a pore volume represented by a sum of a micropore volume and a mesopore volume is 0.05 mL/g or more. 7. The carbonaceous material according to claim 1 , wherein a specific surface area measured by a BET method is 35 m 2 /g or less, and wherein a pore volume represented by a sum of a micropore volume and a mesopore volume is less than 0.05 mL/g. 8. The carbonaceous material according to claim 1 , wherein the carbonaceous material is derived from a saccharide. 9. A negative electrode active material for a non-aqueous electrolyte secondary battery, wherein the negative electrode active material comprises the carbonaceous material according to claim 1 . 10. A non-aqueous electrolyte secondary battery negative electrode comprising the carbonaceous material according to claim 9 . 11. A non-aqueous electrolyte secondary battery comprising the non-aqueous electrolyte secondary battery negative electrode according to claim 10 . 12. A method of producing the carbonaceous material according to claim 1 , the method comprising: (1) mixing a saccharide with a substance capable of generating ammonia gas to obtain a mixture; (2) increasing a temperature of the mixture in an inert gas atmosphere at a temperature increase rate of 100° C./hour or more to a first predetermined temperature between 500 and 1200° C.; (3) applying a heat treatment at a temperature of 500 to 1200° C. with an inert gas at a flow rate of 0.5 to 5.0 L/min relative to 5 g of the saccharide to obtain a char; (4) increasing a temperature of the obtained char in an inert gas atmosphere at a temperature increase rate of 100° C./hour or more to a second predetermined temperature between the first predetermined temperature and 1400° C.; and (5) applying a heat treatment at a temperature of 1000 to 1400° C. with an inert gas at a flow rate of 0.5 to 5.0 L/min relative to 5 g of the char. 13. The method according to claim 12 , wherein the first predetermined temperature is between 800 and 1100° C.
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