# US 12,113,220 B2 · Multi-layer negative electrode comprising natural graphite and artificial graphite and lithium secondary battery comprising the same > Agents: this data is available as JSON from the patentgrep API and MCP server — see https://patentgrep.com/llms.txt - Number: US 12,113,220 B2 - Document ID: US12113220B2 - Status: Granted - Kind: B2 - Application number: 17/850,570 - Filed: 2022-06-27 - Published: 2022-10-13 - Granted: 2024-10-08 - Earliest claimed: 2016-09-29 - Assignees: LG Energy Solution, Ltd. - Applicants: LG Energy Solution, Ltd. - Inventors: Taek Soo Lee; Chang Wan Koo; Sang Hoon Choi; Jung Min Yang; Il Jae Moon - Web page: https://patentgrep.com/patent/US12113220B2 ## CPC - H01M 4/587: for inserting or intercalating light metals - H01M 4/133: Electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx - H01M 4/364: {as mixtures} - H01M 4/366: {as layered products} - H01M 4/621: {Binders} - H01M 4/624: {Electric conductive fillers} - H01M 10/0525: Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries - H01M 2004/027: {Negative 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 - Y02E: REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION ## Abstract The present disclosure relates to a multilayer negative electrode comprising a negative electrode current collector configured to transfer electrons between an outer lead and a negative electrode active material, a first negative electrode mixture layer formed on one surface or both surfaces of the current collector and containing natural graphite as a negative electrode active material and a second negative electrode mixture layer formed on the first negative electrode mixture layer and containing artificial graphite as a negative electrode active material, and a lithium secondary battery including the same. ## Claims ### Claim 1 A multilayer negative electrode comprising: a negative electrode current collector configured to transfer electrons between an outer lead and a negative electrode active material; a first negative electrode mixture layer formed on one surface or both surfaces of the current collector and comprising natural graphite and artificial graphite as a negative electrode active material; and a second negative electrode mixture layer formed on the first negative electrode mixture layer and comprising a negative electrode active material consisting of artificial graphite, wherein an amount of the natural graphite present in the first negative electrode mixture layer is from 15% by weight to 75% by weight based on a total weight of the first negative electrode mixture layer, wherein a weight ratio of the first negative electrode mixture layer to the second negative electrode mixture layer is 1:9 to 5:5, and wherein an amount of the artificial graphite is greater than an amount of the natural graphite based on a total amount of the first negative electrode mixture layer and second negative electrode mixture layer. ### Claim 2 (depends on 1) The multilayer negative electrode of claim 1, wherein the natural graphite has a specific surface area (BET) of 2 m2/g to 8 m2/g. ### Claim 3 (depends on 2) The multilayer negative electrode of claim 2, wherein the weight ratio of the first negative electrode mixture layer to the total weight of the first negative electrode mixture layer and the second negative electrode mixture layer is decreased as the content of the natural graphite of the first negative electrode mixture layer is increased. ### Claim 4 (depends on 1) The multilayer negative electrode of claim 1, wherein the natural graphite is flake graphite, vein graphite, or amorphous graphite. ### Claim 5 (depends on 1) The multilayer negative electrode of claim 1, wherein the natural graphite has a tap density of 0.9 g/cc to 1.3 g/cc. ### Claim 6 (depends on 1) The multilayer negative electrode of claim 1, wherein a ratio of I110 to I003 of particles of the natural graphite at XRD diffraction is 20 to 40. ### Claim 7 (depends on 1) The multilayer negative electrode of claim 1, wherein the natural graphite has an average particle diameter (D50) of 5 μm to 30 μm. ### Claim 8 (depends on 1) The multilayer negative electrode of claim 1, wherein the artificial graphite is 0.5 m2/g to 5 m2/g in a range in which a specific surface area (BET) of the artificial graphite is smaller than that of the natural graphite. ### Claim 9 (depends on 1) The multilayer negative electrode of claim 1, wherein the artificial graphite is in a form of a powder, a flake, a block, a plate, or a rod. ### Claim 10 (depends on 1) The multilayer negative electrode of claim 1, wherein a ratio of I110 to I003 of particles of the artificial graphite at XRD diffraction is 5 to 20. ### Claim 11 (depends on 1) The multilayer negative electrode of claim 1, wherein at least one of the natural graphite and the artificial graphite is pitch-coated. ### Claim 12 (depends on 1) The multilayer negative electrode of claim 1, wherein some of solid contents of the first negative electrode mixture layer and the second negative electrode mixture layer is mixed therebetween so as not to form a boundary surface. ### Claim 13 (depends on 1) A lithium secondary battery comprising the multilayer negative electrode of claim 1. ### Claim 14 (depends on 1) The multilayer negative electrode of claim 1, wherein a weight ratio of natural graphite to artificial graphite in the first negative electrode mixture layer is from 4:6 to less than 1:1. ### Claim 15 (depends on 1) The multilayer negative electrode of claim 1, wherein a loading amount of the first negative electrode mixture layer ranges from 6 mg/cm2 to 8 mg/cm2. ### Claim 16 (depends on 1) The multilayer negative electrode of claim 1, wherein a loading amount of the second negative electrode mixture layer ranges from 8 mg/cm2 to 10 mg/cm2. ### Claim 17 (depends on 1) The multilayer negative electrode of claim 1, wherein the second negative electrode mixture layer is applied on the first negative electrode mixture layer before drying the first negative electrode mixture layer. ### Claim 18 A multilayer negative electrode comprising: a negative electrode current collector configured to transfer electrons between an outer lead and a negative electrode active material; a first negative electrode mixture layer formed on one surface or both surfaces of the current collector and comprising natural graphite and artificial graphite as a negative electrode active material; and a second negative electrode mixture layer formed on the first negative electrode mixture layer and comprising natural graphite and artificial graphite as a negative electrode active material, wherein an amount of the natural graphite present in the first negative electrode mixture layer is from 15% by weight to 75% by weight based on a total weight of the first negative electrode mixture layer, wherein an amount of the natural graphite present in the second negative electrode mixture layer is from 0.1% by weight to 10% by weight based on a total weight of the second negative electrode mixture layer, wherein a weight ratio of the first negative electrode mixture layer to the second negative electrode mixture layer is 1:9 to 5:5, wherein an amount of the artificial graphite is greater than an amount of the natural graphite based on a total amount of the first negative electrode mixture layer and second negative electrode mixture layer.