METHOD FOR PRODUCING A CATHODE FOR A RECHARGEABLE LITHIUM-ION BATTERY

Abstract

Method for producing a cathode for a rechargeable lithium-ion battery with the components polymer structure, aluminum foil, lithium sulfide particles and carbon particles (CB), wherein the polymer structure alternates (AB) nis formed from monomers A and B via an imine linkage, and wherein the polymer structure has an aromatic or heteroaromatic branching core and an aromatic or heteroaromatic bridge, and wherein the aromatic or heteroaromatic branching core is formed from the monomeric unit of monomer A and the aromatic or heteroaromatic bridge is formed from the monomeric unit of monomer B, and wherein the monomers A have at least three amine end groups and at least one aromatic or heteroaromatic ring, and wherein the monomers B have at least two aldehyde or keto end groups and at least one aromatic or heteroaromatic ring, comprising the following steps: i. Overcoating and / or undercoating the aluminum foil with a suspension of monomer A, monomer B, lithium sulfide powder and carbon particles (CB) in one or more solvents (mixture 1); ii. Allowing the mixture 1 to react at temperatures between 20 °C and 120 °C for times between 5 min and 1 h in a one-pot reaction; iii. Removal and drying of the cathode material; iv. Cutting the cathode material to the desired size using a punch.

Description

[0001] The invention relates to a method for producing a cathode for a rechargeable lithium-ion battery.

[0002] Rechargeable batteries basically consist of an electrolyte, a cathode, and an anode. One advantage of rechargeable lithium-ion batteries is that they can be operated in any orientation, making them suitable for mobile and consumer electronics applications. These applications in particular require small and lightweight batteries with high performance (specific output capacity, energy density, and capacity retention over charging cycles).

[0003] There is a need to improve the performance of rechargeable lithium-ion batteries while maintaining good mechanical stability and without reducing the number of possible charge and discharge cycles.

[0004] DE 10 2013 018 350 A1 describes the production of polymer-lithium sulfite-carbon composites, which are proposed for use as cathode material in lithium batteries.

[0005] In Meng et al.'s "Impregnation of sulfur into a 2D pyrene-based covalent organic framework for high-rate lithium-sulfur batteries," J. Mater. Chem. A. 2018, 6, 17186, a cathode for a rechargeable lithium-ion battery is proposed. The cathode is composed of sulfur and an imine-linked pyrene-based 2D polymer structure. To prepare the cathode, a polymer structure is first generated by condensing an amine monomer (1,3,6,8-tetrakis(4-aminophenyl)pyrene (PyTTA)) and an aldehyde monomer (terephthaldehyde (TA)), and then mixed with sulfur in a second step.

[0006] A disadvantage of the cathodes currently known is that the composition of the cathode is not very chemically and physically resistant, and quickly loses its performance as a result of operation because the active components are only mixed together and are not connected by strong covalent chemical bonds of the polymer structure.

[0007] DE 10 2019 110 450 B3 describes an anode for a rechargeable lithium-ion battery and a method for its production. The anodes exhibit high lithiation capacity and excellent durability because, during the anode production process, the polymer structure is (i) generated in situ from monomers, (ii) grown around the active material, and (iii) grown on the metallic current collector (aluminum). This achieves a particularly advantageous bond between all components and with the current collector.

[0008] DE 10 2012 109 641 A1 discloses a process for producing an active material for batteries, comprising introducing electrochemically active particles, optionally comminuting the electrochemically active particles, adding an organic carbon compound, optionally in a suitable organic solvent, and mixing and heating the mixture under a protective gas to a temperature above the decomposition limit of the organic compound and below the decomposition temperature of the electrochemically active particles. Active materials produced in this way, as well as corresponding applications and uses, are also described.

[0009] CN 111 682 207 A discloses a heteroatom-containing covalent organic framework electrode material, as well as a manufacturing method and application thereof. The electrode material is a composite electrode material prepared by applying a nitrogen heteroatom-containing two-dimensional covalent organic imino framework material to the surface of a carbon nanotube and subsequent mechanical stripping.

[0010] Furthermore, DE 10 2019 110 450 B3 discloses an anode for a rechargeable lithium-ion battery comprising the components polymer structure, copper foil, and silicon nanoparticles, wherein the polymer structure is formed from a monomer and wherein the polymer structure consists of a 1,3,5-triazine core (1) and a bridge acting as an electron donor, and wherein the bridge contains at least one aromatic or heteroaromatic member. Furthermore, the invention relates to a manufacturing method for an anode comprising the steps of over- and / or under-coating the copper foil with a suspension of silicon nanoparticles and monomer in a weight ratio of 3:1 in solvent (mixture 1), reacting the mixture 1 at 20°C to 120°C for 12 to 96 hours in a one-pot reaction, removing, washing, and drying the anode material, and cutting the anode material to the desired size using a punch.

[0011] US 2022 0 223 917 A1 describes an electrolyte comprising: (a) a polymer that is a polymerization or crosslinking product of a reactive additive, wherein the reactive additive comprises at least one reactive polymer, reactive oligomer, or reactive monomer and a curing agent or initiator, and wherein the reactive polymer, oligomer, or monomer comprises at least one reactive carboxyl and / or hydroxyl group; (b) a lithium salt; and (c) an organic liquid solvent or an ionic liquid. The polymer preferably comprises a crosslinked network of chains of poly(acrylic acid), poly(vinyl alcohol), polyethylene glycol, carboxymethylcellulose, or a combination thereof. Furthermore, a lithium battery containing such an electrolyte is provided.

[0012] Furthermore, in Wang et al.'s "An imine-linked covalent organic framework as the host material for sulfur loading in lithium-sulfur batteries," J. Energy Chem. 2017, 28, 54, an imine-linked TAPB (1,3,5-tris(aminophenyl)benzene)-PDA (terephthaldehyde)-COF is used as a host material for sulfur loading (60%) in Li-S batteries. The TAPB-PDA-COF has a spike-like morphology with high thermal stability (up to 500 °C). In the electrochemical experiment, the performance of the composite cathode is investigated separately using acetylene black and Super-P as conductive additives.

[0013] It is an object of the invention to provide a method for producing a cathode for a rechargeable lithium-ion battery which, even after undergoing several charge and discharge cycles at discharge rates between C / 8 and 2C, has a lithiation capacity of at least 400 mAh g -1 has.

[0014] The object of the invention is achieved by a method for producing a cathode for a rechargeable lithium-ion battery with the components polymer structure, aluminum foil, lithium sulfide particles and carbon particles (CB), wherein the polymer structure is alternately (AB) nis formed from the monomers A and B via an imine linkage and wherein the polymer structure has an aromatic or heteroaromatic branching core and an aromatic or heteroaromatic bridge and wherein the aromatic or heteroaromatic branching core is formed from the monomeric unit of the monomer A and the aromatic or heteroaromatic bridge is formed from the monomeric unit of the monomer B and wherein the monomers A have at least three amine end groups and at least one aromatic or heteroaromatic ring and wherein the monomers B have at least two aldehyde or keto end groups and at least one aromatic or heteroaromatic ring, comprising the following steps i. Overcoating and / or undercoating the aluminum foil with a suspension of monomer A, monomer B, lithium sulfide powder and carbon particles (CB) in one or more solvents (mixture 1), ii. Allowing the mixture 1 to react at temperatures between 20 °C and 120 °C for times between 5 min and 1 h in a one-pot reaction, iii. Removal and drying of the cathode material iv. Cutting the cathode material to the desired size using a punch.

[0015] Optionally, the cut cathodes can be subjected to a heat treatment at 300 °C for several hours in a further process step.

[0016] In a particular embodiment of the process, the cathodes obtained after step iv or v are treated with dried hydrogen sulphide gas (H2S) in a further process step.

[0017] In a further particular embodiment of the process according to the invention for producing a cathode for a rechargeable lithium-ion battery, the provision of mixture 1 (step i) comprises the following steps a. Monomer A is dissolved in one or more solvents (mixture 1a) b. Addition of a lithium sulfite-carbon composite (Li2S / CB) (mixture 1b) c. Homogenization of mixture 1b d. Addition of monomer B (mixture 1d) e. Stirring mixture 1d f. Bringing the mixture 1d into contact with the aluminum foil by overlaying and / or underlaying

[0018] In an alternative, particular embodiment of the process according to the invention for producing a cathode for a rechargeable lithium-ion battery, the provision of mixture 1 (step i) comprises the following steps g. Monomer A is dissolved in solvent g (mixture 1g) h. Addition of Li2S and mechanical homogenization of the mixture (mixture 1h) i. Addition of carbon particles (CB) to the homogeneous mixture 1h and mechanical homogenization of the mixture (mixture 1i) j. Dispersing mixture 1i (mixture 1j) k. Drying of mixture 1j to remove solvent g (mixture 1k) I. Bringing the mixture 1k into contact with the aluminum foil by overlaying and / or underlaying

[0019] Polar, aprotic organic solvents are suitable as solvents. The solvents are preferably selected from the group consisting of N-methyl-2-pyrrolidone (NMP), N,N-dimethylformamide (DMF), pyridine, dimethyl ether (DME), and 1,3-dioxolane (DOL). Solvent g can be selected from the group consisting of anhydrous, dried primary, secondary, and tertiary alcohols with a carbon chain length of 1 to 6 (methanol, ethanol, propanol, isopropanol, butanol, isobutanol, pentanol, isopentanol, hexanol, and isohexanol).

[0020] Homogenization (steps c, h and i) can be carried out by stirring, shaking, ball milling or ultrasound.

[0021] Dispersal (step j.) can be carried out by stirring, shaking, ball milling or ultrasound.

[0022] In a preferred embodiment of the process, the 100% complementary weight ratios of the components monomer A and monomer B / lithium sulfide powder / carbon (CB) are in the percentage range of 20 (+ / -10):48 (+ / -20):32 (+ / -31).

[0023] In another aspect, the cathode for a rechargeable lithium-ion battery may comprise the components: - Polymer structure - aluminum foil - Lithium sulfide particles - Carbon particles (CB)where the polymer structure is alternating (AB) nis formed from the monomers A and B via an imine linkage and wherein the polymer structure has an aromatic or heteroaromatic branching core and an aromatic or heteroaromatic bridge and wherein the aromatic or heteroaromatic branching core is formed from the monomeric unit of the monomer A and the aromatic or heteroaromatic bridge is formed from the monomeric unit of the monomer B and wherein the monomers A have at least three amine end groups and at least one aromatic or heteroaromatic ring and wherein the monomers B have at least two aldehyde or keto end groups and at least one aromatic or heteroaromatic ring.

[0024] In a particular embodiment, the monomers A are selected from the group 1,3,5-tris(4-aminophenyl)benzene (TAPB), 2,4,6-tris(4-aminophenyl)-1,3,5-triazine (TAPT), tris(4-aminophenyl)amine (TAPA), 5,10,15,20-tetrakis(4-aminophenyl)porphyrin (T4APP), 1,2,4,5-tetraaminobenzene tetrahydrochloride (T4AB)

[0025] In a further particular embodiment, the monomers B are selected from the group of terephthalaldehyde (TA), benzene-1,3,5-tricarbaldehyde (TAB), 2,5-thiophenedicarboxaldehyde (TDCA), 2,2'-bithiophene-5,5'-dicarboxaldehyde 98% (BTDCA), thieno[3,2-b]thiophene-2,5-dicarboxaldehyde (TTDCA), 2,5-dihydroxyterephthalaldehyde 95% (DHTA), cyclohexanehexone octahydrate (CHHO)

[0026] In a preferred embodiment of the cathode produced according to the invention, the 100% complementary weight ratios of the components monomer A and monomer B / lithium sulfide powder / carbon (CB) are in the percentage range of 20 (+ / -10):48 (+ / -20):32 (+ / -31).

[0027] For example, industrially processed meter-length aluminum foil can be used.

[0028] The lithium sulfide powder can be purchased, for example, as commercial bulk material (purity 99.9%, e.g. from Alfa Aeser Fisher Scientific GmbH (Germany)).

[0029] Carbon particles in the form of conductive carbon black powder (carbon black) (CB), for example, can be purchased as commercial bulk material.

[0030] In Fig. is an example of a polymer structure that alternates (AB) n formed from the monomers A =TAPB and B=TA via an imine linkage (1).

[0031] In this case, the aromatic branching core from the monomeric unit of monomer A (TAPB) and the aromatic bridge from the monomeric unit of monomer B (TA) can be seen.

[0032] In Fig. is an example of a polymer structure that alternates (AB) n formed from the monomers A =TAPB and B=TDCA via an imine linkage.

[0033] In this case, the aromatic branching core from the monomeric unit of monomer A (TAPB) and the heteroaromatic bridge from the monomeric unit of monomer B (TDCA) can be seen.

[0034] Without limiting the generality of the teaching, the following describes the production and performance of the cathode produced according to the invention. Materials used:

[0035] Terephthalaldehyde 99% (TA), 2,5-thiophenedicarboxaldehyde 99% (TDCA), melamine 99% (MA), 1,2,4,5-tetraaminobenzene tetrahydrochloride technical grade (T4AB), cyclohexanehexone octahydrate 97% (CHHO), and tris(4-aminophenyl)amine 97% (TAPA) were purchased from Sigma-Aldrich Chemie GmbH (Germany). 1,3,5-Tris(4-aminophenyl)benzene 93% (TAPB), 2,4,6-tris(4-aminophenyl)-1,3,5-triazine 98% (TAPT), 5,10,15,20-tetrakis(4-aminophenyl)porphyrin 95% (T4APP), benzene-1,3,5-tricarbaldehyde 98% (TAB), 2,2'-bithiophene-5,5'-dicarboxaldehyde 98% (BTDCA), and thieno[3,2-b]thiophene-2,5-dicarboxaldehyde 93% (TTDCA) were purchased from TCI Deutschland GmbH (Germany). 2,5-Dihydroxyterephthalaldehyde 95% (DHTA) was purchased from abcr GmbH (Germany). Before use, TDCA, BTDCA, TTDCA, and TA were dried for 12 hours under vacuum at 60 °C; TAPB, TAPT, MA, T4APP, TAB, and CHHO were dried for 12 hours under vacuum at 80 °C; DHTA was dried for 12 hours under vacuum at RTdried; T4AB was dried at 180 °C for 12 hours to remove possible traces of water and oxygen and stored under an inert atmosphere.

[0036] Lithium bis(trifluoromethane)sulfonimide 99.95% (LiTFSI) and lithium nitrate 99% (LiNO3) were purchased from Sigma-Aldrich Chemie GmbH (Germany). Conductive carbon black (CB) powder (TIMCAL Super C65) was purchased from MTI Corporation (USA). These solids were dried under vacuum at 120 °C for 12 hours before use. Lithium sulfide 99.9% (Li2S, 200 mesh powder) was purchased from Fisher Scientific GmbH (Germany). Aluminum foil measuring 430 mm × 600 mm × 0.03 mm was purchased from VWR International GmbH (Germany).

[0037] Anhydrous N-methylpyrrolidone 99.5% (NMP) and anhydrous N,N-dimethylformamide 99.8% (DMF), anhydrous 1,3-dioxolane 98% (DOL), and anhydrous 1,2-dimethoxyethane 99% (DME) were purchased from Sigma-Aldrich Chemie GmbH (Germany). Before use, all these solvents were purged with argon to remove oxygen, and molecular scavengers were added to capture any traces of water. 1 Preparation of the imine-COF / Li2S / CB electrodes according to method 11.1 Preparation of the Li2S / CB composites

[0038] All processes described below are carried out under an inert atmosphere (H2O ≤ 1 ppm, O2 ≤ 1 ppm). Composites with different compositions were prepared by mixing Li2S with CB by ball milling (PULVERISETTE 7 planetary mill) for different times at different speeds using zirconia cups and balls under an argon atmosphere. For each ball milling, 0.7 g of the mixed powder was used; the ratio of this powder to the zirconia balls was 1:14. The different compositions of Li2S and CB used to prepare the composites were 9:1, 8:2, 7:3, 6:4, and 5:5. The milling processes were operated at speeds of 400 rpm, 600 rpm, and 800 rpm. Different milling times were used to prepare the Li2S / CB composite material, namely 4 hours, 6 hours, 8 hours and 10 hours. 1.2 Processing of the imine COF / Li2S / CB electrodes according to Method 1

[0039] Each preparation of the imine-COF Li2S / CB electrodes involves the combination of an amino-based monomer with an aldehyde-based monomer to create a covalent organic imine framework used as an electrode binder. The first preparation step consists of dissolving the amino-based monomer in 150 µL of NMP and 150 µL of DMF (the masses used for each amino-based monomer are given in Table 1, and the mass of the ketone CHHO is given in Table 2) under stirring, followed by the addition of 100 mg of Li2S / CB composite. NMP is used to disperse the composite material, while DMF is used to dissolve the amino-based monomer. The solution is then homogenized by ultrasonication for 15 min. After complete dispersion of the composite material in the solution, the aldehyde-based monomer of the ketone-based monomer is added and the mixture is stirred for 1 min.The mixture is poured directly onto a 300 µm thick aluminum foil using a doctor blade. The preparation is then heated to 120 °C for 2 hours. After cooling the preparation, which consists of an electrode film deposited on aluminum foil, to room temperature, discs with a diameter of 1.8 cm are punched. The discs can be subjected to heat treatment at 300 °C for 20 hours.

[0040] The method is particularly suitable for preparations with TAPB, TAPT and MA as amino-based monomers and TA, TDCA, BTDCA, TTDCA and DHTA 2 Preparation of the imine-COF / Li2S / CB electrodes according to method 2

[0041] Similar to Method 1, each preparation of the imine-COF Li2S / CB electrodes involves combining an amino-based monomer with an aldehyde-based monomer to create a covalent organic imine framework used as an electrode binder. Method 2 here does not involve composite materials prepared by ball milling but starts with pristine Li2S and CB. The first step of the preparation consists of dissolving the amino-based monomer (weight ratios between the amino-based monomers and the aldehyde-based monomers are listed in Table 1; weight ratios between the amino-based monomers and the ketone-based monomers are listed in Table 2) in 4 mL of anhydrous EtOH, followed by the addition of 60 mg of Li2S. Once these two components are dissolved, 40 mg of CB is added to the solution. The solution is then treated in a sonic bath for 10 min to allow proper dispersion of the CB.The solution is dried at 120 °C to remove all EtOH. This step enables the formation of nanoscopic Li2S domains due to the steric effect of the amino-based monomer. The resulting powder is then dispersed in 150 µL of NMP and 150 µL of DMF, followed by the addition of the aldehyde-based monomer or the ketone-based monomer. The mixture is cast directly onto an aluminum foil using a doctor blade to a thickness of 300 µm. The preparation is then heated at 120 °C for 2 hours. After cooling the mixture to room temperature, a sample consisting of an electrode film deposited on an aluminum foil is prepared.

[0042] Discs with a diameter of 1.8 cm are punched. The discs are subjected to heat treatment at 300 °C for 20 hours if necessary. H2S treatment of the IMIN-COF / LI2S / CB electrodes

[0043] To improve the performance of the sample for battery testing, the discs can be subjected to H2S treatment. For this purpose, the discs are placed in a 100 ml Schlenk tube under vacuum. Meanwhile, a 100 ml Schlenk tube is filled with H2S gas at atmospheric pressure. The H2S-filled Schlenk tube is then connected to one side of a drying column containing phosphorus(V) oxide to remove any traces of water. The other side of the drying column is connected to the vacuum-operated Schlenk tube containing the H2S-treated electrode discs. The H2S gas is then introduced into the vacuum-operated Schlenk tube containing the electrode discs. Once the H2S gas has been introduced into the Schlenk tube containing the electrode discs, the Schlenk tube is sealed and allowed to react for 20 hours, then degassed. Electrochemical measurements

[0044] The electrochemical properties of the samples were determined using coin cells. Circular discs made of Whatman membranes (fiberglass, grade GF / D, Whatman, USA) were used as separators. Metallic lithium discs served as counter and reference electrodes. The electrolyte composition used for the electrochemical testing of the samples was 1 M LiTFSI in DOL / DME = 1:1 (v / v) with or without the presence of 1 wt% LiNO3. The coin cells were compressed using a mechanical press at 70 kg cm². -2 sealed. All GCPL experiments were evaluated on a CT2001A Battery Analyzer (Wuhan LAND Electronics Co., Ltd., China). S-cathodes were tested in constant current mode in a voltage range of 3-1.7 V vs. Li / Li + tested. For S-cathodes, the current densities are based on the weighted mass of S (1C = 1675 mA g -1 ) is calculated. Li2S cathodes were tested in constant current mode in a voltage range of 3-1.6 V vs. Li / Li +tested, except for the first charge, where the cut-off voltage was 3.6 V vs. Li / Li + For Li2S cathodes, the current densities are based on the weighted mass of Li2S (1C = 1166 mA g -1 ) calculated.

[0045] Fig. shows the capacity retention of a cathode produced according to the invention with a polymer structure of TAPB (monomer A) and TDCA (monomer B) prepared according to Method 1 (imine-COF / Li2S / CB). The mass ratio of the produced electrode consisting of Li2S, CB, and the polymer is 48:32:20. More than 50 charge and discharge cycles were performed at a discharge rate of C / 8. The specific capacity remains stable above 400 mAh / g.

[0046] Fig. shows the corresponding galvanostatic plot of the cathode produced according to the invention with a polymer structure made of TAPB (monomer A) and TDCA (monomer B) prepared according to Method 1 (imine-COF / Li2S / CB). The mass ratio of the produced electrode made of Li2S, CB, and the polymer is 48:32:20.

[0047] Fig. shows the capacity retention of the cathode produced according to the invention with a polymer structure of TAPB (monomer A) and TDCA (monomer B) prepared according to Method 1 (imine-COF / Li2S / CB). The mass ratio of the produced electrode consisting of Li2S, CB, and the polymer is 48:32:20. The cathode was additionally treated with H2S. More than 50 charge and discharge cycles were performed at a discharge rate of C / 8. The specific capacity remains stable above 700 mAh / g.

[0048] Fig. shows the corresponding galvanostatic plot of the cathode produced according to the invention with a polymer structure of TAPB (monomer A) and TDCA (monomer B) prepared according to Method 1 (imine-COF / Li2S / CB). The cathode was additionally treated with H2S. The mass ratio of the produced electrode consisting of Li2S, CB, and the polymer is 48:32:20. The discharge rate was C / 8.

[0049] Fig. shows the capacity retention of a cathode produced according to the invention with a polymer structure of TAPB (monomer A) and TDCA (monomer B) prepared according to Method 2 (imine-COF / Li2S / CB). The mass ratio of the produced electrode consisting of Li2S, CB, and the polymer is 48:32:20. More than 50 charge and discharge cycles were performed at a discharge rate of C / 8. The specific capacity remains stable above 600 mAh / g.

[0050] Fig. shows the galvanostatic plot of a cathode produced according to the invention with a polymer structure of TAPB (monomer A) and TDCA (monomer B) prepared according to method 2 (imine-COF / Li2S / CB). The cathode was additionally treated with H2S. The mass ratio of the produced electrode consisting of Li2S, CB, and the polymer is 48:32:20. The discharge rate was C / 8.

[0051] To demonstrate the performance and durability of the cathode produced according to the invention, measurements were compared with commercially available cathodes. The results are presented below.

[0052] Four commercial cathodes, including NCM811 (Ningbo Ronbay New Energy Technology Co., Ltd., China), NCM532 (Targray Technology International Inc., Canada), NCM622 (Nantong Ruixiang New Material Co., Ltd., China), and NCA (Beiterui Inc., China), were investigated by fabricating cathode films with the same parameters. Of the four commercial cathodes, the NCM811 cathode exhibited the highest and most stable specific capacity (128 to 163 mA hg). -1 ), and was used for comparison purposes.

[0053] The active cathode material used was Li[Ni 0.8 Co 0.1 Mn 0.1]O2 (NCM811, Grade S800C, Ningbo Ronbay New Energy Technology Co., Ltd., China) was used. NCM811, poly(vinylidene difluoride) (PVdF, Alfa Aesar), and carbon black (carbon) in N-methylpyrrolidone (NMP, Sigma-Aldrich, anhydrous 99.5%) were mixed by ball milling (PULVERISETTE 7 planetary mill) for 2 hours at 250 rpm using zirconia cups and beads. The final mass ratio of NCM811 / PVdF / CB was 94.5:2.5:3. The slurry was spread with a razor blade onto an Al foil with a thickness of 200 µm to 250 µm and left in a glove box at room temperature overnight to allow the NMP to evaporate. The NCM811 preparation was punched into discs with a diameter of 18 mm and then dried in a glass chamber under vacuum at 120 °C for 8 h to remove possible traces of moisture and oxygen, and then transferred to a glove box under argon atmosphere (H2O ≤ 1 ppm, O2 ≤ 1 ppm).

[0054] Fig. shows half-cell performance data showing the specific capacities / CE as a function of the number of cycles at C / 2 with initial five cycles at C / 8 for NCM811 electrodes within the potential window of 3.0-4.2 V vs. Li / Li+.

[0055] Compared to the cathodes produced according to the invention, the specific capacity is significantly lower at less than 200 mAh / g! List of figures: Fig. : Polymer structure alternating (AB) n formed from the monomers A =TAPB and B=TA via an imine linkage (1) Fig. : Polymer structure alternating (AB) n formed from the monomers A =TAPB and B=TDCA via an imine linkage (1) Fig. : Capacity of a cathode prepared according to the invention with a polymer structure of TAPB (monomer A) and TDCA (monomer B) prepared according to Method 1 (imine-COF / Li2S / CB). The mass ratio of the prepared electrode consisting of Li2S, CB, and the polymer is 48:32:20. Fig. : Galvanostatic plot of the cathode prepared according to the invention with a polymer structure of TAPB (monomer A) and TDCA (monomer B) prepared according to Method 1 (imine-COF / Li2S / CB). The mass ratio of the prepared electrode consisting of Li2S, CB, and the polymer is 48:32:20. Fig. : Capacity of a cathode prepared according to the invention with a polymer structure of TAPB (monomer A) and TDCA (monomer B) prepared according to Method 1 (imine-COF / Li2S / CB). The mass ratio of the prepared electrode consisting of Li2S, CB, and the polymer is 48:32:20. The cathode was also treated with H2S. Fig. : Galvanostatic plot of the cathode prepared according to the invention with a polymer structure of TAPB (monomer A) and TDCA (monomer B) prepared according to Method 1 (imine-COF / Li2S / CB). The cathode was additionally treated with H2S. The mass ratio of the prepared electrode consisting of Li2S, CB, and the polymer is 48:32:20. The discharge rate was C / 8. Fig. : Capacity retention of a cathode prepared according to the invention with a polymer structure of TAPB (monomer A) and TDCA (monomer B) prepared according to Method 2 (imine-COF / Li2S / CB). The mass ratio of the prepared electrode consisting of Li2S, CB, and the polymer is 48:32:20. More than 50 charge and discharge cycles were performed at a discharge rate of C / 8. Fig. : Galvanostatic plot of a cathode prepared according to the invention with a polymer structure of TAPB (monomer A) and TDCA (monomer B) prepared according to Method 2 (imine-COF / Li2S / CB). The cathode was additionally treated with H2S. The mass ratio of the prepared electrode consisting of Li2S, CB, and the polymer is 48:32:20. The discharge rate was C / 8. Fig. : Half-cell performance data of a commercially available cathode at C / 2 with initial five cycles at C / 8 for NCM811 electrodes within the potential window of 3.0-4.2 V vs. Li / Li+. List of reference symbols: 1 Imine linkage

Claims

[1] Method for producing a cathode for a rechargeable lithium-ion battery with the components polymer structure, aluminum foil, lithium sulfide particles and carbon particles (CB), wherein the polymer structure alternates (AB) nis formed from monomers A and B via an imine linkage, and wherein the polymer structure has an aromatic or heteroaromatic branching core and an aromatic or heteroaromatic bridge, and wherein the aromatic or heteroaromatic branching core is formed from the monomeric unit of monomer A and the aromatic or heteroaromatic bridge is formed from the monomeric unit of monomer B, and wherein the monomers A have at least three amine end groups and at least one aromatic or heteroaromatic ring, and wherein the monomers B have at least two aldehyde or keto end groups and at least one aromatic or heteroaromatic ring, comprising the following steps: i. Overcoating and / or undercoating the aluminum foil with a suspension of monomer A, monomer B, lithium sulfide powder and carbon particles (CB) in one or more solvents (mixture 1); ii. Allowing the mixture 1 to react at temperatures between 20 °C and 120 °C for times between 5 min and 1 h in a one-pot reaction; iii. Removal and drying of the cathode material; iv. Cutting the cathode material to the desired size using a punch. [2] Method according to claim 1, characterized by that the cut cathodes are subjected to a further heat treatment at 300 °C for several hours in a further process step. [3] Method according to claim 1 or 2, characterized by that the cathodes are treated with dried hydrogen sulfide gas (H2S) in a further process step. [4] Method according to one or more of the preceding claims, characterized by that the provision of Mixture 1 (step i) comprises the following steps: a. Monomer A is dissolved in one or more solvents (mixture 1a) b. Addition of a lithium sulfite-carbon composite (Li2S / CB) (mixture 1b) c. Homogenization of mixture 1b d. Addition of monomer B (mixture 1d) e. Stirring mixture 1d f. Bringing the mixture 1d into contact with the aluminum foil by overlaying and / or underlaying [5] Method according to one or more of the preceding claims 1 to 3, characterized by that the provision of Mixture 1 (step i) comprises the following steps: g. Monomer A is dissolved in solvent g (mixture 1g) h. Addition of Li2S and mechanical homogenization of the mixture (mixture 1h) i. Addition of carbon particles (CB) to the homogeneous mixture 1h and mechanical homogenization of the mixture (mixture 1i) j. Dispersing mixture 1i (mixture 1j) k. Drying of mixture 1j to remove solvent g (mixture 1k) I. Bringing mixture 1k into contact with the aluminum foil by overlayering and / or underlayering. [6] Method according to one or more of the preceding claims, characterized by that the weight ratios of the components monomer A and monomer B / lithium sulfide powder / carbon (CB) which add up to 100 are in the range 20 (+ / -10):48 (+ / -20):32 (+ / -31).

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