Classifications

• • H—ELECTRICITY
  • H01—ELECTRIC ELEMENTS
  • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
  • H01M10/00—Secondary cells; Manufacture thereof
  • H01M10/05—Accumulators with non-aqueous electrolyte
  • H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
  • H01M10/0561—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of inorganic materials only
  • H01M10/0562—Solid materials
• • H—ELECTRICITY
  • H01—ELECTRIC ELEMENTS
  • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
  • H01M10/00—Secondary cells; Manufacture thereof
  • H01M10/05—Accumulators with non-aqueous electrolyte
  • H01M10/052—Li-accumulators
  • H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
• • H—ELECTRICITY
  • H01—ELECTRIC ELEMENTS
  • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
  • H01M10/00—Secondary cells; Manufacture thereof
  • H01M10/05—Accumulators with non-aqueous electrolyte
  • H01M10/058—Construction or manufacture
  • H01M10/0585—Construction or manufacture of accumulators having only flat construction elements, i.e. flat positive electrodes, flat negative electrodes and flat separators
• • H—ELECTRICITY
  • H01—ELECTRIC ELEMENTS
  • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
  • H01M10/00—Secondary cells; Manufacture thereof
  • H01M10/42—Methods or arrangements for servicing or maintenance of secondary cells or secondary half-cells
  • H01M10/4235—Safety or regulating additives or arrangements in electrodes, separators or electrolyte
• • H—ELECTRICITY
  • H01—ELECTRIC ELEMENTS
  • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
  • H01M4/00—Electrodes
  • H01M4/02—Electrodes composed of, or comprising, active material
  • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
  • H01M4/131—Electrodes based on mixed oxides or hydroxides, or on mixtures of oxides or hydroxides, e.g. LiCoOx
• • H—ELECTRICITY
  • H01—ELECTRIC ELEMENTS
  • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
  • H01M4/00—Electrodes
  • H01M4/02—Electrodes composed of, or comprising, active material
  • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
  • H01M4/134—Electrodes based on metals, Si or alloys
• • H—ELECTRICITY
  • H01—ELECTRIC ELEMENTS
  • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
  • H01M4/00—Electrodes
  • H01M4/02—Electrodes composed of, or comprising, active material
  • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
  • H01M4/139—Processes of manufacture
  • H01M4/1395—Processes of manufacture of electrodes based on metals, Si or alloys
• • H—ELECTRICITY
  • H01—ELECTRIC ELEMENTS
  • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
  • H01M4/00—Electrodes
  • H01M4/02—Electrodes composed of, or comprising, active material
  • H01M4/36—Selection of substances as active materials, active masses, active liquids
  • H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
  • H01M4/386—Silicon or alloys based on silicon
• • H—ELECTRICITY
  • H01—ELECTRIC ELEMENTS
  • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
  • H01M4/00—Electrodes
  • H01M4/02—Electrodes composed of, or comprising, active material
  • H01M4/64—Carriers or collectors
  • H01M4/66—Selection of materials
  • H01M4/661—Metal or alloys, e.g. alloy coatings
• • H—ELECTRICITY
  • H01—ELECTRIC ELEMENTS
  • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
  • H01M4/00—Electrodes
  • H01M4/02—Electrodes composed of, or comprising, active material
  • H01M2004/021—Physical characteristics, e.g. porosity, surface area
• • H—ELECTRICITY
  • H01—ELECTRIC ELEMENTS
  • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
  • H01M4/00—Electrodes
  • H01M4/02—Electrodes composed of, or comprising, active material
  • H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
  • H01M2004/027—Negative electrodes
• • H—ELECTRICITY
  • H01—ELECTRIC ELEMENTS
  • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
  • H01M4/00—Electrodes
  • H01M4/02—Electrodes composed of, or comprising, active material
  • H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
  • H01M2004/028—Positive electrodes
• • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
  • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
  • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
  • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
  • Y02E60/10—Energy storage using batteries
• • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
  • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
  • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
  • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
  • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

Definitions

• the invention relates to a method for producing a planar silicon anode-solid electrolyte compound which is suitable for use in a solid-state battery and a planar silicon anode-solid electrolyte compound produced in this way.
• the invention also relates to a solid-state battery cell that includes a cathode and the planar silicon-anode-solid electrolyte compound according to the invention, as well as a solid-state battery that includes at least one solid-state battery cell.
• Batteries are electrochemical energy storage devices and are divided into primary and secondary batteries.
• Primary batteries are electrochemical power sources in which chemical energy is irreversibly converted into electrical energy. A primary battery is therefore not rechargeable. Secondary batteries, also called accumulators, on the other hand, are rechargeable electrochemical energy storage devices in which the chemical reaction that occurs is reversible, so that multiple use is possible. When charging, electrical energy is converted into chemical energy, and during discharging it is converted from chemical energy into electrical energy.
• Battery is the generic term for cells connected together.
• Cells are galvanic units consisting of two electrodes, electrolytes, separator and cell housing.
• Figure 1 shows an exemplary structure and the function of a lithium-ion cell during the discharging process.
• Each Li-ion cell consists of two different electrodes 7, 9, an electrode 9 that is negatively charged in the charged state and an electrode 7 that is positively charged in the charged state. Since during energy release, i.e. during discharge, ions migrate from the negatively charged electrode to the positively charged electrode, the positively charged electrode is called cathode 7 and the negatively charged electrode is called anode 9.
• the electrodes are each composed of a current collector 2, 8 (also called a collector) and an active material applied to it. Between the electrodes there is, on the one hand, the ion-conducting electrolyte 4, which enables the necessary charge exchange, and the separator 5, which ensures the electrical separation of the electrodes.
• Solid-state accumulators or batteries differ from conventional accumulators in particular because of the solid electrolyte.
• the job of the electrolyte is to conduct ions between the anode and cathode.
• Battery cells can be connected together in different ways. If you connect two battery cells in series, the anode (negative electrode) of one battery cell is connected to the cathode (positive electrode) of the other (consideration during the discharging process). When battery cells are connected in series, the total voltage increases: the voltages of the individual cells are added together. If you connect battery cells in parallel, all cathodes (positive electrodes) are connected to each other and all anodes (negative electrodes) - consideration during discharge. In the Connecting cells in parallel doubles the capacity (Ah) of the battery. The same applies to the parallel connection of batteries to battery modules.
• a liquid electrolyte is used to utilize lithium between the electrodes (anode and cathode) to store and release energy. Since water-based electrolytes only have a small potential window for stable operation, organic solvents are used. These have a high flame potential and increase the risk of the batteries catching fire.
• the use of solid electrolytes, which have significantly lower flammability, is seen as a solution.
• the solid electrolyte can replace the previous liquid electrolyte and separator with the properties of good ionic conductivity combined with good electrical insulation.
• the volume and weight are reduced due to increased energy density, especially when using metallic lithium, which means that the packing density can be significantly increased.
• the disadvantage of solid electrolytes is their low flexibility and the difficult contact with the anode and cathode for good ion conductivity.
• the surface contact between the anode and the solid electrolyte is crucial.
• the limited ionic contact at the interface between cathode-electrolyte or Electrolyte anode massively reduces the performance of the battery.
• Lithium metal also forms at high Surface currents with ceramic solid electrolyte dendrites, which can destroy the battery.
• lithium reacts with the solid electrolyte on the surface, so that the ionic conductivity decreases during operation.
• Argyrodites are lithium-rich solid-state compounds.
• the argyrodite family consists of more than 100 crystalline solids and extends, for example, to those solid-state compounds in which the silver is replaced by copper, the germanium by gallium or phosphorus and the sulfur by selenium.
• high pressing pressures are also used, which are particularly necessary when volume expands during battery operation in order to ensure consistent contact.
• the high pressure required for this requires a lot of effort for a commercial setup.
• a multilayer structure is deposited on a porous solid electrolyte as the active layer of the Si anode in a dry deposition process, whereby the Multilayer structure is subjected to short-term tempering and a current collector, preferably made of copper, is deposited on the multilayer structure.
• a porous solid electrolyte is a layer of sintered powder. The powder is formed from ceramics that are pressed into a layer and heated.
• a multilayer structure is understood to mean a layer structure that consists of two or more layers, but the term multilayer structure also includes a single layer within the scope of the disclosure of this invention.
• the method according to the invention is particularly suitable for the production of battery cells for a wide variety of battery applications because it enables a complete and planar solid electrolyte-silicon anode structure in particulate form with additives to stabilize the multilayer structure of the active layer of the anode.
• dry manufacturing processes such as sputtering or electron beam evaporation
• both a multilayer structure can be deposited planarly on the solid electrolyte directly as the active layer of the anode and an additional intermediate layer can be applied without additional effort to stabilize the solid electrolyte-anode interface.
• short-term annealing the energy input into the layers can be specifically controlled.
• an intermediate layer for stabilization is deposited between the solid electrolyte and the multilayer structure between the solid electrolyte and the active layer of the Si anode.
• Silicon anode solid electrolyte connection in reverse Sequence to previously known methods. This makes it possible to place the anode directly on the solid electrolyte, so that optimal ionic contact with the solid electrolyte, which is normally difficult to contact, can be achieved.
• the current collector on the anode side can be optimized so that it no longer has to fulfill a supporting function. This means that the material thickness of the copper current collector can be reduced to the current density actually required in the application and thus the weight and layer thickness, without the thermal waste heat having a negative influence. As a result, a significant reduction in weight and thus an increase in the gravimetric energy density can be achieved.
• the multilayer structure is therefore deposited in layers, with the multilayer structure being formed from at least one layer made of a metal and/or silicon or formed from a mixed system which consists of silicon mixed with at least one metal.
• the multilayer structure is formed from at least one layer.
• a layer is understood to mean a deposited layer of active material of the anode, whereby, depending on the layer thickness, the active layer of the electrode/anode can be made up of one or more layers.
• the at least one layer can be formed from at least one metal and/or silicon. The silicon and the at least one metal are applied alternately through a separate layer deposition of the materials.
• a layer is thus formed from at least one layer of at least one metal and one layer of silicon, with several layers being formed in the multilayer structure in order to achieve the target thickness of the anode.
• the at least one layer can also be formed by a mixing system, the mixing system consisting of silicon mixed with at least one metal. This mixture of at least one metal and silicon, usually in powder form, is deposited to the target thickness of the active layer.
• the metal is made from at least one of the materials manganese (Mn), cobalt (Co), iron (Fe), titanium (Ti), nickel (Ni), aluminum (Al), tin (Sn), gold (Au) and / or silver (Ag) or a mixture of these materials.
• the dry deposition process is a PVD process, for example sputtering.
• Preferred methods are sputtering and electron beam evaporation.
• CVD processes Chemical Vapor Deposition
• PECVD Plasma Enhanced CVD
• PVD processes Physical Vapor Deposition
• thermal evaporation or the PLD process (Pulsed Laser Deposition) are also possible.
• an energy input into the deposited layers of the multilayer structure and / or layers of the Si anode-solid electrolyte compound or solid-state battery cell and / or solid-state battery is controlled by means of short-term annealing.
• the planar structure of the Si anode-solid electrolyte connection according to the invention can take place in the order shown above: solid electrolyte-active layer-current collector, as well as in the reverse order starting with Current collector followed by the active layer of the anode and the construction of a solid electrolyte with further processes or PVD process. Since the contact between the solid electrolyte-anode interface is particularly crucial for battery performance, only a thin layer is sufficient to create a stable contact. By means of short-term annealing, the necessary crystallinity or ion conductivity can be produced in the solid electrolyte.
• the process steps for the production of the planar silicon anode-solid electrolyte connection are carried out in the reverse order in such a way that the multilayer structure acts as an active layer on the current collector of the Si anode, preferably copper, in a dry Deposition process is deposited, which is then subjected to a short-term tempering with a controlled and adjustable energy input into the multilayer structure of the Si anode, an intermediate layer is deposited on the multilayer structure for stabilization between the solid electrolyte and the active layer of the Si anode and the solid f electrolyte is deposited, which is subjected to short-term tempering to crystallize the solid electrolyte.
• the short-term annealing is a flash lamp annealing and is carried out by means of a flash lamp with a flash duration in the range of 0.2 to 20 ms and an energy density in the range of 0.3 to 160 J/cm 2 as well as preheating or cooling in the range Can be carried out from 4 ° C to 200 ° C .
• the short-term annealing is a laser annealing and is carried out by means of a laser with an annealing time in the range from 0.01 to 100 ms by setting a scanning speed of a local heating point and an energy density in the range from 0.1 to 100J/cm 2 as well as with preheating or cooling in the range from 4°C to 200°C.
• the temperature range from 4°C to 200°C this refers to the surface temperature of the substrate or the layer to be tempered.
• Ti silicide is formed, which can be Li-storable in the right phase (see: Xu, J. et al. Preparation of TiSi2 Powders with Enhanced Lithium-Ion Storage via Chemical Oven Self-Propagating High-Temperature Synthesis . Nanomaterials 11, 2279 (2021) ) .
• This has the advantage that there is no clear Li-active-inactive interface exists and therefore good electrical contact also exists during cycling.
• Other metals such as aluminum do not form a compound with silicon, i.e. no silicides. The consequence is that these metals mix in silicon and the electrical conductivity is increased.
• the short-term annealing step the morphology and hardness of the silicon-metal layer can also improve compared to the hard pure silicon.
• the heating ramps achieved in the short-term tempering are in the range of 10 4 - 10 7 K/s required for the process.
• Flash lamp annealing uses a spectrum in the visible wavelength range, whereas laser annealing uses discrete wavelengths in the infrared (IR) to ultraviolet (UV) spectrum.
• the solid electrolyte preferably consists of an oxidic material, in particular garnet structure oxides, NAS ICON-type phosphate glass ceramics any oxynitrides.
• garnet structure oxides belong to the island silicates, such as the widely studied lithium lanthanum zirconium oxide (LLZO).
• NASICON-type phosphate glass ceramics get their name from the chemical structure of NaZr2 (PO4) and have a high ionic conductivity for lithium ions. Examples include LAGP (lithium aluminum germanium phosphate) and LATP (lithium aluminum titanium phosphate).
• Oxynitrides are oxides that create many defects in the lattice by replacing some oxygen atoms with nitrogen, which creates high ionic conductivity, for example xLi20: yP2Os: zPON, LiPON for short. LiPON can be produced by sputtering Li 3 PO4 in reactive N2 plasma.
• the Si anode solid electrolyte compound according to the invention has a solid electrolyte which is made from oxidic materials, in particular from garnet structure oxides, e.g. B. LLZO, NASICON-type phosphate glass ceramics, e.g. B. LATP or LAGP and oxynitrides, e.g. B. LiPON.
• oxidic materials for good ionic conductivity, require a high degree of crystallinity, which requires a high process temperature.
• the process temperatures are in the range of room temperature for LiPON sputtered layers, up to 1230°C for sufficiently crystalline sintered LLZO ceramics and around 700°C for the glass transition temperature of NASICON ceramics.
• the oxidic materials mentioned are particularly suitable for use in an ASSB because they have an ionic conductivity of over ImS/cm (milli-Siemens per centimeter) and are thermally and chemically very stable.
• the solid electrolyte has a crystallinity with high ionic conductivity, which can be specifically adjusted using short-term tempering.
• the short-term tempering enables the construction of the planar Si anode solid electrolyte compound according to the invention.
• the flat contact enables good ionic conductivity between the active layer of the Si anode and the solid electrolyte.
• the artificial SEI as an intermediate layer between the Si anode and the solid electrolyte can further improve the contact between the two layers. Otherwise, poor contact between the Si anode and the solid electrolyte would be characterized by degradation of the surface of the solid electrolyte, especially in the case of Li metal anodes.
• the object of the invention is also achieved by a solid-state battery cell which comprises a cathode and a planar silicon-anode-solid electrolyte compound which is produced using the method according to claims 1 to 9, wherein the Si anode, the solid f electrolyte and the cathode are designed to be planar.
• the production of a complete solid-state battery cell or Solid-state battery in a planar deposition process together with the solid electrolyte is particularly advantageous because the planar structure enables both the production of a solid electrolyte on a planar Si anode and the application of a Si anode and a copper current conductor directly on the solid f makes electrolytes feasible.
• a Active layer is formed as a cathode made of LiFePCy, LiMnO2 or LiCoO2 and a current collector, preferably made of aluminum, is formed on the active layer as a cathode.
• anode-side structure which includes the Si anode-solid electrolyte connection, a Si-anode-copper current collector connection and a cathode-side structure which includes a solid electrolyte-cathode-aluminum current collector connection and / or a catholyte-aluminum current collector connection, which can be produced and constructed separately from one another, wherein the Si-anode-solid electrolyte connection, the Si-anode-copper current collector connection and the solid electrolyte-cathode-aluminum Current collector connection and / or the catholyte-aluminum current collector connection are designed to be connectable to one another in a final manufacturing step via a respective bulk contact.
• the method according to the invention makes it possible for the first time to realize the production sequence of the layers of a complete solid-state battery cell in different production sequences. All parts of the solid-state battery cell can also be manufactured separately from one another, with the special feature that the transition contacts are already fully formed.
• a transition contact is understood to mean, for example, the interface between the Si anode and the solid electrolyte. Therefore, only materials of the same design need to be joined together.
• the planar structure it is possible for the first time, thanks to the planar structure, to apply the active layer of the Si anode directly to a solid electrolyte and then deposit the copper current collector or first to deposit the planar active layer on the Cu current collector and then the solid f electrolytes.
• the cathode-side structure methods already exist to couple the solid electrolyte and the cathode to one another, i.e. H .
• the layer compositions i.e. Si anode-solid electrolyte and/or Cu current collector-Si anode and/or solid electrolyte-cathode-aluminum current collector, can now be manufactured separately from one another to simplify production, for which Manufacturing or When forming the solid-state battery cell, these layer compositions are connected/connected to one another via their respective bulk contacts.
• Si anode is used in the connection between the layer compositions.
• Solid electrolyte and Cu current collector-Si anode understood the coupling of the active layer parts or in the connection between the layer compositions Si anode solid electrolyte and solid electrolyte cathode aluminum current collector is under the bulk contact the coupling understood via the solid electrolyte. If necessary, the coupling can be supported by a temperature step.
• the object of the invention is also achieved by a solid-state battery which consists of more than one solid-state battery cell, the more than one solid-state battery cell being applied and stacked in a planar manner on one another using the manufacturing methods provided.
• the contacting can be designed to be connected to one another in parallel and/or in series.
• Fig. 1 Exemplary structure and function of a lithium-ion cell with liquid electrolyte during the discharging process (state of the art);
• Fig. 2 Sequence of the production process according to the invention for a Si anode solid electrolyte compound a) in the order: solid electrolyte anode; b) in the order: current collector-active layer-solid electrolyte;
• Fig. 3 Structure of a solid-state battery cell or further layers produced according to the invention Process by stacking battery cell components;
• FIG. 4 Schematic representation of a solid-state battery cell with material examples for the individual layers
• FIG. 5 Schematic representation of a further production variant for a solid-state battery cell according to the method according to the invention for producing a Si anode-solid material electrolyte compound
• Fig. 6 Structure of a solid-state battery consisting of several solid-state battery cells connected in parallel and manufactured in one process.
• the method according to the invention is suitable for realizing a stable anode structure in order to either apply an anode structure 9 to the solid electrolyte 11 (FIG. 2a) or to apply a solid electrolyte to a current collector 2 with an active layer 9, which together form an anode 9 11 (Fig. 2b).
• the short-term annealing in particular the flash lamp annealing, can subsequently be used to crystallize the position of the solid electrolyte through a targeted energy input without significantly damaging the anode (according to FIG. 2b).
• the method according to the invention advantageously enables the silicon anode-solid electrolyte compound 10 to be processed in two directions to carry out.
• Either a multilayer structure 9 is deposited on a solid electrolyte 11 as the active layer of the anode in a dry process and then the current collector 2 is deposited (Fig. 2a) or on a current collector 2 the multilayer structure 9 is first deposited for the active layer of the anode and then the solid f electrolyte 11 is deposited (FIG. 2b), i.e. in the reverse order.
• the layers or Layers are stabilized by short-term tempering. This means that the solid-state electrolyte can be produced separately from the anode production.
• the Si anode is deposited in the manufacturing process from at least one layer made of a metal and/or silicon or from a mixed system which consists of silicon mixed with at least one metal, particulate with additional layers.
• the direct application of the anode 9 to the solid electrolyte 11 enables optimal ionic contact with the solid electrolyte 11, which is normally difficult to contact.
• the necessary process parameters and annealing processes using flash lamp annealing should only have a negligible influence on the existing solid electrolyte 11.
• a current collector 2 with a suitable layer thickness can be applied to the “solid electrolyte and Si anode” structure.
• the current collector 2 can be optimized on the anode side in the process with regard to electrical conductivity, layer thickness (e.g. 3 ⁇ m) and weight, since it does not have to fulfill a load-bearing function.
• a flat contact is required to attach a current lead necessary, which can be realized, for example, by rolling a suitable thick arrester flag onto the anode 9 directly or onto the anode 9, prepared with a flat metal deposit to reduce resistance.
• the subsequent new deposition of a Si anode 9 can still be implemented independently of the substrate 2.
• any stack of a battery (FIG. 6) can be constructed from several cells 14. This means that the capacity of a solid-state battery 15 can also be easily realized. be set.
• This stacking of anode 9 / solid electrolyte 11 / cathode 7 allows a highly integrated approach to the construction of all-solid-state batteries.
• the intermediate layer 16 between anode 9 and solid electrolyte 11 serves for interface engineering and allows the anode 9 to be specifically applied to the solid electrolyte 11 without additional effort.
• FIG. 5 shows a production variant for a solid-state battery cell 14 according to the method according to the invention for producing a Si anode-solid electrolyte compound 10.
• both the Si-anode-solid electrolyte connection 10 and the Si-anode-copper current collector connection 20 and the solid electrolyte-cathode-aluminum current collector connection and/or catholyte-aluminum current collector - Connection 19 made separately from each other.
• the separately produced layer compositions tongues 10, 20, 19 are connected to one another via their respective bulk contacts.
• a bulk contact is understood to mean, for example, the active layer 9 in the connection between Si anode-solid electrolyte 10 and Cu current collector-Si anode 20 and in the connection between the Si anode-solid electrolyte 10 and the solid electrolyte -Cathode-aluminum current collector 19 is understood as the bulk contact of the solid electrolyte 11.
• a catholyte 17 is understood to mean the mixture of the cathode 7 with the solid electrolyte 11.
• the invention makes it possible to realize the production sequence of the layers of a solid-state battery cell in different production sequences. Parts of the solid-state battery cell with a defined interface can also be manufactured separately from one another and then easily connected to one another in a final process.
• the stack of layers shown in Figure 6 for a solid-state battery 15 can be produced either according to a first variant of the production process for a silicon anode-solid electrolyte compound 10, in which the active layer 9 and the current collector 2 of the anode are on the solid f electrolytes 11 are applied, or according to a second variant of the manufacturing process for a silicon anode-solid electrolyte compound 10, in which an active layer 9 as an anode and then the solid f electrolyte 11 are applied to a current collector 2, or a combination of both variants.
• Solid electrolyte 11 allows stacking in one single process instead of, as before, in several systems or concepts. This opens up new possibilities for increasing performance by specifically influencing the interfaces. The number of production facilities is reduced.
• a stack of individual solid-state battery cells 14, as shown in FIG. 6 is necessary to realize sufficient total capacity for a solid-state battery 15.
• this was not possible because there was no reversible production to build a Si anode-solid electrolyte connection 10 starting from a solid electrolyte 11. This is only made possible by the planar structure of the solid electrolyte 11 and the planar anode, the short-term tempering and the use of dry deposition processes.

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• 2023
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