Process and system for mechanochemical synthesis of a solid electrolyte, solid electrolyte, and uses thereof

Abstract

The invention relates to a process and a system for mechanochemical synthesis of a solid electrolyte. The process comprises continuously feeding a homogeneous reactant mixture, which is suitable for producing a solid electrolyte, to a device for continuous mechanical stressing, and continuously mechanically stressing the homogeneous reactant mixture in said device such that the homogeneous reactant mixture is continuously converted into a solid electrolyte by means of a chemical reaction caused by the continuous mechanical stressing. The system is configured to carry out the process according to the invention.

Description

[0001] Fraunhofer Society...eV

[0002] P149360PC00

[0003] Method and apparatus for the mechanochemical synthesis of a solid electrolyte, solid electrolyte and uses thereof

[0004] A method and a plant for the mechanochemical synthesis 5 of a solid electrolyte are provided. The method comprises the continuous feeding of a homogeneous reactant mixture suitable for the production of a solid electrolyte into a device for continuous mechanical stress and the continuous mechanical stressing of the homogeneous reactant mixture in said device, such that the solid reactant mixture is continuously converted into a solid electrolyte via a chemical reaction induced by the continuous mechanical stress. The plant is configured to carry out the method according to the invention. Novel materials, such as a solid electrolyte, are required for the production of new generations of energy storage devices (e.g., batteries, solid-state batteries, fuel cells, etc.).

[0005] It is known in the art to produce solid electrolytes using wet chemical processes, particularly on a larger scale, employing organic solvents. The disadvantage of these processes is that the organic solvents used are expensive, can be toxic, pose an environmental hazard, and must be removed from the product, i.e., the solid electrolyte. This makes carrying out these known processes complex and costly, and the risk of toxicity to personnel and the environment cannot be ruled out.

[0006] Based on this, the object of the present invention was to provide a method and a plant for the large-scale production of a solid electrolyte that overcomes at least one disadvantage of the prior art. In particular, the method and plant should make it possible to produce a solid electrolyte in a simpler and more cost-effective manner, minimizing risks to personnel and the environment and achieving the highest possible product yield per unit of time. Furthermore, a solid electrolyte with improved properties should be provided, and its uses should be specified.

[0007] The problem is solved by the method with the features of claim 1, the system with the features of claim 10, the solid electrolyte with the features of claim 19, and the use with the features of claim 23. The dependent claims describe advantageous embodiments.

[0008] According to the invention, a method for the mechanochemical synthesis of a solid electrolyte is provided, comprising the following steps: a) Continuously feeding a homogeneous reactant mixture suitable for the production of a solid electrolyte to a device for continuous mechanical stressing; and b) Continuously mechanically stressing the homogeneous reactant mixture in the device for continuous mechanical stressing, such that the homogeneous reactant mixture is continuously converted into a solid electrolyte via a chemical reaction induced by the continuous mechanical stressing.

[0009] The inventive method makes it possible to produce a solid electrolyte in a simpler and more cost-effective manner, minimizing the risk to personnel and the environment and achieving a very high product yield per unit of time.

[0010] The process is simpler (i.e., less complex) than known methods because it is a mechanochemical process. This means that no organic solvents are added to the reactant mixture, or at most, they are added as an additive in a proportion of no more than 0.1% by volume, relative to the total volume of the reactant mixture. Therefore, no or only a minimal amount of organic solvents needs to be removed from the resulting solid electrolyte at the end of the process. This also results in a higher product quality of the solid electrolyte; that is, the produced solid electrolyte contains fewer impurities caused by the presence of organic solvents in the manufacturing process and exhibits higher ionic conductivity.An additional advantage is that the process according to the invention can be carried out more cost-effectively and with a minimized risk to personnel and the environment than wet chemical processes, since no or only negligible amounts of organic solvents are used in the process.

[0011] Since the process according to the invention comprises or consists of continuously performed steps, the product yield per unit time is very high, which contributes to the process being more economical than known wet chemical processes whose steps are carried out as batch processes. Furthermore, the continuously performed process steps of the process according to the invention make it easy to scale up, which can further increase the product yield per unit time. The process can include providing the homogeneous reactant mixture from step a) by (preferably continuously) mixing reactants suitable for producing a solid electrolyte and supplying the provided homogeneous reactant mixture to the device for the continuous (preferably continuous) feeding of a reactant mixture.

[0012] The reactants can be mixed in a stoichiometric ratio and / or already be present in the homogeneous reactant mixture in step a) of the process, which is required to produce a specific solid electrolyte. This measure prevents unnecessary raw material consumption and makes the process more economical. Furthermore, it ensures that the produced solid electrolyte is free of reactant impurities.

[0013] Furthermore, the reactants and / or the reactant mixture present in step a) of the process may contain at least one alkali metal, wherein the alkali metal is preferably selected from the group consisting of lithium, sodium and combinations thereof.

[0014] Furthermore, the reactants and / or the reactant mixture present in step a) of the process may contain phosphorus.

[0015] Furthermore, the reactants and / or the reactant mixture present in step a) of the process may contain sulfur. The advantage is that a sulfide solid electrolyte can be produced.

[0016] Apart from this, the reactants and / or the reactant mixture present in step a) of the process may contain at least one halogen, wherein the at least one halogen is preferably selected from the group consisting of chlorine, bromine, iodine and combinations thereof.

[0017] Furthermore, the reactants and / or the reactant mixture present in step a) of the process may contain an alkali metal intercalating material, wherein the alkali metal intercalating material is preferably a lithium intercalating material, wherein the lithium intercalating material is particularly preferably selected from the group consisting of silicon, germanium, aluminium, tin, selenium and combinations thereof.

[0018] In a preferred embodiment, the reactants and / or the reactant mixture present in step a) of the process contain organic solvents in a concentration of <0.1 vol%, based on the total volume of the reactant mixture. The lower the proportion of organic solvents in the reactant mixture, the more cost-effective the process and the higher the quality of the solid electrolyte produced.

[0019] In a further preferred embodiment, the reactants are mixed to form a homogeneous mixture such that no substances containing or consisting of carbon atoms are added during the continuous mixing process. In other words, no such substances are added to the reactant mixture and / or the reactant mixture present in step a) of the process contains no such substances. The advantage is that a solid electrolyte is provided which contains no carbon-containing impurities and thus exhibits very high product quality (e.g., very high ionic conductivity with low electrical conductivity).

[0020] The reactants and / or the reactant mixture present in step a) of the process can consist of lithium, phosphorus and sulfur, preferably in an atomic ratio of lithium:phosphorus:sulfur of 3:1:4 or 11:3:7.

[0021] Furthermore, the reactants and / or the reactant mixture present in step a) of the process can consist of lithium, phosphorus, sulfur and a halogen, preferably in the following atomic ratio: Lie-y : P : Ss- y : Xi+ y , wherein y is between 0 and 1 and X is a halogen, wherein the halogen is particularly preferably selected from the group consisting of chlorine, bromine, iodine and combinations thereof, wherein y is particularly 0 or 0.5, and wherein X is optionally chlorine;.

[0022] Apart from this, the reactants and / or the reactant mixture present in step a) of the process can consist of lithium, phosphorus, sulfur and a lithium-intercalating material, wherein the lithium-intercalating material is preferably selected from the group consisting of silicon, germanium, aluminium, tin, selenium and combinations thereof.

[0023] The mixing of the reactants to form a homogeneous reactant mixture can be carried out in a process chamber of a device for the continuous mixing of reactants.

[0024] The process chamber of the device for the continuous mixing of reactants can have a dew point of < -30°C, preferably < -45°C. The advantage is that the reactant mixture cannot absorb moisture, and thus the product quality of the solid electrolyte produced is higher.

[0025] Apart from that, all spaces in which the reactant mixture and the solid electrolyte (preferably also the reactants) are present in the process can be located in an atmosphere having a dew point of < -30 °C, preferably < -45 °C. For this purpose, said spaces in the process can, for example, be purged with an inert gas and / or dry air with a dew point of < -30 °C, preferably < -45 °C.

[0026] Alternatively, the entire process can be carried out in an atmosphere with a dew point of < -30°C, preferably < -45°C. For example, the entire process can be carried out in a room consisting of an inert gas and / or dry air with a dew point of

[0027] < -30 °C, preferably < -45 °C.

[0028] Furthermore, (only) the process chamber of the device for continuous mixing of reactants may have an inert gas atmosphere or an atmosphere consisting of air with a dew point of < -30°C, preferably

[0029] < -45 °C, exists.

[0030] The inert gas atmosphere contains or consists of an inert gas, preferably selected from the group consisting of argon, nitrogen, and combinations thereof. An inert gas atmosphere has the advantage that a damaging oxidative influence of oxygen on the product quality of the solid electrolyte produced can be excluded. In step b) of the process, continuous mechanical stress can be carried out at a circumferential speed in the range of 0.15 m / s to 6 m / s, preferably in the range of 1 m / s to 5 m / s, to effect a chemical reaction phase in which the reactant mixture is converted into the solid electrolyte.

[0031] Furthermore, in step b) of the process, the continuous mechanical stress following a chemical reaction phase can be carried out at a lower circumferential speed than during the chemical reaction phase to effect a cooling phase, wherein the lower circumferential speed is preferably in the range of 0.15 m / s to <1 m / s, and wherein the cooling phase is preferably followed by another chemical reaction phase. The cooling phase has the advantage that a damaging thermal influence on the quality of the produced solid electrolyte can be avoided.

[0032] The device for continuous mechanical stress can include or consist of a continuously operable mill, wherein the continuously operable mill is preferably selected from the group consisting of ball mills, stirred ball mills, attritor mills, high-energy mills, vibrating mills, impact mills, jet mills, roller mills and combinations thereof, wherein the continuously operable mill particularly preferably includes or consists of a stirred ball mill.

[0033] Furthermore, the device can be filled for continuous mechanical stress until its grinding media fill level is in the range of 30 vol.% to 90 vol.%, preferably 40 vol.% to 75 vol.%, with respect to the total internal volume of the stirred ball mill.

[0034] Furthermore, the device for continuous mechanical stress can be operated with grinding media ranging in size from 0.1 mm to 30 mm, preferably from 0.5 mm to 15 mm. In addition, the device for continuous mechanical stress can have a grinding media material that contains or consists of a ceramic, the ceramic preferably having a density of > 2.5 g / cm³. 3 exhibits. The ceramic can be selected from the group consisting of Al2O3, ZrÜ2, WC, Y-stabilized ZrCh and combinations thereof.

[0035] Furthermore, the device for continuous mechanical stress can have an inert gas atmosphere or an atmosphere consisting of air with a dew point of < -30°C, preferably < -45°C, wherein the inert gas atmosphere preferably contains or consists of an inert gas selected from the group consisting of argon, nitrogen, and combinations thereof. An inert gas atmosphere has the advantage that a damaging oxidative influence of oxygen on the product quality of the manufactured solid electrolyte can be excluded.

[0036] Furthermore, the device for continuous mechanical stress can continuously draw reactant mixture from a chamber or a device for the continuous mixing of reactants, in which the reactants are continuously mixed in step a) of the process. This embodiment makes the process particularly fast and efficient.

[0037] The process can further include, after step b), a thermal post-treatment of the solid electrolyte as step c), preferably carried out continuously, to produce a modified solid electrolyte. The advantage is that, for example, a crystallized solid electrolyte can be provided.

[0038] The thermal post-treatment, preferably carried out continuously, can include heating the solid electrolyte to a temperature in the range of 200 °C to 700 °C, preferably to a temperature in the range of 350 °C to 575 °C.

[0039] Furthermore, the thermal post-treatment, preferably carried out continuously, can include heating the solid electrolyte for a period ranging from 1 second to 24 hours, preferably from 5 seconds to less than 3 hours. In addition, the thermal post-treatment, preferably carried out continuously, can include heating the solid electrolyte for a period long enough for it to crystallize.

[0040] The thermal post-treatment, preferably carried out continuously, in step c) can be performed in a device for continuous thermal post-treatment.

[0041] The thermal post-treatment device may include or consist of a device selected from the group consisting of muffle furnace, rotary kiln, tube furnace, spray dryer, heated fluidized bed and combinations thereof.

[0042] Furthermore, the device for thermal post-treatment can have an inert gas atmosphere or an atmosphere consisting of air with a dew point of < -30°C, preferably < -45°C, wherein the inert gas atmosphere preferably contains or consists of an inert gas selected from the group consisting of argon, nitrogen, and combinations thereof. An inert gas atmosphere has the advantage that a damaging oxidative influence of oxygen on the product quality of the produced solid electrolyte can be excluded.

[0043] Furthermore, the device for thermal post-treatment (e.g., continuously) can obtain solid electrolyte from a chamber or a device for continuous mechanical stress in which the reactant mixture is continuously comminuted in step b) of the process. This embodiment makes the process particularly fast and efficient.

[0044] The process can include, as step d) after step c), continuous mechanical comminution of the modified solid electrolyte. This has the advantage that a solid electrolyte with a desired (smaller) particle size can be provided. By selecting the process parameters, the particle size can be variably adjusted according to the application, and the particle size distribution can be defined, e.g., in the form of a narrower particle size distribution. The continuous mechanical comminution can be carried out in a continuous mechanical comminution device.

[0045] The device for continuous mechanical comminution can include or consist of a continuously operated mill, preferably selected from the group consisting of ball mills, stirred ball mills, attritor mills, high-energy mills, vibrating mills, impact mills, jet mills, roller mills, and combinations thereof, wherein the continuously operated mill particularly includes or consists of a stirred ball mill, jet mill, impact mill, and / or roller mill. The stirred ball mill, jet mill, impact mill, and / or roller mill have the advantage of providing a solid electrolyte with a very narrow particle size distribution.

[0046] Furthermore, the device for continuous mechanical comminution can be filled with modified solid electrolyte until its grinding media fill level is in the range of 30 vol.% to 90 vol.%, preferably 40 vol.% to 75 vol.%, with respect to the total internal volume of the device for continuous mechanical comminution.

[0047] Furthermore, the device for continuous mechanical comminution can be operated with grinding media of a size equal to or smaller than the size of the grinding media in step b) of the process. This allows for the provision of a solid electrolyte with a smaller particle size.

[0048] Apart from that, the device for continuous mechanical comminution can be operated at a peripheral speed that is lower than the peripheral speed in step b) of the method.

[0049] Furthermore, the device for continuous mechanical comminution can have a grinding media material that contains or consists of a ceramic, wherein the ceramic preferably has a density in the range of > 2.5 g / cm³. 3 The ceramic material can be selected from the group consisting of Al₂O₃, ZrÜ₂, WC, Y-stabilized ZrCh, and combinations thereof. Furthermore, the device for continuous mechanical comminution can have an inert gas atmosphere or an atmosphere consisting of air with a dew point of < -30°C, preferably < -45°C, wherein the inert gas atmosphere preferably contains or consists of an inert gas selected from the group consisting of argon, nitrogen, and combinations thereof. An inert gas atmosphere has the advantage that a damaging oxidative influence of oxygen on the product quality of the solid electrolyte produced can be excluded.

[0050] Furthermore, the device for continuous mechanical comminution can draw continuously changing solid electrolyte from a room or a device for thermal post-treatment in which the solid electrolyte is thermally post-treated in step c) of the process (e.g., continuously thermally post-treated). This embodiment makes the process particularly fast and efficient.

[0051] Apart from this, the device for continuous mechanical comminution can include a separation device, and the comminuted, modified solid electrolyte can be separated into different particle size ranges via this separation device. The separation device can be selected from the group consisting of classifiers, cyclones, sieves, and combinations thereof. Furthermore, the separation device can have an inert gas atmosphere or an atmosphere consisting of air with a dew point of < -30°C, preferably < -45°C. An inert gas atmosphere has the advantage that a detrimental oxidative influence of oxygen on the product quality of the produced solid electrolyte can be excluded.

[0052] According to the invention, a plant for the mechanochemical synthesis of a solid electrolyte is further provided, comprising: a) a device for the continuous mechanical stressing of a reactant mixture; b) a device for the continuous supply of a reactant mixture to the device for the continuous mechanical stressing;(c) a control unit, wherein the control unit is configured to cause the device for the continuous supply of a reactant mixture to continuously supply a homogeneous reactant mixture suitable for the production of a solid electrolyte to the device for continuous mechanical stressing, and to cause the device for continuous mechanical stressing to continuously mechanically stress the homogeneous reactant mixture supplied by the device for the continuous supply of a reactant mixture such that the homogeneous reactant mixture is continuously converted into a solid electrolyte via a chemical reaction induced by the continuous mechanical stressing.

[0053] The system according to the invention has the same advantages as the method according to the invention.

[0054] The plant may further include a device for (preferably continuously) mixing reactants, wherein the control unit of the plant is configured to cause the device for mixing reactants to mix reactants suitable for the production of a solid electrolyte (preferably continuously) into a homogeneous reactant mixture and to supply the homogeneous reactant mixture (preferably continuously) to the device for the continuous supply of a reactant mixture.

[0055] In this process, the reactants (before being mixed and thus in a homogeneous reactant mixture) can be present in a stoichiometric ratio that is required to produce a specific solid electrolyte.

[0056] Furthermore, the reactants and / or the homogeneous reactant mixture can contain at least one alkali metal, wherein the alkali metal is preferably selected from the group consisting of lithium, sodium and combinations thereof.

[0057] Furthermore, the reactants and / or the homogeneous reactant mixture may contain phosphorus.

[0058] Furthermore, the reactants and / or the homogeneous reactant mixture may contain sulfur. In addition, the reactants and / or the homogeneous reactant mixture may contain at least one halogen, wherein the at least one halogen is preferably selected from the group consisting of chlorine, bromine, iodine, and combinations thereof.

[0059] Furthermore, the reactants and / or the homogeneous reactant mixture can contain an alkali metal intercalating material, wherein the alkali metal intercalating material is preferably a lithium intercalating material, wherein the lithium intercalating material is particularly preferably selected from the group consisting of silicon, germanium, aluminium, tin, selenium and combinations thereof.

[0060] In a preferred embodiment, the reactants and / or the homogeneous reactant mixture contain organic solvents in a concentration of <0.1 vol.%, with respect to the total volume of the reactant mixture.

[0061] In another preferred embodiment, the reactants and / or the homogeneous reactant mixture contain, in addition to the reactants, no substances that contain or consist of carbon atoms.

[0062] The reactants and / or the homogeneous reactant mixture can consist of lithium, phosphorus and sulfur, preferably in an atomic ratio of lithium:phosphorus:sulfur of 3:1:4 or 11:3:7.

[0063] Furthermore, the reactants and / or the homogeneous reactant mixture can consist of lithium, phosphorus, sulfur and a halogen, preferably in the following atomic ratio: Lie- y : P : Ss- y : Xi+ y, where y is between 0 and 1 and X is a halogen, wherein the halogen is particularly preferably selected from the group consisting of chlorine, bromine, iodine and combinations thereof, wherein y is particularly 0 or 0.5, and wherein X is optionally chlorine.

[0064] Furthermore, the reactants and / or the homogeneous reactant mixture can consist of lithium, phosphorus, sulfur and a lithium-intercalating material, wherein the lithium-intercalating material is preferably selected from the group consisting of silicon, germanium, aluminium, tin, selenium and combinations thereof.

[0065] The device for continuously mixing reactants may include a process chamber and the control unit may be configured to cause the reactants in the process chamber to be continuously mixed to form a homogeneously mixed reactant mixture.

[0066] The process chamber of the device for continuous mixing of reactants can have a dew point of < -30°C, preferably < -45°C.

[0067] Apart from that, all rooms of the plant containing the reactant mixture and the solid electrolyte (optionally also the reactants themselves) can be located in an atmosphere with a dew point of < -30 °C, preferably < -45 °C. For this purpose, said rooms of the plant can, for example, be purged with an inert gas and / or dry air with a dew point of < -30 °C, preferably < -45 °C.

[0068] Alternatively, the entire system can be located in an atmosphere with a dew point of < -30°C, preferably < -45°C. For example, the entire system can be located in a room consisting of an inert gas and / or dry air with a dew point of < 30°C, preferably < -45°C.

[0069] Furthermore, (only) the process chamber of the device for continuous mixing of reactants may have an inert gas atmosphere or an atmosphere consisting of air with a dew point of < -30°C, preferably < -45°C.

[0070] The inert gas atmosphere contains or consists of an inert gas, preferably selected from the group consisting of argon, nitrogen and combinations thereof.

[0071] The control unit of the plant can be configured to cause the device to be subjected to continuous mechanical stress, to carry out continuous mechanical comminution at a peripheral speed in the range of 0.15 m / s to 6 m / s, preferably in the range of 1 m / s to 5 m / s, in order to effect a chemical reaction phase in which the reactant mixture is converted into the solid electrolyte.

[0072] Furthermore, the control unit of the system can be configured to cause the device to be subjected to continuous mechanical stress, to carry out the continuous mechanical comminution following a chemical reaction phase at a lower peripheral speed than during the chemical reaction phase in order to effect a cooling phase, wherein the lower peripheral speed is preferably in the range of 0.15 m / s to <1 m / s, and wherein the control unit is preferably configured to cause the device to be subjected to continuous mechanical stress, to allow another chemical reaction phase to follow the cooling phase.

[0073] The device for continuous mechanical stress can include or consist of a continuously operable mill, wherein the continuously operable mill is preferably selected from the group consisting of ball mills, stirred ball mills, attritor mills, high-energy mills, vibrating mills, impact mills, jet mills, roller mills and combinations thereof, wherein the continuously operable mill particularly preferably includes or consists of a stirred ball mill.

[0074] Furthermore, the device for continuous mechanical stress can be caused by a configuration of the control unit to be filled until its grinding media fill level is in the range of 30 vol.% to 80 vol.%, preferably 40 vol.% to 70 vol.%, with respect to the total internal volume of the stirred ball mill.

[0075] Furthermore, the device for continuous mechanical stress can be configured by the control unit to operate with grinding media ranging in size from 0.1 mm to 30 mm, preferably from 0.5 mm to 15 mm, or the device for continuous mechanical stress can have grinding media of said size. In addition, the device for continuous mechanical stress can have a grinding media material that contains or consists of a ceramic, the ceramic preferably having a density of > 2.5 g / cm³. 3 exhibits. The ceramic can be selected from the group consisting of Al2O3, ZrÜ2, WC, Y-stabilized ZrCh and combinations thereof.

[0076] Furthermore, the device for continuous mechanical stress can have an inert gas atmosphere or an atmosphere consisting of air with a dew point of < -30°C, preferably < -45°C, wherein the inert gas atmosphere preferably contains or consists of an inert gas selected from the group consisting of argon, nitrogen and combinations thereof.

[0077] Furthermore, the device for continuous mechanical stress can be caused by a configuration of the control unit to continuously obtain reactant mixture from a room, or a device for continuous mixing of reactants, in which the reactants are continuously mixed.

[0078] The control unit of the system can be configured to initiate a (e.g., continuously performed) thermal post-treatment of the solid electrolyte in order to produce a modified solid electrolyte.

[0079] The control unit can be configured to heat the solid electrolyte (preferably continuously) to a temperature in the range of 200 °C to 700 °C, preferably to a temperature in the range of 350 °C to 575 °C.

[0080] Furthermore, the control unit can be configured to cause the solid electrolyte (preferably continuously) to be heated for a period of time ranging from 1 second to 24 hours, preferably from 5 seconds to < 3 hours.

[0081] Furthermore, the control unit can be configured to heat the solid electrolyte (preferably continuously) for a period of time until it crystallizes. The system can include a device for (preferably continuous) thermal post-treatment, and the control unit can be configured to cause the thermal post-treatment device to perform the thermal post-treatment (preferably continuously).

[0082] The thermal post-treatment device may include or consist of a device selected from the group consisting of muffle furnace, rotary kiln, tube furnace, spray dryer, heated fluidized bed and combinations thereof.

[0083] Furthermore, the device for thermal post-treatment can have an inert gas atmosphere or an atmosphere consisting of air with a dew point of < -30°C, preferably < -45°C, wherein the inert gas atmosphere preferably contains or consists of an inert gas selected from the group consisting of argon, nitrogen and combinations thereof.

[0084] Furthermore, the device for thermal post-treatment can be caused by a configuration of the control unit to obtain (preferably continuously) solid electrolyte from a room or device for continuous mechanical stress in which the reactant mixture is continuously crushed.

[0085] The system's control unit can be configured to initiate continuous mechanical comminution of the modified solid electrolyte. The system can include a device for continuous mechanical comminution, and the control unit can be configured to cause the device to continuously mechanically comminute the modified solid electrolyte.

[0086] The device for continuous mechanical comminution can include or consist of a continuously operated mill, preferably selected from the group consisting of ball mills, agitated ball mills, attritor mills, high-energy mills, vibrating mills, impact mills, jet mills, roller mills and combinations thereof, wherein the continuously operated mill particularly includes or consists of an agitated ball mill, jet mill, impact mill and / or roller mill.

[0087] Furthermore, the device for continuous mechanical comminution can be caused by a configuration of the control unit to be filled with modified solid electrolyte until its grinding media fill level is in the range of 30 vol.% to 90 vol.%, preferably 40 vol.% to 75 vol.%, with respect to the total internal volume of the device for continuous mechanical comminution.

[0088] Furthermore, the device for continuous mechanical comminution can be caused by a configuration of the control unit to be operated with grinding media of a size equal to or smaller than a size of the grinding media of the device for continuous mechanical stress on the plant, or the device for continuous mechanical comminution can have grinding media of said size.

[0089] Apart from that, the device for continuous mechanical comminution can be caused by a configuration of the control unit to operate at a peripheral speed that is lower than the peripheral speed of the device for continuous mechanical stressing of the plant.

[0090] Furthermore, the second device for continuous mechanical comminution can have a grinding media material containing or consisting of a ceramic, wherein the ceramic preferably has a density in the range of > 2.5 g / cm³ 3 exhibits. The ceramic can be selected from the group consisting of Al2O3, ZrÜ2, WC, Y-stabilized ZrCh and combinations thereof.

[0091] Furthermore, the second device for continuous mechanical comminution can have an inert gas atmosphere or an atmosphere consisting of air with a dew point of < -30°C, preferably < -45°C, wherein the inert gas atmosphere preferably contains or consists of an inert gas selected from the group consisting of argon, nitrogen, and combinations thereof. In addition, the second device for continuous mechanical comminution can be caused by a configuration of the control unit to continuously draw changed solid electrolyte from a room or a device for thermal post-treatment in which the solid electrolyte is continuously thermally post-treated.

[0092] Apart from that, the second device for continuous mechanical comminution may include a separation device and the control unit may be configured to cause the separation device to separate the comminuted, modified solid electrolyte into different particle size ranges.

[0093] The separation device can be selected from the group consisting of classifier, cyclone, sieve and combinations thereof.

[0094] Furthermore, the separation device can have an inert gas atmosphere or an atmosphere consisting of air with a dew point of < -30°C, preferably < -45°C.

[0095] According to the invention, a solid electrolyte is further provided which contains or consists of particles with an average roundness in the range of > 0.4. The example and Figure 4 show how the average roundness of the particles of the solid electrolyte can be determined.

[0096] The advantage of medium particle roundness in the solid electrolyte in this range, and generally of a comparatively higher roundness, is that the solid electrolyte exhibits improved flow properties compared to a solid electrolyte with fewer round particles, which could, for example, become misaligned or form-fitted. This is particularly advantageous during dosing and further processing of the solid electrolyte into shaped components (e.g., when processing the solid electrolyte into material mixtures, electrode suspensions, dry electrode mixtures, and / or battery components). Due to the improved flow properties, less energy is required in mixing processes, and shaped components (e.g., battery components) with lower porosity (i.e., with fewer gaseous spaces between the solid material of the shaped components) can be achieved, as the particles can be packed more efficiently into a small volume.This lower porosity (or compactness) has the advantage in components such as energy storage devices, especially in solid-state batteries, that the energy density is increased and the charge transport is improved by a larger electrochemically active contact area.

[0097] The average roundness of the particles of the solid electrolyte according to the invention can be in the range of > 0.45, preferably in the range of > 0.48.

[0098] The solid electrolyte according to the invention can contain or consist of particles with a roundness in the range of 0.30 to 0.85.

[0099] In a preferred embodiment, the solid electrolyte according to the invention contains no particles exhibiting a roundness in the range of < 0.15, preferably in the range of < 0.20, particularly preferably in the range of < 0.25, and especially in the range of < 0.30. The absence of particles with a roundness in these ranges is advantageous because particles with low roundness can reduce the flow properties in subsequent processing – particularly in battery applications (e.g., electrode mixtures, dry coatings) – and thus increase the energy consumption of subsequent mixing processes, reduce the mixing quality, and increase the porosity in the manufactured battery component through mechanical blockages at the particle level (increased porosity corresponds to a reduced energy density in a solid-state battery).

[0100] The solid electrolyte according to the invention can be characterized in that it exhibits a mass loss of < 5 wt.%, preferably < 4 wt.%, particularly preferably < 3 wt.%, most preferably < 2 wt.%, and in particular < 1 wt.%, based on the total weight of the solid electrolyte at a temperature of 800 °C in an atmosphere of argon.

[0101] Furthermore, the solid electrolyte according to the invention can be characterized in that, at a temperature of 400 °C in an atmosphere of synthetic air for analytical purposes, it exhibits a mass loss of < 4 wt.%, preferably < 3 wt.%, particularly preferably < 2 wt.%, and most preferably < 1 wt.%, based on the total weight of the solid electrolyte.

[0102] Apart from that, the solid electrolyte according to the invention can be characterized in that it does not release CO2 at a temperature between 500 °C and 600 °C in an atmosphere of synthetic air for analytical purposes.

[0103] Furthermore, the solid electrolyte according to the invention can be characterized in that it does not release SO2 at a temperature of up to 230 °C, preferably up to 250 °C, particularly preferably up to 280 °C, most preferably up to 300 °C, particularly up to 320 °C, optionally up to 334 °C, in an atmosphere of synthetic air for analytical purposes.

[0104] The low mass loss and / or the absence of CO2 and / or SO2 release due to heat exposure offer the advantage that the solid electrolyte is more dimensionally stable under heat. Furthermore, due to reduced or even nonexistent gas formation during heat exposure (e.g., during thermal heat treatment and / or operation of a component containing or consisting of the solid electrolyte), fewer or no voids (pores) remain in the solid electrolyte, which could reduce its mechanical stability, energy density, and charge transport. The solid electrolyte according to the invention thus exhibits very high mechanical stability, very high energy density, and very high ionic conductivity.

[0105] The electrolyte according to the invention can be produced using the process according to the invention. The solid electrolyte according to the invention thus exhibits characteristics that it necessarily acquires through its production via the process according to the invention. For example, the solid electrolyte according to the invention has a higher ionic conductivity and a lower impurity with carbon-containing substances (and thus a lower electrical conductivity) than a comparable solid electrolyte produced from identical starting materials using a wet chemical process. Furthermore, the solid electrolyte according to the invention exhibits higher thermal stability in argon and synthetic air for analytical purposes than a comparable solid electrolyte produced from identical starting materials using a wet chemical process.The higher thermal stability also results in higher mechanical stability and a higher specific energy density, since less or no gas is formed during thermal treatment of the solid electrolyte that could leave porous spaces in the solid electrolyte (or in a shaped body formed therefrom). Furthermore, the solid electrolyte according to the invention has a different morphology than a comparable solid electrolyte produced from identical starting materials via a wet chemical process, namely particles with a higher average roundness in the range of > 0.4, and the associated advantages (see above).

[0106] The increased thermal stability of the solid electrolyte according to the invention has the advantage of increased safety in subsequent applications, for example in a solid-state battery, in applications with high power densities and high temperature development, as well as in the event of damage to an energy storage device.

[0107] According to the invention, the use of a solid electrolyte according to the invention is also proposed as a component of an electrode of an energy storage device, as an electrolyte of an energy storage device and / or as a separator of an energy storage device, wherein the energy storage device is preferably a battery, particularly preferably a solid-state battery.

[0108] The following figures and example will be used to explain the subject matter of the invention in more detail, without limiting it to the specific embodiments shown here.

[0109] Figure 1 schematically shows a specific embodiment of the method according to the invention.

[0110] Figure 2 shows scanning electron micrographs (magnification: 1500x) of a solid electrolyte according to the invention before thermal treatment (Figure 2A) and of a reference solid electrolyte, which is presumed to have undergone thermal treatment (Figure 2B). The solid electrolyte according to the invention was produced via the inventive process without thermal treatment, and the reference solid electrolyte was produced via a wet chemical process (i.e., a solvent-based process), presumably with thermal treatment.

[0111] Figure 3 shows scanning electron micrographs (magnification: 1000x) of the same solid electrolyte according to the invention, shown in the state before thermal treatment in Figure 2A, after thermal treatment (Figure 3A), and of the same reference solid electrolyte, also shown in Figure 2B, which is presumed to have also undergone thermal treatment (Figure 3A). The solid electrolyte according to the invention was produced by the inventive process with thermal treatment, and the reference solid electrolyte was produced by a wet chemical process (i.e., a solvent-based process), presumably with thermal treatment.

[0112] Figure 4 shows a method for determining the average roundness of the particles of a solid electrolyte. First, individual roundness values ​​of individual particles of the solid electrolyte are recorded by generating a binary image from scanning electron micrographs (magnification: 1000x) of the solid electrolyte according to the invention (see also Figures 2A and 3A) and the reference solid electrolyte (see also Figures 2B and 3B). The binary image of the solid electrolyte according to the invention is shown in Figure 4A, and the binary image of the reference solid electrolyte is shown in Figure 4B. For both cases, the respective frequency of individual roundness values ​​is then used to calculate an average value from the respective frequencies, for example, by graphically representing the frequencies and calculating an average value using the formula given in Figure 4C (see Figure 4C).Figure 4C shows that the mean roundness of the particles of the reference solid electrolyte is only about 0.369, whereas the mean roundness of the particles of the solid electrolyte according to the invention is about 0.568, meaning that the particles of the solid electrolyte according to the invention are on average significantly rounder than the particles of the reference solid electrolyte.

[0113] Figure 5 shows an investigation of the thermal stability of the solid electrolyte according to the invention after thermal treatment (see also Figure 3A) and of the reference electrolyte (shown in Figures 2B and 3B), which was presumably subjected to thermal treatment, in argon by thermogravimetric analysis. The solid electrolyte according to the invention exhibits thermal stability in argon up to approximately 800 °C (see Figure 5A), whereas the reference solid electrolyte exhibits thermal stability in argon only up to approximately 280 °C (see Figure 5B). The "TG" on the y-axis in Figure 5 stands for "thermogravimetry," and the percentage (%) represents the percentage mass loss of the respective sample during heating. The mass loss during heating is caused by a temperature-induced transformation of solids in the respective sample (e.g.,carbon impurities) into gaseous substances, whereby the gaseous substances are lost in the sample mass.

[0114] Figure 6 shows an investigation of the thermal stability of the solid electrolyte according to the invention after thermal treatment (see also Figure 3A) and of the reference electrolyte (shown in Figures 2B and 3B), which was presumably subjected to thermal treatment, in synthetic air for analytical purposes by thermogravimetric analysis. Synthetic air for analytical purposes has an identical composition to ordinary ambient air, except that it does not contain impurities that can occur in ordinary ambient air and is very dry (dew point < -30 °C, usually even < 10 ppm H₂O). The solid electrolyte according to the invention exhibits higher thermal stability (comparatively lower mass loss when the sample is heated) in synthetic air for analytical purposes up to approximately 400 °C (see Figure 6A) than the reference solid electrolyte in synthetic air for analytical purposes (see Figure 6B).The "TG" on the y-axis in Figure 6 stands for "thermogravimetry," and the percentage (%) represents the percentage mass loss of the respective sample during heating. This mass loss during heating is caused by a temperature-induced conversion of solid components of the sample (e.g., carbon impurities) into gaseous substances, with the gaseous components being lost within the sample mass. The reference solid electrolyte forms CO2 from approximately 500 °C due to impurities from carbon-containing solvents, whereas the solid electrolyte according to the invention (which was produced without the use of solvents and carbon-containing materials) exhibits significantly lower CCh formation and no SCh formation. Example: Determination of the (average) roundness of particles in the solid electrolyte.

[0115] The term roundness was originally coined by Hakon Wadell (e.g. Wadell, H., “Volume, Shape and Roundness of Quartz Particles”, Journal of Geology, 43(3): 250-280, DOI:10.1086 / 624298).

[0116] According to Wadell and according to the inventive understanding of this term, the roundness R of a (single) particle is the ratio of the mean radius of all outer radii n of the particle to the largest inner radius of the particle n. ns : where

[0117] R: roundness of the particle (here: roundness of a particle of the solid electrolyte), n: outer radius of the particle, edge radius (here: outer radius of a particle of the solid electrolyte), nns: largest inner radius of the particle (here: largest inner radius of a particle of the solid electrolyte).

[0118] Based on Wadell, the definition and determination of the roundness R of a particle (i.e., its outer contour) can be achieved using the particle radii n and n'.ns The following graphical representation: According to the invention, the average roundness of solid electrolyte particles (i.e., a plurality of solid electrolyte particles) refers to an average value of individual roundness values ​​determined for individual solid electrolyte particles. The average roundness can be calculated, for example, using the following formula: where

[0119] R: medium roundness,

[0120] N: Total number of (determined) roundness values,

[0121] Ri: single determined roundness value (individual value)

Claims

Fraunhofer Society...eV P149360PC00 Patent claims 1. A method for the mechanochemical synthesis of a solid electrolyte, comprising the following steps: a) Continuously feeding a homogeneous reactant mixture suitable for the production of a solid electrolyte into a device for continuous mechanical stressing; and b) Continuously mechanically stressing the homogeneous reactant mixture in the device for continuous mechanical stressing, such that the homogeneous reactant mixture is continuously converted into a solid electrolyte via a chemical reaction induced by the continuous mechanical stressing.

2. A method according to the preceding claim, characterized in that the method comprises providing the homogeneous reactant mixture from step a) by, preferably continuously, mixing reactants suitable for the preparation of a solid electrolyte, and supplying the provided homogeneous reactant mixture to the apparatus for the continuous supply of a reactant mixture, preferably continuously, wherein the reactants preferably i) are mixed in a stoichiometric ratio required for the preparation of a particular solid electrolyte; and / or ii) contain at least one alkali metal, wherein the alkali metal is preferably selected from the group consisting of lithium, sodium, and combinations thereof; and / or iii) contain phosphorus; and / or iv) contain sulfur; and / or v) contain at least one halogen, wherein the at least one halogen is preferably selected from the group consisting of chlorine, bromine, iodine and combinations thereof; and / or vi) contain an alkali metal intercalating material, wherein the alkali metal intercalating material is preferably a lithium intercalating material, wherein the lithium intercalating material is particularly preferably selected from the group consisting of silicon, germanium, aluminium, tin, selenium and combinations thereof; and / or vii) contain organic solvents in a concentration of <0.1 vol%, with respect to the total volume of the reactant mixture; and / or viii) are mixed to a homogeneously mixed reactant mixture such that, during continuous mixing, no substances containing or consisting of carbon atoms are added in addition to the reactants.

3. A method according to the preceding claim, characterized in that the reactants i) consist of lithium, phosphorus, and sulfur, preferably in an atomic ratio of lithium:phosphorus:sulfur of 3:1:4 or 11:3:7; or ii) consist of lithium, phosphorus, sulfur, and a halogen, preferably in the following atomic ratio: Lie-y : P : Ss- y : Xi+y, where y is between 0 and 1 and X is a halogen, wherein the halogen is particularly preferably selected from the group consisting of chlorine, bromine, iodine and combinations thereof, wherein y is particularly 0 or 0.5, and wherein X is optionally chlorine; or iii) consisting of lithium, phosphorus, sulfur and a lithium-intercalating material, wherein the lithium-intercalating material is preferably selected from the group consisting of silicon, germanium, aluminium, tin, selenium and combinations thereof.

4. A method according to claim 2 or 3, characterized in that the mixing of reactants is carried out in a process chamber of a device for the continuous mixing of reactants, wherein the process chamber preferably i) has a dew point of < -30°C, preferably < -45°C; and / or ii) has an inert gas atmosphere or an atmosphere consisting of air having a dew point of < -30°C, preferably < -45°C, wherein the inert gas atmosphere preferably contains or consists of an inert gas selected from the group consisting of argon, nitrogen and combinations thereof.

5. A method according to one of the preceding claims, characterized in that in step b) the continuous mechanical stress is carried out i) at a circumferential speed in the range of 0.15 m / s to 6 m / s, preferably in the range of 1 m / s to 5 m / s, to effect a chemical reaction phase in which the reactant mixture is converted into the solid electrolyte; and / or ii) following a chemical reaction phase is carried out at a lower circumferential speed than during the chemical reaction phase to effect a cooling phase, wherein the lower circumferential speed is preferably in the range of 0.15 m / s to <1 m / s, and wherein the cooling phase is preferably followed by another chemical reaction phase.

6. A method according to one of the preceding claims, characterized in that the device for continuous mechanical stress i) includes or consists of a continuously operable mill, wherein the continuously operable mill is particularly preferably selected from the group consisting of ball mills, stirred ball mills, attritor mills, high-energy mills, vibrating mills, impact mills, jet mills, roller mills and combinations thereof, wherein the continuously operable mill particularly preferably includes or consists of a stirred ball mill; and / or ii) is filled until its grinding media fill level is in the range of 30 vol.% to 90 vol.%, preferably 40 vol.% to 75 vol.%.-%, in relation to the total internal volume of the stirred ball mill; and / or iii) is operated with grinding media of a size in the range of 0.1 mm to 30 mm, preferably in the range of 0.5 mm to 15 mm; and / or iv) has a grinding media material which contains or consists of a ceramic, wherein the ceramic preferably has a density in the range of > 2.5 g / cm³. 3comprising, wherein the ceramic is particularly preferably selected from the group consisting of Al2O3, ZrÜ2, WC, Y-stabilized ZrÜ2 and combinations thereof; and / or v) comprising an inert gas atmosphere or an atmosphere consisting of air having a dew point of < -30°C, preferably < -45°C, wherein the inert gas atmosphere preferably contains or consists of an inert gas selected from the group consisting of argon, nitrogen and combinations thereof; and / or vi) continuously obtains reactant mixture from a room or device for continuously mixing reactants in which, in step a), the reactants are continuously mixed.

7. A method according to any of the preceding claims, characterized in that the method further comprises, after step b), a thermal post-treatment of the solid electrolyte as step c) to produce a modified solid electrolyte, wherein the thermal post-treatment preferably comprises heating the solid electrolyte i) to a temperature in the range of 200 °C to 700 °C, preferably to a temperature in the range of 350 °C to 575 °C; and / or ii) heating it for a period of time in the range of 1 second to 24 hours, preferably in the range of 5 seconds to < 3 hours; and / or iii) heating it for such a period of time until the solid electrolyte crystallizes.

8. Method according to claim 7, characterized in that in step c) the thermal post-treatment is carried out in a thermal post-treatment device, wherein the thermal post-treatment device preferably comprises i) a device selected from the group consisting of a muffle furnace, rotary kiln, tube furnace, spray dryer, heated fluidized bed and combinations thereof; and / or ii) has an inert gas atmosphere or an atmosphere consisting of air having a dew point of < -30°C, preferably < -45°C, wherein the inert gas atmosphere preferably comprises an inert gas selected from the group consisting of argon, nitrogen and combinations thereof; and / or iii) obtains solid electrolyte from a room or device for continuous mechanical stress in which, in step b), the reactant mixture is continuously comminuted.

9. A method according to one of claims 7 or 8, characterized in that the method further comprises, after step c), as step d), a continuous mechanical comminution of the modified solid electrolyte, wherein the continuous mechanical comminution is preferably carried out in a device for continuous mechanical comminution, wherein the device for continuous mechanical comminution particularly preferably i) includes or consists of a continuously operated mill, which is most preferably selected from the group consisting of ball mills, stirred ball mills, attritor mills, high-energy mills, vibrating mills, impact mills, jet mills, roller mills and combinations thereof, wherein the continuously operated mill particularly includes or consists of a stirred ball mill, jet mill, impact mill and / or roller mill;and / or ii) is filled with modified solid electrolyte until its grinding media fill level is in the range of 30 vol.% to 90 vol.%, preferably 40 vol.% to 75 vol.%, with respect to the total internal volume of the continuous mechanical comminution apparatus; and / or iii) is operated with grinding media of a size equal to or smaller than the size of the grinding media in step b); and / or iv) is operated at a peripheral speed lower than the peripheral speed in step b); and / or v) has a grinding media material that contains or consists of a ceramic, wherein the ceramic preferably has a density in the range of > 2.5 g / cm³; 3 comprising, wherein the ceramic is particularly preferably selected from the group consisting of Al2O3, ZrÜ2, WC, Y-stabilized ZrÜ2 and combinations thereof; and / or vi) comprising an inert gas atmosphere or an atmosphere consisting of air with a dew point of < -30°C, preferably < -45 °C, wherein the inert gas atmosphere preferably contains or consists of an inert gas selected from the group consisting of argon, nitrogen and combinations thereof; and / or vii) continuously modified solid electrolyte from a room or a thermal post-treatment device in which the solid electrolyte is continuously thermally post-treated in step c); and / or viii) has a separation device and the comminuted, modified solid electrolyte is separated into different particle size ranges by means of the separation device, wherein the separation device is selected in particular from the group consisting of classifiers, cyclones, sieves and combinations thereof and / or the separation device has in particular an inert gas atmosphere or an atmosphere consisting of air with a dew point of < -30 °C, preferably < -45 °C.

10. Apparatus for the mechanochemical synthesis of a solid electrolyte, comprising: a) a device for the continuous mechanical stressing of a reactant mixture; b) a device for the continuous supply of a reactant mixture to the device for the continuous mechanical stressing; c) a control unit, wherein the control unit is configured to cause the device for the continuous supply of a reactant mixture to continuously supply a homogeneous reactant mixture suitable for the production of a solid electrolyte to the device for the continuous mechanical stressing; and to cause the device to be subjected to continuous mechanical stress, to continuously mechanically stress the homogeneous reactant mixture supplied by the device for the continuous supply of a reactant mixture in such a way that the homogeneous reactant mixture is continuously converted into a solid electrolyte via a chemical reaction caused by the continuous mechanical stress.

11. Plant according to claim 10, characterized in that the plant further comprises a device for, preferably continuously, mixing reactants, wherein the control unit of the plant is configured to cause the device for mixing reactants to mix reactants suitable for the production of a solid electrolyte into a homogeneous reactant mixture and to supply the homogeneous reactant mixture to the device for the continuous supply of a reactant mixture, wherein the reactants preferably i) are present in a stoichiometric ratio required for the production of a specific solid electrolyte; and / or ii) contain at least one alkali metal, wherein the alkali metal is preferably selected from the group consisting of lithium, sodium and combinations thereof; and / or iii) contain phosphorus; and / or iv) contain sulfur;and / or v) contain at least one halogen, wherein the at least one halogen is preferably selected from the group consisting of chlorine, bromine, iodine and combinations thereof; and / or vi) contain an alkali metal intercalating material, wherein the alkali metal intercalating material is preferably a lithium intercalating material, wherein the lithium intercalating material is particularly preferably selected from the group consisting of silicon, germanium, aluminium, tin, selenium and combinations thereof; and / or; vii) contain organic solvents in a concentration of <0.1 vol%, in relation to the total volume of the reactant mixture; and / or viii) do not contain, in addition to the reactants, any substances containing or consisting of carbon atoms.

12. Plant according to claim 11, characterized in that the reactants i) consist of lithium, phosphorus and sulfur, preferably in an atomic ratio of lithium:phosphorus:sulfur of 3:1:4 or 11:3:7; or ii) consist of lithium, phosphorus, sulfur and a halogen, wherein the following atomic ratio preferably applies: Lie-y : P : Ss- y : Xi+y, where y is between 0 and 1 and X is a halogen, wherein the halogen is particularly preferably selected from the group consisting of chlorine, bromine, iodine and combinations thereof, wherein y is particularly 0 or 0.5, and wherein X is optionally chlorine; or iii) consisting of lithium, phosphorus, sulfur and a lithium-intercalating material, wherein the lithium-intercalating material is preferably selected from the group consisting of silicon, germanium, aluminium, tin, selenium and combinations thereof.

13. Plant according to one of claims 11 or 12, characterized in that the device for continuously mixing reactants includes a process chamber and the control unit is configured to cause the reactants to be continuously mixed in the process chamber to form a homogeneously mixed reactant mixture, wherein the process chamber preferably i) has a dew point of < -30°C, preferably < -45°C; and / or ii) has an inert gas atmosphere or an atmosphere consisting of air with a dew point of < -30°C, preferably < -45 °C, wherein the inert gas atmosphere preferably contains or consists of an inert gas selected from the group consisting of argon, nitrogen and combinations thereof.

14. System according to any one of claims 10 to 13, characterized in that the control unit is configured to cause the device to perform continuous mechanical stress i) at a circumferential speed in the range of 0.15 m / s to 6 m / s, preferably in the range of 1 m / s to 5 m / s, in order to effect a chemical reaction phase in which the reactant mixture is converted into the solid electrolyte; and / or ii) following a chemical reaction phase, to perform it at a lower circumferential speed than during the chemical reaction phase in order to effect a cooling phase, wherein the lower circumferential speed is preferably in the range of 0.15 m / s to <1 m / s, and wherein the control unit is preferably configured to cause the device to perform continuous mechanical stress to again follow the cooling phase with a chemical reaction phase.

15. Plant according to one of claims 10 to 14, characterized in that the device for continuous mechanical stress i) includes or consists of a continuously operable mill, wherein the continuously operable mill is particularly preferably selected from the group consisting of ball mills, stirred ball mills, attritor mills, high-energy mills, vibrating mills, impact mills, jet mills, roller mills and combinations thereof, wherein the a continuously operable mill, particularly preferably comprising or consisting of a stirred ball mill; and / or ii) is caused by a configuration of the control unit to be filled until its grinding media fill level is in the range of 30 vol.% to 90 vol.%, preferably 40 vol.% to 75 vol.%, with respect to the total internal volume of the stirred ball mill; and / or iii) is caused by a configuration of the control unit to be operated with grinding media of a size in the range of 0.1 mm to 30 mm, preferably in the range of 0.5 mm to 15 mm; and / or iv) has a grinding media material that contains or consists of a ceramic, wherein the ceramic preferably has a density in the range of > 2.5 g / cm³ 3comprising, wherein the ceramic is particularly preferably selected from the group consisting of Al2O3, ZrÜ2, WC, Y-stabilized ZrÜ2 and combinations thereof; and / or v) comprising an inert gas atmosphere or an atmosphere consisting of air having a dew point of < -30°C, preferably < -45°C, wherein the inert gas atmosphere preferably contains or consists of an inert gas selected from the group consisting of argon, nitrogen and combinations thereof; and / or vi) is caused by a configuration of the control unit to continuously draw reactant mixture from a room or device for continuously mixing reactants, in which the reactants are continuously mixed.

16. Plant according to any one of claims 10 to 15, characterized in that the control unit is configured to initiate a thermal post-treatment of the solid electrolyte in order to produce a modified solid electrolyte, wherein the The control unit is preferably configured to cause the solid electrolyte to i) heat to a temperature in the range of 200 °C to 700 °C, preferably to a temperature in the range of 350 °C to 575 °C; and / or ii) heat for a period of time in the range of 1 second to 24 hours, preferably in the range of 5 seconds to < 3 hours; and / or iii) heat for a period of time long enough for the solid electrolyte to crystallize.

17. Plant according to claim 16, characterized in that the plant includes a thermal post-treatment device and the control unit is configured to cause the thermal post-treatment device to perform the thermal post-treatment, wherein the thermal post-treatment device preferably includes or consists of: i) a device selected from the group consisting of a muffle furnace, rotary kiln, tube furnace, spray dryer, heated fluidized bed and combinations thereof; and / or ii) an inert gas atmosphere or an atmosphere consisting of air with a dew point of < -30°C, preferably < -45°C, wherein the inert gas atmosphere preferably includes or consists of an inert gas selected from the group consisting of argon, nitrogen and combinations thereof;and / or iii) is caused by a configuration of the control unit to obtain solid electrolyte from a room or device for continuous mechanical stress in which the reactant mixture is continuously crushed.; 18. Plant according to one of claims 16 or 17, characterized in that the control unit is configured to initiate continuous mechanical comminution of the modified solid electrolyte, wherein the plant preferably includes a device for continuous mechanical comminution and the control unit is configured to cause the device for continuous mechanical comminution to continuously mechanically comminute the modified solid electrolyte, wherein the device for continuous mechanical comminution particularly preferably includes or consists of a continuously operated mill, which is most preferably selected from the group consisting of ball mills, stirred ball mills, attritor mills, high-energy mills, vibrating mills, impact mills, jet mills, roller mills and combinations thereof, wherein the continuously operated mill is in particular a stirred ball mill, jet mill,The device contains or consists of an impact mill and / or roller mill; and / or ii) is caused by a configuration of the control unit to be filled with modified solid electrolyte until its grinding media fill level is in the range of 30 vol.% to 90 vol.%, preferably 40 vol.% to 75 vol.%, with respect to the total internal volume of the device for continuous mechanical comminution; and / or iii) is caused by a configuration of the control unit to be operated with grinding media of a size equal to or smaller than a size of the grinding media of the device for continuous mechanical stress on the system; and / or iv) is caused by a configuration of the control unit to be operated at a peripheral speed that is less than the peripheral speed of the device for, continuous mechanical stress on the system; and / or v) a grinding media material which contains or consists of a ceramic, wherein the ceramic preferably has a density in the range of > 2.5 g / cm³ 3comprising, wherein the ceramic is particularly preferably selected from the group consisting of Al₂O₃, ZrÜ₂, WC, Y-stabilized ZrÜ₂ and combinations thereof; and / or vi) comprising an inert gas atmosphere or an atmosphere consisting of air with a dew point of < -30°C, preferably < -45°C, wherein the inert gas atmosphere preferably contains or consists of an inert gas selected from the group consisting of argon, nitrogen and combinations thereof; and / or vii) is caused by a configuration of the control unit to obtain continuously modified solid electrolyte from a room or device for thermal post-treatment in which the solid electrolyte is continuously thermally post-treated;and / or viii) a separation device and the control unit is configured to cause the separation device to separate the comminuted, modified solid electrolyte into different particle size ranges, wherein the separation device is in particular selected from the group consisting of classifiers, cyclones, sieves and combinations thereof and / or the separation device in particular has an inert gas atmosphere or an atmosphere consisting of air with a dew point of < -30°C, preferably < -45°C.

19. Solid electrolyte containing or consisting of particles with a mean roundness in the range of > 0.4.; 20. Solid electrolyte according to claim 19, characterized in that the solid electrolyte i) contains or consists of particles with a mean roundness in the range of > 0.45, preferably in the range of > 0.48; and / or ii) contains or consists of particles with a roundness in the range of 0.30 to 0.85; and / or iii) does not contain any particles having a roundness in the range of < 0.15, preferably in the range of < 0.20, particularly preferably in the range of < 0.25, especially in the range of < 0.

30.

21. Solid electrolyte according to one of claims 19 or 20, characterized in that the solid electrolyte i) exhibits a mass loss of < 5 wt.%, preferably < 4 wt.%, particularly preferably < 3 wt.%, most preferably < 2 wt.%, in particular < 1 wt.%, based on the total weight of the solid electrolyte, at a temperature of 800 °C in an atmosphere of argon; and / or ii) exhibits a mass loss of < 4 wt.%, preferably < 3 wt.%, particularly preferably < 2 wt.%, most preferably < 1 wt.%, at a temperature of 400 °C in an atmosphere of synthetic air for analytical purposes.-%, based on the total weight of the solid electrolyte; and / or iii) does not release CO2 at a temperature between 500 °C and 600 °C in an atmosphere of synthetic air for analytical purposes; and / or iv) does not release SO2 at a temperature up to 230 °C, preferably up to 250 °C, particularly preferably up to 280 °C, most preferably up to 300 °C, particularly up to 320 °C, optionally up to 334 °C, in an atmosphere of synthetic air for analytical purposes.

22. Solid electrolyte according to one of claims 19 to 21, characterized in that the solid electrolyte is produced by a method according to one of claims 1 to 9.

23. Use of a solid electrolyte according to one of claims 19 to 22 as a component of an electrode of an energy storage device, as electrolyte of an energy storage device and / or as a separator of an energy storage device, wherein the energy storage device is preferably a battery, particularly preferably a solid-state battery.

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