Lithium silicate composite and method comprising quenching step

Abstract

The invention is based on a composite having a solid structure (10a), a silicate, lithium ions and at least one paramagnetic or diamagnetic element different from lithium, silicon and oxygen, wherein the solid structure (10a) has two regions (20), wherein the solid structure (10a) forms the same crystal orientation. In order to provide utilizable improved material properties, it is proposed to arrange the regions (20) at a distance of at least one millimeter (30) from each other. On the other hand, the invention is based on a method having a quenching step, which produces a solid structure (10b) of a composite (60), which is different from the ambient temperature solid structure, wherein the composite (60) has a silicate, lithium ions and an element different from lithium, silicon and oxygen. In order to provide utilizable improved material properties, it is proposed to produce at least one gram of phase pure composite (60) in the quenching step.

Description

TECHNICAL FIELD

[0001] The present invention relates to a composite according to the preamble of claim 1 and 7 and to a process according to the preamble of claim 12. BACKGROUND

[0002] The dissertation of Christoph Neef entitled "Growth and Characterization of LiMPO4 and Li2MSiO4 M=(Mn, Fe, Co) Micro- and Macrocrystals" discloses the preparation of polyanionic LiMPO4 and Li2MSiO4 M=(Mn, Fe, Co) compounds in micro- and macrocrystals by microwave-assisted hydrothermal synthesis and optical floating zone technique. The prepared materials were structurally characterized by single crystal or powder X-ray diffractometry as well as metallurgically, chemically, and their morphology was investigated by microscopy and X-ray spectroscopy, and further by electrochemical cycling, impedance spectroscopy, magnetic force analysis, and μSR (muon spin rotation) and relaxation measurements. In LiCoPO4 prepared by additive assisted hydrothermal synthesis, the significant influence of the particle morphology on the electrochemical properties and the usability as lithium ion battery material was determined. The influence of the transition metal substitution and the doping with Zn and Fe on the magnetic and electrochemical properties of two polycrystalline LiCoPO4 modifications was further investigated. The spin dynamics of the tetrahedral modifications were investigated by means of NMR and μSR. Thereby, magnetic fluctuations were observed at high temperatures. Macroscopic single crystals of LiMnPO4 (x=0, 0.1, 0.2, 0.3, 0.5, 1) and Li2FeSiO4 were prepared by floating zone technique at elevated pressure and their exact growth parameters were determined. The magnetic properties and the electrical conductivity of LiMnPO4 were investigated and showed a significant doping dependence of the magnetic ground state of the lithium ion and the magnetic anisotropy as well as the high-temperature mobility of the anisotropy. The single crystal structure of the prepared Li2FeSiO4 modification was determined and its magnetic properties were investigated for the first time. 1-x Fe x PO4 (x=0, 0.1, 0.2, 0.3, 0.5, 1) and Li2FeSiO4 were prepared by floating zone technique at elevated pressure and their exact growth parameters were determined. The magnetic properties and the electrical conductivity of LiMnPO4 were investigated and showed a significant doping dependence of the magnetic ground state of the lithium ion and the magnetic anisotropy as well as the high-temperature mobility of the anisotropy. The single crystal structure of the prepared Li2FeSiO4 modification was determined and its magnetic properties were investigated for the first time. 1- x Fe x PO4 were investigated and showed a significant doping dependence of the magnetic ground state of the lithium ion and the magnetic anisotropy as well as the high-temperature mobility of the anisotropy. The single crystal structure of the prepared Li2FeSiO4 modification was determined and its magnetic properties were investigated for the first time.

[0003] The object of the present application is in particular to provide a composite with improved material properties which are available, in particular improved properties in terms of measurability. According to the application, this object is achieved by the features of claim 1, 7 and 12, while advantageous embodiments and further developments of the application can be derived from the dependent claims. SUMMARY

[0004] The present application is derived from a composite with a solid structure, a silicate, lithium ions and at least one paramagnetic or diamagnetic element which is different from lithium, silicon and oxygen, wherein the solid structure has two regions, wherein the solid structure forms the same crystal orientation.

[0005] It is proposed to arrange the regions at a distance of at least one millimeter from each other. Thereby, the composite can have more advantageous material properties and, as a result, the cross section between the two regions is more likely to have the same crystal orientation, so that a composite can be formed which is single-crystalline on a cross section of at least one millimeter in one extension direction. Thus, the solid structure of the composite can be defined more precisely by preferred single-crystal measurement methods.

[0006] "Composite with a solid structure, a silicate, lithium ions and at least one paramagnetic or diamagnetic element" is to be understood as meaning that the composite has (i) a solid structure, (ii) a silicate, (iii) lithium ions, (iv) at least one paramagnetic or diamagnetic component. The composite must therefore have all four features. The silicate, the lithium ions and / or the element are preferably arranged in the solid structure. The silicate, the lithium ions and / or the element preferably form the solid structure at least partially or to a large extent. "The silicate, the lithium ions and / or the element form the solid structure at least partially" is to be understood in particular as meaning that at least 10%, in particular at least 20%, of the solid structure is formed by the silicate, the lithium ions and / or the element. "The silicate, the lithium ions and / or the element form the solid structure preferably to a large extent" is to be understood in particular as meaning that at least 50%, in particular at least 70%, of the solid structure is formed by the silicate, the lithium ions and / or the element. The silicate, the lithium ions and the element preferably have a mass of at least 0.1 g, in particular at least 1 g, individually or in combination. "Solid structure" is to be understood as meaning a structure which is held together under ionic bonds, wherein this is based on electrostatic attraction forces of oppositely charged ions. The solid structure is in particular characterized by a number of differently arranged lattices. The term "silicate" is to be understood as meaning in particular an electrically charged ionic solid compound which consists of oxygen and silicon elements in bonded form. The silicate is formed in particular as a nesosilicate, a sorosilicate, a cyclosilicate, an inosilicate, a phyllosilicate or a tectosilicate. The silicate preferably has a tetrahedral solid structure and / or SiO4, wherein the silicate in particular carries a quadruple negative charge. The silicate preferably has a SiO4 tetrahedral solid structure, wherein the silicate in particular carries a quadruple negative charge. A number of lithium ions can preferably be moved within the solid structure and / or into or out of the solid structure by an external electromagnetic field. "Diamagnetic element" is to be understood as meaning a material which has a magnetic susceptibility χ of less than 0 or a relative magnetic permeability of less than 1 in the pure material state. "Paramagnetic component" is to be understood as meaning a material which has a positive magnetic susceptibility or a magnetic permeability of more than 1 in the pure material state, wherein no persistent magnetic order can be produced with the aid of the material. "Paramagnetic or diamagnetic component" is not to be understood as meaning a ferromagnetic component. "Element" is to be understood as meaning a chemical raw material which cannot be further decomposed by chemical methods or a pure substance which cannot be further chemically decomposed. "Region" is to be understood as meaning a three-dimensional part of the solid structure which forms a volume of not less than one cubic micrometre and at most 0.001 cubic millimetres, wherein in particular the minimum extension in all three spatial directions is 1 micrometre and in particular the maximum extension in all three spatial directions is 0.1 millimetres. The volume is preferably not less than 100 cubic micrometres and / or at most 1000 cubic micrometres."identical crystal orientation" is to be understood as meaning that one of the two regions is specially translated in such a way that its solid-state structure coincides with the solid-state structure of the other region. It is also alternatively understood that a main axis of the solid-state structure of one of the two regions differs by at most 5°, in particular at most 1°, from a particularly identical main axis of the solid-state structure of the second region. Or again, it is alternatively understood that the main axis reflectivity of one region cannot be angularly differentiated from the main axis reflectivity of the second region in a measurement by means of a commercially available Laue diffractometer. "Main axis reflection" is to be understood as meaning, in particular, a reflection of, for example, X-ray radiation which is dependent on a main axis of the solid-state structure. "Main axis" is to be understood as meaning, in particular, an axis which is parallel to the normal orientation of a lattice plane of the solid-state structure. The solid-state structure has, in particular, exactly three main axes. "Distance" is to be understood as meaning the shortest connecting distance between two mass centres of the respective regions. The element is preferably a transition metal ion. "Transition metal ion" is to be understood as meaning a charged subgroup element which has an incomplete d-subshell. Alternatively or additionally, the "transition metal ion" is a zinc subgroup element. Alternatively or additionally, the subgroup element also includes lanthanide elements and actinide elements. Since the element is a transition metal ion, the solid-state structure can have a particularly advantageous regular solid-state structure which is particularly suitable for single crystal measurements. The transition metal ion is particularly and advantageously a subgroup element of the seventh subgroup. The transition metal ion is particularly preferably a manganese ion. Since the transition metal ion is a manganese ion, a particularly advantageous solid-state structure can be produced.

[0007] It is also proposed that the solid-state structure is formed at least partially and, in particular, predominantly as a single crystal having a size of not less than one cubic millimetre, wherein the regions are arranged within the single crystal. "Solid-state structure is formed at least partially as a single crystal" is to be understood as meaning that the solid-state structure is formed as a single crystal at least to the extent of 10%, in particular at least to the extent of 20%, advantageously at least to the extent of 30%. "Solid-state structure is formed at least predominantly as a single crystal" is to be understood as meaning that the solid-state structure is formed as a single crystal at least to the extent of 50%, in particular at least to the extent of 80%, advantageously at least to the extent of 90%. "Single crystal" is to be understood as meaning a solid material whose atoms or molecules are also arranged in a regularly repeating lattice structure over a long-range distance. This also includes double crystals and products which consist predominantly of single crystals. "Double crystal" is to be understood as meaning a crystalline material in which adjoining lattices are arranged mirror-symmetrically to one another. "Product which consists predominantly of single crystals" is to be understood as meaning a product which comprises at least 90% by weight of single crystals, in particular consists of only one single crystal. However, double crystals and products which consist predominantly of single crystals are preferably excluded. By virtue of the advantageous configuration, the composite has at least partially a single crystal, wherein a very high material purity can be ensured in these cross sections and the solid-state structure is particularly regularly arranged, whereby a particularly precise determination of the lattice constant of the solid-state structure can be achieved.

[0008] It is further proposed that the composite has a body side, wherein the two regions are arranged directly on the body side. By "body side" is to be understood in particular a surface of the composite which is visible from a precise viewing direction. By "surface" is to be understood a boundary surface of a three-dimensional body formed predominantly by the composite. By "side" is to be understood one or more surfaces which delimit the body and form a visible portion of the body surface from a viewing direction. The composite has in particular at least two and / or at most six body sides. By virtue of this advantageous configuration, the measurement surface of the composite is improved, since not one region but two regions exhibit a high degree of crystallinity. The measurement surface which the solid structure to be investigated can have is thus increased. This embodiment of the composite is therefore particularly suitable for surface measurements for determining the lattice constant of the solid structure.

[0009] It is further proposed that the composite is produced in a production process having one treatment step in which the solid structure is formed in a growth direction, wherein the regions are arranged at a distance of at least one millimetre perpendicular to the growth direction. By "production process" is to be understood a process having at least one treatment step. The production process has preferably at least two and in particular at least four treatment steps. The treatment steps are preferably characterised by optical floating zone technology. By "optical floating zone technology" is to be understood a floating zone technology by means of electromagnetic radiation. By "optical floating zone technology" is to be understood a process for forming a crystal by means of melting, subsequent cooling and crystallisation, in which the molten zone or the starting material in the starting material zone can be displaced, so that the entire starting material or a part thereof can be transferred into the crystal. The production process is in particular characterised by further previous treatment steps, in particular at least two solid state synthesis steps, in which the components of the composite are produced. One solid state synthesis step is in particular characterised by at least two and preferably exactly three sintering steps. One treatment step which is located between a preceding solid state synthesis step and the optical floating zone technology comprises in particular at least one substrate ingot production step. By "growth direction" is to be understood the direction in which the solid structure grows in a treatment step, in particular in which the solid structure is produced. The optical floating zone technology which defines the growth direction is particularly preferred. By virtue of the advantageous embodiment, it can be assumed that it is very likely that a macroscopic single crystal will be produced which will extend in particular perpendicular to the growth direction.

[0010] The complex advantageously has a second element different from lithium, silicon, oxygen and the paramagnetic or diamagnetic element. The second element is preferably a transition metal ion. The transition metal ion is preferably a subgroup element of the eighth subgroup. The transition metal ion is particularly preferably an iron ion. By virtue of this advantageous embodiment, the complex is easier to produce. The complex can be characterized, inter alia, by further elements different from lithium, silicon, oxygen, the paramagnetic or diamagnetic element and the second element. The second element and / or, in particular, the further elements can preferably be arranged within the solid-state structure and / or the second element and the further elements, inter alia, at least partially and, in particular, largely form the solid-state structure.

[0011] In another embodiment of the application, it is proposed that the complex has a chemical composition defined at least by a molar ratio, wherein the molar ratio is the quotient of the amount of substance of the paramagnetic or diamagnetic element and the amount of substance of the silicate. In this case, the molar ratio is less than 0.4, preferably less than 0.3, in particular greater than 0.1. The "molar ratio" is understood to mean the quotient of the amounts of substance. The "quotient" is understood to mean a mathematical expression having a dividend and a divisor. The "molar ratio is the quotient of the amount of substance of the paramagnetic or diamagnetic element and the amount of substance of the silicate" is understood to mean that in the quotient, the amount of substance of the paramagnetic or diamagnetic element is the dividend and the amount of substance of the silicate is the divisor. By virtue of this particularly advantageous embodiment of the application, a complex having improved crystallinity properties can be obtained, and therefore a particularly advantageous cross section having a high material purity and a high homogeneity in the complex.

[0012] All of the aforementioned embodiments can be explicitly combined with one another.

[0013] In another aspect of the application, the application is based on a method having a quenching step for producing a solid-state structure of a complex, which is different from the ambient-temperature solid-state structure, wherein the complex has a silicate, lithium ions and an element different from lithium, silicon and oxygen.

[0014] It is proposed that at least one gram of a phase-pure complex is produced in the quenching step. The process is improved in terms of material utilization in the quenching step, since, inter alia, the proportion of waste material is reduced. The complex, which can be analyzed, for example, by neutron scattering experiments, can additionally be advantageously produced by this method, since the mass is sufficiently high. In this way, inter alia, the atomic positions can be measured directly, and thus a more precise determination of the solid-state structure can be achieved.

[0015] The "quenching step" is understood to mean a limited time, preferably less than one minute, rapid cooling process in which a solid state structure of the composite which is different from the solid state structure at ambient temperature is produced. The "a solid state structure of the composite which is different from the solid state structure at ambient temperature" is understood to mean, in particular, at least 10% by volume or 10% by weight, preferably at least 50% by volume or 50% by weight, of a solid state structure which is different from the solid state structure at ambient temperature. The "solid state structure at ambient temperature" is understood to mean the solid state structure which has the lowest energy at ambient temperature. The "ambient temperature" is understood to mean a temperature between 273 Kelvin and 303 Kelvin. The "production of at least one gram of a phase-pure composite" is understood to mean that the composite is first of all weighed at least one gram and secondly can be obtained in phase-pure form. "Phase-pure" is understood to mean that the purity of the composite is at least 95% by weight, in particular at least 99% by weight, in particular with respect to the foreign phase, and the solid state structure in the composite is identical, at least 95% by volume, in particular at least 99% by volume. Alternatively, it can also be understood that no other phase can be determined by means of a commercially available XRD measuring device.

[0016] Furthermore, it is proposed that the solid state structure is produced directly below the melting temperature of the composite. The "melting temperature" is understood to mean the temperature at which the liquid phase and the solid phase of the material are just in equilibrium, in which the crystal lattice of the solid state structure begins to change into the liquid state. The "solid state structure is produced directly below the melting temperature of the composite" is understood in particular to mean that, for example, from the liquid phase during the cooling process, the solid state structure is formed directly without a solid state structure conversion. By means of the advantageous embodiment, it is possible to produce a solid state structure which can improve, for example, the ion mobility.

[0017] In addition, it is proposed that transition metal ions are used as elements. Since transition metal ions are used as elements, it is possible to produce particularly advantageous regular solid state structures which are particularly suitable for single crystal measurements. Elements of the eighth subgroup are preferably used as transition metal ions. Iron ions are particularly preferably used as transition metal ions. Since iron ions are used as transition metal ions, particularly advantageous homogeneous solid state structures are produced. It is particularly preferred that a Pmnb solid state structure is formed in the quenching step.

[0018] The quenching step is advantageously carried out by means of a liquid. The "liquid" is understood to mean something which is in the liquid physical state at room temperature. The "quenching step is carried out by means of a liquid" is understood to mean that the liquid absorbs the thermal energy of the composite and is therefore heated, so that an accelerated cooling process can be carried out compared to a cooling process without a liquid. Preferably, the composite is cooled by means of a liquid which is in direct contact. By means of this advantageous embodiment, the quenching step can be carried out particularly quickly, so that a high cooling speed can be achieved. In addition, the use of a liquid makes it possible to achieve a high heat transfer from the composite to the liquid; this is based on the high heat capacity of the liquid. Water and / or oil are particularly used as the liquid.

[0019] It is further proposed that the oxidation of the compound is reduced or prevented in the quenching step by means of an oxygen-absorbing preparation. "Oxidation" is to be understood as meaning the emission of electrons from elements and / or chemical bonds. "Oxygen-absorbing preparation" is to be understood as meaning a compound or a device which absorbs oxygen in the quenching step, thereby producing an oxygen-reduced environment, in particular within a range of ten centimetres, for example, of the product. "Reduced or prevented oxidation of the compound" is to be understood as meaning that the oxygen content in the compound is lower than without the oxygen-absorbing preparation. The difference is at least 10%, in particular at least 20%. By means of this advantageous embodiment, the quenching step is particularly efficient in terms of material, thereby producing particularly little waste in the quenching step.

[0020] In a further embodiment of the application, it is proposed that the compound is cooled in the quenching step at a rate of at least ten Kelvin per second. Thereby, particularly pure solid structures can be produced, while at the same time particularly solid structures which form just below the melting temperature can be produced.

[0021] It is further proposed that the method has a heating process which is carried out in an oxygen-free atmosphere, wherein the final temperature of the heating process is the starting temperature of the quenching step, and thus the solid structure after heating is homogeneous. "Heating process" is to be understood as meaning a process in which the temperature is increased. "Oxygen-free atmosphere" is to be understood as meaning a gas composition which has a maximum of 1% oxygen, in particular a maximum of 0.01% oxygen. "Homogeneous" is to be understood as meaning that the solid structure is likewise at least 95% by weight, in particular at least 99% by weight, and / or at least 95% by volume, in particular at least 99% by volume.

[0022] In a further embodiment of the application, it is proposed that the compound is produced by a method which is characterised by a quenching step.

[0023] All of the aforementioned embodiments can explicitly be combined with one another.

[0024] In order to explain the present patent application, the papers of the prior art can also be used to explain the terms.

[0025] Batteries, secondary cells, optical devices, jewellery, sample crystals, surface coatings of devices and / or electronic components, such as are disclosed, for example, in patent publication DE 3433150 C2 by Ludwig Rausch, can have a compound according to the application, or these components can in particular be produced by a method according to the application. However, other intended purposes are not excluded. It is particularly conceivable that a product which meets the intended purposes mentioned above can be produced from a compound in further method steps. It is particularly conceivable that the method has further production steps which are not claimed in the present patent application, thereby obtaining a product which can meet the intended purposes mentioned above.

[0026] Further advantages are obtained from the following description of the figures. In the figures, embodiments of the invention are shown. The figures, the description and the claims comprise a number of combined features. The person skilled in the art will also actually consider these features separately and combine them into further useful combinations. BRIEF DESCRIPTION OF DRAWINGS

[0027] Figure 1 representing a composite having lithium ions, manganese ions, iron ions and silicates;

[0028] Figure 2 representing a composite for preparing a Laue diffractometer measurement;

[0029] Figure 3 representing a Laue diffraction pattern of a region of the composite;

[0030] Figure 4 representing a second Laue diffraction pattern of a second region of the composite;

[0031] Figure 5 representing an electron microscope SEM micrograph of the composite;

[0032] Figure 6 representing a composite having lithium ions, iron ions and silicates before passing through a method;

[0033] Figure 7 representing a composite after passing through a method; and

[0034] Figure 8 representing an XRD measurement of the composite.

[0035] The composite is prepared by a preparation process. The preparation process has two solid state synthesis steps. The first solid state synthesis prepares Li2Si03. The first solid state synthesis step utilizes Li2C03and Si02as educts in a ratio of 1.01 : 1. The first solid state synthesis step has a milling step by a marumi mill with 5 mm balls in acetone at 300 rpm for eight hours, wherein the first solid state synthesis step has a subsequent drying step which dries the educts in an ambient atmosphere at 60 °C. The first solid state synthesis step has a first synthesis step after the drying step which is performed in a tube furnace at 700 °C for six hours under an argon atmosphere of 100 mbar and a gas flow of 150 sccm (standard cubic centimeters per minute). The heating and cooling rate of the tube furnace is 150 K / h. It is particularly used for the emission of waste gas reaction products, in particular C02. The first solid state synthesis step has a second sintering step which sinters the milled raw material of the first sintering step at 750 °C for six hours in air.

[0036] Li₂CO₃ + SiO₂ → Li₂SiO₃ + CO₂

[0037] The second solid-state synthesis step includes a mixing step in which previously sintered Li₂SiO₃ is mixed with Fe, Fe₃O₄, and MnO in a ratio of 1:0.25x:0.25x:1-x, where the value of x must be less than 1. The second solid-state synthesis step consists of three sintering steps following the mixing step. Between each sintering step, there is a manual one-hour breakup step. Each of these three sintering steps involves a one-hour phase formation at 300°C under a negative pressure of 100 mbar and an argon flow of 150 sccm. The temperature of the first sintering step is 800°C. The temperatures of the second and third sintering steps are 900°C. The heating and cooling rates are both 150 K / h. The sintering time is twelve hours for each step. During these sintering steps, Li₂SiO₃ undergoes a chemical reaction with Fe, Fe₃O₄, and MnO.

[0038]

[0039] The mixing step can be carried out alternatively by replacing Fe3O4 with Fe2O3.

[0040]

[0041] The preparation process includes a substrate ingot preparation step, which follows two solid-state synthesis steps. An optical floating zone technique is also incorporated after the substrate ingot preparation step. This technique is performed under an argon atmosphere. The optical floating zone technique is executed using a device with two pulling drives operating at a pulling speed of 2.5 mm / h to 10 mm / h. The floating zone technique utilizes a mixture of Fe3O4 mixed powders.

[0042] Figure 1 and Figure 2 The composite shown has a solid structure 10a, a silicate, lithium ions, and at least one manganese ion. The solid structure 10a has two regions 20, which are arranged in the same crystal orientation, and the regions 20 are arranged at a distance 30 of at least one millimeter from each other. The silicate, lithium ions, and manganese ions are arranged within the solid structure 10a, and / or the silicate, lithium ions, and manganese ions at least constitute a majority of the solid structure 10a. The regions 20 form a volume of not less than 1 cubic micrometer.

[0043] The solid structure 10a can be formed at least partially as a single crystal with dimensions not less than one cubic millimeter, wherein the regions 20 can be arranged within the single crystal. The composite has a bulk side 40, wherein two regions 20 are arranged directly on the bulk side 40.

[0044] The solid structure 10a forms a growth direction 50 during the production with the optical float-zone technique, whereas the regions 20 are arranged at a distance 30 of at least one millimeter perpendicular to the growth direction 50. The composite has a chemical composition defined at least by a molar ratio, wherein the molar ratio constitutes the quotient of the amount of substance of paramagnetic or diamagnetic elements and the amount of substance of silicates, whereas the molar ratio is between 0.24 and 0.27. The composite is formed at least partially as a Li2Fe0.75±0.02Mn0.25±0.02SiO4 single crystal.

[0045] The two regions 20 each produce a Laue diffraction image as shown in Figure 3 and 4 The Laue image in Figure 3 shows that the principal axis reflection 90 is located directly to the right of the protection of the Photonic Sciences Laue CCD (charge-coupled device). The Laue measurement direction thus corresponds to the growth direction 50. Three to four weakly visible lines 100 intersect at this point. In comparison to the Laue image of Figures 3 to 4 the composite was measured rotated by 10°. As shown in Figure 2 the rotation leads to a change in the measurement position. The distance 30 between the measurement positions is greater than one millimeter. Figure 4 In Figure 3 the principal axis reflection 90 has shifted to the right of the center point. The lines 100 which were perpendicular in Figure 4 have a curved trajectory in The other two to three lines 100 are no longer visible.

[0046] Figure 5 The SEM micrograph (scanning electron microscope image) in represents a one-millimeter-sized electron microscope of the composite. The composite forms a solid structure 10a of at least 90 vol.-%, preferably 98 vol.-%, which is formed as a Li2Fe0.75±0.02Mn0.25±0.02SiO4 crystal. The composite has at least one foreign phase 110. The foreign phase 110 is made of ferrous oxide, wherein the composite forms a maximum of 10 vol.-%, preferably less than 2 vol.-%, of the foreign phase. Another foreign phase 120 is made of SiO2, wherein the composite forms a maximum of 5 vol.-%, preferably less than 1 vol.-%, of the foreign phase 120. The solid structure 10a has cracks 130.

[0047] A method has a first solid state synthesis step, which is identical to the first solid state synthesis step mentioned in the preparation process. The method has a second solid state synthesis step after the first solid state synthesis step, which is identical to the alternative mixing step mentioned in the preparation process. In contrast to the preparation process, the second solid state synthesis step has an x value of 1. The second solid state synthesis step has a first sintering step, which is carried out at 800°C for twelve hours.

[0048] Figure 6 A ceramic boat 140 is shown, which has a complex of lithium ions, iron ions and silicates and an oxygen absorbing article 80 made of sacrificial iron before it is subjected to the method. The complex should be placed as compactly as possible in the same place in order to keep the surface and volume ratio of the complex as small as possible.

[0049] The method is characterized by a quenching step, by which a solid structure 10b of the complex 60 is produced, which is different from the room temperature solid structure, wherein the complex 60 has silicates, lithium ions and elements different from lithium, silicon and oxygen, wherein at least one gram of phase-pure complex 60 is produced in the quenching step. The quenching step is carried out with the aid of a liquid 70. Due to the oxygen absorbing article 80 made of sacrificial iron, in particular, oxidation of the complex 60 is reduced or prevented in the quenching step.

[0050] The method is characterized by a heating process carried out in an oxygen-free atmosphere, wherein a temperature of 950°C is maintained for more than 16 hours. This temperature represents the starting temperature of the quenching step of the method. The quenching step is carried out in 15 ± 2 seconds. In the quenching step, the complex 60 cools down by at least ten Kelvin per second.

[0051] Figure 7 The complex 60 is shown after it has been subjected to the method. The complex 60 must be placed as compactly as possible so that certain parts can react with the liquid 70 consisting of deionized (fully desalted) water and / or oxygen from the air in the quenching step at 950°C. Therefore, a large part of the complex 60, preferably at least 60% by weight, is subjected only to the quenching step without any chemical reaction.

[0052] In addition to the quenching step, the method has a subsequent, in particular manual, sorting step, in which at least one gram of phase-pure complex 60 is produced.

[0053] Figure 8XRD (x-ray diffraction) measurements of the composite 60 (upper graph; note: the data shown in the central and lower graphs are better than the upper graph (non-actual width of the peaks)). The composite, which is phase pure and forms a Pmnb solid state structure, was used as the basis for the simulation (central graph). The measurements of the composite 60, prepared using the method of the present invention, show no evidence of any foreign phase after removal of the simulated basis (lower graph). The solid state structure 10b was prepared to form directly below the melting temperature of the composite 60.

[0054] List of Reference Signs

[0055] Solid State Structure 10

[0056] Region 20

[0057] Distance 30

[0058] Body Side 40

[0059] Growth Direction 50

[0060] Composite 60

[0061] Liquid 70

[0062] Article 80

[0063] Principal Axis Reflection 90

[0064] Line 100

[0065] Foreign Phase 110

[0066] Foreign Phase 120

[0067] Crack 130

[0068] Ceramic Hull 140

Claims

1. A composite having a solid structure (10a), silicate, lithium ions and at least one paramagnetic or diamagnetic element, which is different from lithium, silicon and oxygen and is a transition metal ion, wherein the transition metal ion is a subgroup element of the seventh subgroup, wherein the solid structure (10a) has two regions (20) in which the solid structure (10a) forms the same crystal orientation, characterized in that the regions (20) are arranged at a distance (30) of at least one millimeter from one another.

2. The composite of claim 1, wherein, The solid structure (10a) is formed at least partially as a single crystal of not less than one cubic millimeter, wherein the regions (20) are arranged within the single crystal.

3. The composite of claim 1, wherein, A portion of the lithium ions can be moved within the solid structure (10a) and into or out of the solid structure (10a) by an external electromagnetic field.

4. The composite of claim 1, wherein having a body side (40), wherein the two regions (20) are arranged directly on the body side (40).

5. The composite according to claim 1, produced by a production process having a treatment step, wherein the solid structure (10a) constitutes a growth direction (50), wherein the regions (20) are arranged at a distance (30) of at least one millimeter perpendicular to the growth direction (50).

6. The composite of claim 1, wherein, The chemical composition is defined by at least one molar ratio, wherein the molar ratio is the quotient of the amount of substance of the paramagnetic or diamagnetic element to the amount of substance of the silicate, and in this case the molar ratio is less than 0.

4.

7. A composite having a solid state structure (10a), silicate and lithium ions, wherein, A portion of the lithium ions can be moved within the solid structure (10a) and into or out of the solid structure (10a) by an external electromagnetic field, and have at least one paramagnetic or diamagnetic element different from lithium, silicon and oxygen, wherein the solid structure (10a) has two regions (20) in which the solid structure (10a) forms the same crystal orientation, characterized in that the regions (20) are arranged at a distance (30) of at least one millimeter from one another.

8. The composite of claim 7, wherein, The solid structure (10a) is formed at least partially as a single crystal of not less than one cubic millimeter, wherein the regions (20) are arranged within the single crystal.

9. The composite of claim 7, wherein having a body side (40), wherein the two regions (20) are arranged directly on the body side (40).

10. The composite according to claim 7, produced by a production process having a treatment step, wherein the solid structure (10a) constitutes a growth direction (50), wherein the regions (20) are arranged at a distance (30) of at least one millimeter perpendicular to the growth direction (50).

11. The composite of claim 7, wherein, The chemical composition is defined by at least one molar ratio, wherein the molar ratio is the quotient of the amount of substance of the paramagnetic or diamagnetic element to the amount of substance of the silicate, and in this case the molar ratio is less than 0.

4.

12. A method with a quenching step, which produces a solid state structure (10b) of a compound (60), which is different from an ambient temperature solid state structure, wherein the compound (60) has silicates, lithium ions and elements different from lithium, silicon and oxygen, characterized in that at least one gram of phase pure compound (60) is produced in the quenching step, which solid state structure is characterized by several differently arranged lattices.

13. The method of claim 12, wherein, The heating process is carried out under an oxygen-free atmosphere, wherein the final temperature of the heating process is the starting temperature of the quenching step, whereby the solid state structure (10b) is homogeneous after the heating process.

14. The method of claim 12, wherein The solid state structure (10b) is produced, which is formed directly below the melting temperature of the compound (60).

15. The method of claim 12, wherein, A Pmnb solid state structure (10b) is formed in the quenching step.

16. The method of claim 12, wherein, The quenching step is carried out with the aid of a liquid (70).

17. The method of claim 16, wherein, The compound (60) is cooled by a liquid (70) which is in direct contact with the compound.

18. The method of claim 12, wherein, During the quenching step, oxidation of the compound (60) is reduced or prevented by means of an oxygen absorption article (80).

19. The method of claim 12, wherein, The compound (60) is cooled in the quenching step by at least ten Kelvin per second.

20. The method of claim 12, wherein, Transition metal ions are used as elements, wherein elements of the eighth subgroup are used as the transition metal ions.

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