Complex fluoride composite and method for producing same

Abstract

To provide a double fluoride composite capable of producing a dense molded article without using an auxiliary agent.SOLUTION: The complex fluoride composite has a core-shell structure of a core of a crystalline component or an amorphous component of a complex fluoride containing fluorine, an alkali metal element and a second metal element different from the alkali metal element, and a shell of an amorphous component or a crystalline component of a complex fluoride covering a part of the core, wherein the second metal element is at least one metal element selected from the group consisting of an alkaline earth metal element, aluminum, gallium, indium, zinc and yttrium.SELECTED DRAWING: Figure 1

Description

[Technical Field]

[0001] The present disclosure relates to a complex fluoride complex and a method for producing the same. [Background technology]

[0002] Ceramic materials have been used in a variety of fields, including window materials for optical components and speaker diaphragms. Generally, the ceramic materials described above are obtained by subjecting inorganic compounds such as aluminum oxide to processes such as heating and pressure molding. Because the density of a molded body affects the material properties and, ultimately, the properties of the device in which it is used, a technique for increasing the density of a molded body involves mixing an auxiliary agent to improve the bonding between inorganic compounds and then processing the molded body (see, for example, Patent Document 1). [Prior art documents] [Patent documents]

[0003] [Patent Document 1] Special Publication No. 7-087637 Summary of the Invention [Problem to be solved by the invention]

[0004] However, the above-mentioned methods may result in residues of the auxiliary agent being mixed into the molded product, which may affect the strength and optical properties of the molded product.

[0005] The present disclosure has been made in view of the above-mentioned problems, and has an object to provide a complex fluoride composite that enables the production of a dense molded body without using an auxiliary agent. [Means for solving the problem]

[0006] The complex fluoride complex according to the present disclosure has a core-shell structure comprising a core of a crystalline or amorphous complex fluoride component containing fluorine, an alkali metal element, and a second complex fluoride component different from the alkali metal element, and a shell of the amorphous or crystalline complex fluoride component covering a portion of the core, wherein the second complex fluoride component is at least one metal element selected from the group consisting of alkaline earth metal elements, aluminum, gallium, indium, zinc, and yttrium.

[0007] The method for producing a complex fluoride composite according to the present disclosure includes a generating step of mixing a first solution in which a first compound containing fluorine and an alkali metal element is dissolved with a second solution in which a second compound containing at least one metal element selected from the group consisting of alkaline earth metal elements, aluminum, gallium, indium, zinc, and yttrium is dissolved to produce a complex fluoride, and a growing step of growing the produced complex fluoride to obtain a complex fluoride composite containing a crystalline component and an amorphous component, wherein in the generating step, the product complex fluoride is brought into a supersaturated state within 2500 milliseconds from mixing the first solution and the second solution, and the growing step is completed within 24 hours from mixing the first solution and the second solution. [Effects of the Invention]

[0008] The complex fluoride composite according to the present disclosure contains a crystalline component and an amorphous component, and therefore a dense molded body can be produced without using an auxiliary agent. [Brief explanation of the drawings]

[0009] [Figure 1] 1 is a schematic cross-sectional view showing an example of the cross-sectional structure of a complex fluoride composite according to a first embodiment. [Figure 2] 1 is a schematic enlarged cross-sectional view showing a part of an example of the cross-sectional structure of one particle of a complex fluoride composite according to Embodiment 1. FIG. [Figure 3] 1 is a schematic diagram showing an example of the configuration of an apparatus for producing a multi-fluoride composite according to Embodiment 1. FIG. [Figure 4] FIG. 1 is a graph showing the relationship between the change in solute solubility over time and nucleation and particle growth. [Figure 5] 1 shows XRD patterns of the complex fluoride according to the first embodiment at rotation angles 2θ of 10° to 30°. [Figure 6] 1 shows XRD patterns of the complex fluoride composite according to the first embodiment at rotation angles 2θ=30° to 50°. [Figure 7] 1 shows XRD patterns of the complex fluoride according to the first embodiment at rotation angles 2θ of 50° to 70°. [Figure 8] 1 is Table 1 showing the evaluation results of Example 1 and Reference Example 1. DETAILED DESCRIPTION OF THE INVENTION

[0010] The complex fluoride complex according to the first aspect has a core-shell structure comprising a core of a crystalline or amorphous component of a complex fluoride containing fluorine, an alkali metal element, and a second metal element different from the alkali metal element, and a shell of an amorphous or crystalline component of the complex fluoride covering a part of the core, wherein the second metal element is at least one metal element selected from the group consisting of alkaline earth metal elements, aluminum, gallium, indium, zinc, and yttrium.

[0011] The complex fluoride composite according to the second aspect may be the complex fluoride composite according to the first aspect, wherein the core is a crystalline component of the complex fluoride and the shell is an amorphous component of the complex fluoride.

[0012] The complex fluoride complex according to the third aspect may be the complex fluoride complex of the first or second aspect, wherein, in a powder XRD pattern, a measured value of an intensity ratio between the maximum intensity of a peak signal appearing at a rotation angle 2θ=30° or less and the maximum intensity of a peak signal appearing at a rotation angle 2θ=40° to 50° may have a deviation of 10% or more from the theoretical value, which is calculated by subtracting 100% from the ratio of the measured value to the theoretical value of the intensity ratio between the maximum intensity of a peak signal appearing at a rotation angle 2θ=30° or less and the maximum intensity of a peak signal appearing at a rotation angle 2θ=40° to 50°, in a powder XRD pattern of a complex fluoride consisting only of crystalline components.

[0013] A method for producing a complex fluoride composite according to a fourth aspect includes a generating step of mixing a first solution in which a first compound containing fluorine and an alkali metal element is dissolved with a second solution in which a second compound containing at least one metal element selected from the group consisting of alkaline earth metal elements, aluminum, gallium, indium, zinc, and yttrium is dissolved to generate a complex fluoride, and a growing step of growing the generated complex fluoride to obtain a complex fluoride composite containing a crystalline component and an amorphous component, wherein in the generating step, the complex fluoride product is brought into a supersaturated state within 2500 milliseconds from mixing the first solution and the second solution, and the growing step is completed within 24 hours from mixing the first solution and the second solution.

[0014] The method for producing a complex fluoride complex according to a fifth aspect may be the same as that of the fourth aspect, and may further include a separation and recovery step of separating and recovering the complex fluoride complex from the solution containing the complex fluoride complex at a rate of 20 mL / sec or less.

[0015] Hereinafter, a complex fluoride composite and a method for producing the same according to an embodiment of the present disclosure will be described with reference to the accompanying drawings. However, unless otherwise specified, the components, types, combinations, shapes, relative positions, and the like described in the embodiment are merely illustrative examples and are not intended to limit the scope of the present disclosure.

[0016] (Embodiment 1) [Double fluoride complex] Fig. 1 is a schematic cross-sectional view showing an example of the cross-sectional structure of a complex fluoride composite 101 according to embodiment 1. Fig. 2 is a schematic enlarged cross-sectional view showing an example of the cross-sectional structure of one particle of the complex fluoride composite 101 according to embodiment 1. The complex fluoride complex 101 according to the first embodiment contains an alkali metal element. The complex fluoride may contain at least one alkali metal element selected from the group consisting of lithium, sodium, potassium, rubidium, and cesium, for example. The complex fluoride complex may contain fluorine, an alkali metal element, and an additional metal element other than the alkali metal element as the main component. The additional metal element may include at least one metal selected from the group consisting of alkaline earth metals, aluminum, gallium, indium, zinc, and yttrium. Specifically, the additional metal element may include at least one metal selected from the group consisting of magnesium, calcium, strontium, barium, aluminum, gallium, indium, zinc, and yttrium. Complex fluorides containing these metal elements can be easily produced into molded bodies by, for example, a pressurized and heated method. Note that the term "main component" as used herein means that the total content of fluorine, the alkali metal element, and the additional metal element contained in the complex fluoride is 80% or more in molar ratio. The total content may be 85% or more, 90% or more, 95% or more, or even 100%.

[0017] Specifically, the complex fluoride complex may contain at least one of A3AlF6 and ABF3 (wherein, in the above composition formula, A represents one or more alkali metal elements described above, and B represents one or more alkaline earth metal elements described above). A3AlF6 may contain, for example, at least one element selected from the group consisting of Li3AlF6, Li2NaAlF6, Li2KAlF6, Na3AlF6, Na2LiAlF6, Na2KAlF6, K3AlF6, K2LiAlF6, and K2NaAlF6. ABF3 may contain, for example, at least one element selected from the group consisting of LiMgF3, NaMgF3, KMgF3, LiCaF3, NaCaF3, and KCaF3. More specifically, the complex fluoride complex may contain at least one element selected from the group consisting of Na3AlF6 and NaMgF3.

[0018] The complex fluoride complex may contain fluorine, an alkali metal element, and aluminum as main components. Here, "main components" means that the total content of fluorine, alkali metal element, and aluminum contained in the complex fluoride is 80% or more by molar ratio. The total content may be 85% or more, 90% or more, 95% or more, or even 100%.

[0019] A part of the constituent anions of the complex fluoride complex may be substituted with hydroxide ions or oxide ions. For example, in the case of a complex fluoride synthesized in a liquid phase, a part of the complex fluoride ions may be substituted with at least one of hydroxide ions and oxide ions.

[0020] The complex fluoride composite 101 has a crystalline component 102 and an amorphous component 103. The presence of the amorphous component promotes bonding between particles constituting the complex fluoride composite without using an auxiliary agent when producing a compact by, for example, a pressurized and heated method, and a dense compact can be obtained. Here, the presence or absence of amorphous components can be determined by the ratio of the maximum intensity of peak signals appearing in the XRD pattern at rotation angles 2θ of 30° or less to the maximum intensity of peak signals appearing at rotation angles 2θ of 40° to 50°, and the measured intensity ratio to the theoretical value of the intensity ratio in the case of only crystalline components. In this case, the deviation of the measured intensity ratio from the theoretical value (hereinafter referred to as the "XRD comparison value") may be 10% or more, 20% or more, 30% or more, and preferably 40% or more. Furthermore, the relative positions of the crystalline component and the amorphous component are not particularly limited. For example, as shown in Figures 1 and 2, a shell 103 of the amorphous component may surround a core 102 of the crystalline component, or the crystalline component may surround the amorphous component. Furthermore, the boundary between the crystalline component and the amorphous component does not necessarily have to be clear, and the crystalline component and the amorphous component may have a gradation at the boundary. As shown in FIG. 2, for example, a multi-fluoride composite particle 101 may include a core 102 made of a crystalline component and a shell 103 made of an amorphous component that covers a part of the surface of the core 102.

[0021] The complex fluoride composite may be an aggregate of a plurality of complex fluoride composite particles, as shown in Figure 1. Here, the shape of the complex fluoride composite particles is not particularly limited. In FIG. 2, the core 102 is shown as a sphere, and the shell 103 is shown as a shell that covers the entire surface of the core 102, but this is not limiting. For example, the core 102 may be cubic. Alternatively, the core 102 may have an irregular polyhedral shape. The shell 103 may cover only a portion of the surface of the core 102.

[0022] [Double fluoride composite manufacturing equipment] FIG. 3 is a schematic diagram showing an example of the configuration of an apparatus 301 for producing a multi-fluoride complex according to the first embodiment. The multi-fluoride complex producing apparatus 301 according to the first embodiment includes a liquid sending section 302 , a mixing section 303 , a retention channel section 304 , and a recovery and separation section 305 .

[0023] <Liquid delivery section> The liquid delivery unit 102 is only required to be able to deliver a plurality of liquids, and is configured with a liquid delivery device such as a syringe pump, plunger pump, diaphragm pump, tube pump, mono pump, or piezo pump. In FIG. 3, two flow paths 302a and 302b extending from a liquid delivery section 302 deliver a solution of a first compound, for example, an alkali metal fluoride, and a solution of a second compound having a metal element different from the alkali metal fluoride, respectively.

[0024] <Mixer> The mixer 303 is only required to be able to mix multiple liquids in the flow paths, and is configured with a flow path connecting member such as a union tee or manifold of a pipe joint, or a flat plate with grooves or through holes, which is made by bonding or stacking and fixing multiple flat plates together. Specifically, for example, it may be configured using a three-way joint.

[0025] <Retention flow path section> The retention channel section 304 is a channel that connects the mixing section 303 and the recovery and separation section 305, and in which a growth reaction takes place.

[0026] <Recovery and Separation Department> The generated complex fluoride complex is separated and recovered by the recovery / separation section 305 .

[0027] [Method for producing complex fluoride complex] A description will be given of a method for producing a complex fluoride composite according to the present embodiment 1. The method for producing a complex fluoride composite according to the present embodiment 1 includes a generating step for generating a plurality of complex fluoride composites, a growing step for growing the plurality of complex fluoride composites, and a separating and recovering step for separating and recovering the plurality of complex fluoride composites.

[0028] (1) In the production step, a first solution in which a first compound, which is an alkali metal fluoride, is dissolved and a second solution in which a second compound having a metal element different from the alkali metal element contained in the alkali metal fluoride are dissolved are mixed in a liquid phase and reacted to produce a complex fluoride, which is then brought into a supersaturated state to form nuclei.

[0029] Generally, in the synthesis of inorganic compounds, the number of nuclei formed, the crystal growth process, and the crystallinity of the resulting product vary depending on the time it takes for the product to reach a supersaturated state. To obtain a complex fluoride complex having a crystalline component and an amorphous component, the time required to achieve a supersaturated state in the mixer is preferably within 2500 milliseconds after mixing, more preferably within 1200 milliseconds after mixing, and even more preferably within 600 milliseconds and 40 milliseconds or more after mixing. The method for mixing the first and second solutions is not particularly limited. These solutions may be mixed by adding the second solution to the first solution, or by adding the first solution to the second solution. Alternatively, the two solutions may be simultaneously mixed at any flow rate ratio using a microchannel or the like. For example, water may be used as the solvent.

[0030] FIG. 4 is a graph showing the relationship between the time change in the solubility of a solute and the nucleation and particle growth. As shown in Figure 4, the solubility of the complex fluoride, which is the solute produced by mixing the first solution and the second solution, increases with time from mixing, nucleation occurs at a concentration exceeding the critical supersaturation, the concentration decreases, and particle growth occurs from the generated nuclei over time. The inventors of the present invention found that a relatively large amount of amorphous components can be obtained when the timing of the peak concentration at which nucleation occurs is 2500 milliseconds or less, leading to the present invention. On the other hand, when the supersaturated state is reached in less than 40 milliseconds or more than 2500 milliseconds after mixing, the amount of amorphous components is reduced.

[0031] The concentrations of the first and second solutions when mixed can be adjusted appropriately. The concentration of the first compound may be 100 mM or more, or 200 mM or more. The concentration of the first compound may be 1000 mM or less. The concentration of the second compound may be 20 mM or more, or 40 mM or more. The concentration of the second compound may be 200 mM or less.

[0032] Examples of the alkali metal element contained in the first compound include lithium, sodium, potassium, rubidium, and cesium. Specifically, the first compound may contain at least one alkali metal element selected from the group consisting of lithium fluoride, sodium fluoride, potassium fluoride, rubidium fluoride, and cesium fluoride.

[0033] The second compound may contain at least one metal salt selected from the group consisting of metal chlorides, metal nitrates, metal sulfates, and metal organic acid salts, excluding metal fluorides. The metal element contained in the second compound may be at least one selected from the group consisting of alkaline earth metal elements, aluminum, gallium, indium, zinc, and yttrium. The second compound may contain, for example, aluminum chloride.

[0034] (2) In the growth step, a complex fluoride grows by reaction between the complex fluoride and the raw materials in the liquid phase or by bonding between the complex fluorides. The time for operating the growth step is preferably within 24 hours after mixing, more preferably within 3 hours, and even more preferably within 500 seconds. The method for operating the growth step is not particularly limited, and for example, the mixed solution may be stirred in a container such as a beaker, or may be retained in a microchannel or the like.

[0035] (3) In the separation and recovery step, the precipitated multiple complex fluoride complexes are separated from the solution into solid and liquid phases. The solid-liquid separation method is not particularly limited, and for example, filtration or centrifugation can be used. Even after the growth operation in the growth step is completed, as long as precipitates remain in the solution, changes in crystallinity due to atomic rearrangement on the solid surface may occur. Therefore, the solid-liquid separation rate is preferably 20 mL / sec or less, more preferably 12 mL / sec or less, and even more preferably 0.1 mL / sec or less.

[0036] When the second compound is a metal chloride, a metal nitrate, a metal sulfate, or a metal organic acid salt, in addition to the complex fluoride composite particles, chlorides, nitrates, sulfates, and metal organic acid salts of alkali metal elements are generated as by-products when the first compound and the second compound are mixed. Therefore, a washing operation to remove the by-products may be carried out. The alkali metal compounds may be removed, for example, by washing with a solvent such as water during filtration or centrifugation.

[0037] (Examples and Reference Examples) Hereinafter, Example 1 and Reference Example 1 in which sodium hexafluoroaluminate (Na3AlF6), a complex fluoride, was produced will be described.

[0038] Example 1 In this Example 1, the manufacturing apparatus 301 was a flow synthesis apparatus, and two plunger pumps were used as the solution delivery section 302 to deliver two types of compound solutions. Here, as the compound solutions for synthesizing NaAlF, a first solution was prepared by dissolving sodium fluoride, the first compound, in ultrapure water at 768 mM, and a second solution was prepared by dissolving aluminum chloride hexahydrate, the second compound, in ultrapure water at 640 mM. The flow rate ratio of the second solution to the first solution was set to 1 / 5, and the set flow rates of each plunger pump were adjusted so that the flow rate of the mixed solution was 10 mL / min (flow rate of the first solution:flow rate of the second solution = 5:1). At these flow rates, the time from mixing to reaching a supersaturated state was within 595 milliseconds.

[0039] The mixer 303 for the first and second solutions was a double-pipe mixer connected to a static mixer (SUS316 material, inner diameter 1.59 mm, length 50 mm). The screw section in the static mixer promotes mixing of the solutions, making it easier to form a supersaturated state. The solution mixed in the mixer 303 passes through the retention channel section 304 (PFA material, inner diameter 1.59 mm, length 250 mm), where the growth of complex fluorides progresses. 45 mL of the solution discharged from the retention channel section 304 was suction filtered (pore size 0.2 μm) in the recovery separator 305 to obtain the target product, Na3AlF6.

[0040] (Reference example 1) The apparatus configuration, solution concentration, and flow rate ratio were the same as in Example 1. In Reference Example 1, the flow rate was set so that the flow rate after mixing of the first solution and the second solution was 300 mL / min, and 45 mL of the discharged solution was suction-filtered in the recovery separator 305 to obtain Na3AlF6. When using mixers of the same volume and shape, the flow field state can be changed by adjusting the flow rate. This changes the mixing efficiency of the solutions, which changes the phase diagram from the formation of a supersaturated state to the growth process, and therefore changes the shape, size, or crystallinity of the resulting inorganic compound. At the above flow rate, the time from mixing to reaching a supersaturated state is within 20 milliseconds.

[0041] (evaluation) A powder X-ray diffraction (XRD) instrument was used to evaluate the crystallinity of the complex fluoride Na3AlF6. In addition, the obtained complex fluoride complex Na3AlF6 was molded into a cylindrical shape by a pressure heating method, and the density of the molded body was evaluated by measuring the density. In the molding process, Na3AlF6 powder and H2O were placed inside a cylindrical molding die having an internal space, and heated and pressurized at 180°C and 400 MPa to obtain a molded body. In the density evaluation, the volume and mass of the compact were measured and the apparent density was calculated. The apparent density of the compact was then calculated based on the true density of NaAlF (2.98 g / cm 3 The relative density of the compact was calculated by dividing the density by the mass fraction. Na3AlF6 is also known as a component of cryolite, and its small refractive index anisotropy gives it excellent transmittance, for example, for infrared light. Therefore, the linear transmittance of the molded body was evaluated using an FT-IR device. The linear transmittance was converted based on the Beer-Lambert law to obtain the linear transmittance at a thickness of 1 mm.

[0042] The results of the experiment will be explained with reference to Figures 5 to 7 and Table 1 in Figure 8. Figure 8 is Table 1 showing the evaluation results of Example 1 and Reference Example 1. Figures 5 to 7 show XRD patterns (rotation angle 2θ = 10° to 70°) of Na3AlF6 of Example 1 and Reference Example 1. Figure 5 shows the XRD patterns in the range of rotation angle 2θ = 10° to 30°, Figure 6 shows the XRD patterns in the range of rotation angle 2θ = 30° to 50°, and Figure 7 shows the XRD patterns in the range of rotation angle 2θ = 50° to 70°. Here, the curve for Example 1 is shown by a solid line, and the curve for Reference Example 1 is shown by a dashed line.

[0043] Focusing on Figure 5, it can be seen that the signal intensity of Example 1 is generally higher than that of Reference Example 1. It is known that when measuring an amorphous object such as glass using XRD, a broad signal called a halo is detected on the low-angle side due to X-ray diffraction caused by random atomic arrangement. Therefore, when measuring a structure containing an amorphous component in addition to a crystalline component, a curve is obtained that combines a sharp diffraction pattern derived from the crystalline component and a broad pattern derived from the amorphous component. This suggests that Example 1 contains more amorphous components than Reference Example 1.

[0044] Furthermore, when focusing on the peak positions of the XRD patterns, the peaks of Reference Example appear on the higher angle side compared to Examples. Similarly, even in the region of rotation angle 2θ = 30° to 70° where the influence of the halo is small, it can be seen from Figures 6 and 7 that the peaks of Reference Example 1 appear on the higher angle side compared to Example 1. This result indicates that Reference Example 1 has shorter interatomic distances between crystal planes having the same plane index of the corresponding peaks, and indicates that it has more crystalline components with a more rigid atomic arrangement structure.

[0045] The above results suggest that a complex fluoride complex Na3AlF6 containing a larger amount of amorphous components was formed in Example 1 compared to Reference Example 1. In this specification, the degree of amorphousness is evaluated from the ratio of the maximum intensity of the peak signal appearing at a rotation angle 2θ of 30° or less to the maximum intensity of the peak signal appearing at a rotation angle 2θ of 40° to 50°, and the deviation of the measured value from the theoretical value for crystalline components alone. In this example, when comparing the intensity of the sharp peak observed near a rotation angle 2θ = 22° with the intensity of the sharp peak observed near a rotation angle 2θ = 47°, the intensity ratio was 0.76 for the example and 0.59 for the reference example. Furthermore, when the theoretical value of the XRD pattern of the Na3AlF6 crystal (crystalline components only) was referenced, the intensity ratio was 0.52. The percentage deviation from the theoretical value, calculated by subtracting 100% from the measured / theoretical ratio of the intensity ratios (0.76, 0.59) of the example and reference example relative to this theoretical value intensity ratio (0.52), is shown in the left column of Table 1 and is referred to as the XRD comparison value for convenience. The XRD comparison value was 46.2% for the example and 13.5% for the reference example, indicating that the value of Example 1 is expressed as a larger deviation due to the influence of the halo.

[0046] The relative densities of the Na3AlF6 compacts are shown in the center column of Table 1 in Figure 8. The relative density of Example 1 is higher than that of Reference Example 1, which indicates that a denser compact was produced in Example 1. The right column of Table 1 in Fig. 8 shows the average linear transmittance in the wavelength range of 3.8 µm to 4.4 µm, and Example 1 obtained a higher linear transmittance than Reference Example 1. Factors that cause the transmittance to decrease include scattering due to pores in the molded body, and it is thought that the denser the molded body, the lower the scattering intensity, resulting in a higher transmittance. From the above, it was suggested that by producing a complex fluoride composite having an amorphous component, a dense molded body can be produced without using an auxiliary agent. [Industrial Applicability]

[0047] According to the complex fluoride composite of the present disclosure, it is possible to provide a complex fluoride composite having an amorphous structure that allows for the production of a dense molded body without using an auxiliary agent. As a result, for example, high homogeneity is realized, and a molded body having high translucency is obtained. Furthermore, according to the present disclosure, it is possible to provide a method for producing a complex fluoride composite having the above structural characteristics. [Explanation of symbols]

[0048] 101 Double fluoride complex 102 Crystalline Components 103 Amorphous Components 301 Double fluoride composite manufacturing equipment 302 Liquid delivery unit 303 Mixing section 304 Retention channel section 305 Recovery Separator

Claims

1. A complex fluoride complex having a core-shell structure, comprising a core of a crystalline or amorphous component of a complex fluoride containing fluorine, an alkali metal element, and a second metal element different from the alkali metal element, and a shell of the amorphous or crystalline component of the complex fluoride covering a part of the core, the second metal element is at least one metal element selected from the group consisting of alkaline earth metal elements, aluminum, gallium, indium, zinc, and yttrium; Double fluoride complex.

2. 2. The complex according to claim 1, wherein the core is a crystalline component of the complex fluoride and the shell is an amorphous component of the complex fluoride.

3. In the powder XRD pattern, the complex fluoride complex has a measured value of the intensity ratio between the maximum intensity of a peak signal appearing at a rotation angle 2θ of 30° or less and the maximum intensity of a peak signal appearing at a rotation angle 2θ of 40° to 50°, which satisfies the following:

3. The complex fluoride complex according to claim 1, wherein, in a powder XRD pattern of the complex fluoride consisting only of crystalline components, a ratio of a maximum intensity of a peak signal appearing at a rotation angle 2θ of 30° or less to a maximum intensity of a peak signal appearing at a rotation angle 2θ of 40° to 50° is a theoretical value, and the ratio of the measured value to the theoretical value is a deviation of 10% or more.

4. a generating step of mixing a first solution in which a first compound containing fluorine and an alkali metal element is dissolved with a second solution in which a second compound containing at least one metal element selected from the group consisting of alkaline earth metal elements, aluminum, gallium, indium, zinc, and yttrium is dissolved to generate a complex fluoride; a growing step of growing the produced complex fluoride to obtain a complex fluoride composite containing a crystalline component and an amorphous component; Including, In the generating step, the complex fluoride product is brought into a supersaturated state within 2500 milliseconds from the mixing of the first solution and the second solution, and The method for producing a complex fluoride composite, wherein the growing step is completed within 24 hours from the mixing of the first solution and the second solution.

5. 5. The method for producing a complex fluoride complex according to claim 4, further comprising a separation and recovery step of separating and recovering the complex fluoride complex from the solution containing the complex fluoride complex at a rate of 20 mL / sec or less.

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