Crystal face regulated supported manganese tantalate catalyst and preparation method thereof

Abstract

The invention provides a crystal face regulated supported manganese tantalate catalyst and a preparation method thereof, and relates to the field of catalytic materials. The supported manganese tantalate catalyst comprises manganese tantalate and an activated aluminum oxide carrier, and the structure of the manganese tantalate comprises at least one of an octahedral structure, a nanosheet ball structure and a nanometer flower ball structure. The supported manganese tantalate catalyst provided by the invention can expose supported manganese tantalate with a specific high-activity crystal face, so that a manganese tantalate phase is uniformly distributed on the surface of an activated aluminum oxide ball carrier in a nanoscale octahedron, sheet ball and flower ball morphology, the number and availability of active sites are increased, electron transfer of a solid-liquid interface is accelerated, and the catalytic activity of the catalyst is improved. The activation efficiency of the persulfate is obviously improved.

Description

Technical Field

[0001] The present application relates to the field of catalytic materials, and particularly to a supported manganese tantalate catalyst with crystal plane regulation and a preparation method thereof. Background Art

[0002] The persulfate oxidation technology is a widely used method in the field of advanced oxidation. Its core active species, sulfate radical (SO4 - ), has extremely strong oxidation ability and can efficiently mineralize organic pollutants. However, in actual ore dressing wastewater, sulfate radicals are easily interfered by background substances in the wastewater (such as inorganic anions and dissolved organic matter), resulting in an increase in the dosage of persulfate and a decrease in oxidation efficiency, thus limiting the industrial application of the persulfate oxidation technology. Therefore, developing an efficient and green persulfate non-radical oxidation technology and catalyst under actual working conditions has become an important development direction in this field.

[0003] Manganese is rich in reserves and easy to obtain. Due to its good catalytic performance, manganese-based oxides have become a research hotspot for sewage treatment materials. At the same time, tantalate compounds, as typical representatives of the pyrochlore structure, have the characteristics of regular structure, easy regulation, and variable composition elements. However, there has been no relevant report on using pyrochlore compounds as persulfate catalysts. The manganese tantalate nanomaterials prepared by combining the two can give full play to the synergistic advantages of both, and are expected to develop a new type of efficient persulfate catalyst, providing new ideas and methods for solving the above technical bottlenecks. Summary of the Invention

[0004] The purpose of the present application is to provide a supported manganese tantalate catalyst with crystal plane regulation and a preparation method thereof to solve the above problems.

[0005] To achieve the above purpose, the present application adopts the following technical solutions: The present application provides a supported manganese tantalate catalyst with crystal plane regulation. The supported manganese tantalate catalyst includes manganese tantalate and an activated alumina carrier, and the manganese tantalate is loaded on the activated alumina carrier; the structure of the manganese tantalate includes at least one of an octahedral structure, a nanosheet sphere structure, and a nanoflower sphere structure.

[0006] Optionally, the crystal planes of the manganese tantalate expose at least one of the (621), (211), and (200) crystal planes.

[0007] The present application also provides a preparation method of a supported manganese tantalate catalyst with crystal plane regulation. The method includes: Performing a first mixing of water and glycerol to obtain a mixed solution; Performing a second mixing of the mixed solution with a manganese salt, an amino acid, a chloropyridine compound, and activated alumina to obtain a reaction precursor; The reaction precursor and tantalum pentoxide are subjected to a third mixing and then heat treatment to obtain the manganese tantalate.

[0008] Optionally, the volume ratio of the water to the glycerol is 1:0.5 - 1.

[0009] Optionally, the manganese salt includes at least one of manganese chloride, manganese sulfate, and manganese acetate.

[0010] Optionally, the amino acid includes alanine family amino acids.

[0011] Optionally, the activated alumina includes activated alumina balls.

[0012] Optionally, the alanine family amino acids include at least one of L-2-chlorophenylalanine, L-4-fluorophenylalanine, and Z-L-alanine.

[0013] Optionally, the chlorinated pyridine compounds include at least one of 6-chloro-2-hydroxymethylpyridine, dodecylpyridinium chloride, and 2-chloro-3-hydroxypyridine.

[0014] Optionally, the dosage relationship of the manganese salt, the amino acid, the chlorinated pyridine compounds to the activated alumina is 0.5 - 1.0 mmol: 0.2 - 0.4 g: 0.1 - 0.2 g: 0.3 - 0.5 g.

[0015] Optionally, the dosage relationship of the mixed solution to the tantalum pentoxide is 15 mL: 1 - 2 mmol.

[0016] Optionally, the heat treatment is carried out under closed conditions, the temperature of the heat treatment is 100 - 140 °C, and the time is 4 - 8 hours.

[0017] Compared with the prior art, the beneficial effects of this application include: The supported manganese tantalate catalyst provided by this application can expose the supported manganese tantalate with specific highly active crystal planes, making the manganese tantalate phase uniformly distributed on the surface of the activated alumina ball carrier in the morphology of nanoscale octahedrons, sheet spheres, and flower spheres, which not only increases the number and availability of active sites, but also accelerates the electron transfer at the solid-liquid interface, significantly improving the activation efficiency of persulfate.

[0018] On the one hand, the preparation method provided by this application can finely regulate manganese tantalate through liquid-phase controllable synthesis. On the other hand, the synthesis process is simple, easy to operate, and the synthesis process is stable, and high consistency and repeatability can be achieved. Description of the Drawings

[0019] To more clearly illustrate the technical solutions of the embodiments of the present application, the accompanying drawings required for the embodiments will be briefly introduced below. It should be understood that the following drawings only show some embodiments of the present application and should not be regarded as limiting the scope of the present application.

[0020] Figure 1 Scanning electron microscope image of the crystal plane-regulated supported manganese tantalate catalyst provided for Example 1; Figure 2 Scanning electron microscope image of the crystal plane-regulated supported manganese tantalate catalyst provided for Example 2; Figure 3 Scanning electron microscope image of the crystal plane-regulated supported manganese tantalate catalyst provided for Example 3; Figure 4 XRD spectra of manganese tantalate prepared in Examples 1, 2, and 3; Figure 5 XRD spectrum of manganese tantalate prepared in Comparative Example 1; Figure 6 XRD spectra of manganese tantalate prepared in Comparative Examples 2, 3, and 4; Figure 7 Performance curve diagram of manganese tantalate for activating sodium persulfate to oxidize COD. Detailed implementation manners

[0021] As used herein, the terms: "Prepared from" is synonymous with "comprising". The terms "comprising", "including", "having", "containing" or any other variation thereof as used herein are intended to cover non-exclusive inclusion. For example, a composition, step, method, article or device containing the listed elements is not necessarily limited to those elements, but may include other elements not expressly listed or elements inherent to such composition, step, method, article or device.

[0022] The connecting word "consisting of" excludes any unstated element, step or component. If used in a claim, this phrase will render the claim closed, excluding materials other than those described, except for conventional impurities associated therewith. When the phrase "consisting of" appears in a clause of the claim body rather than immediately following the subject, it only limits the elements described in that clause; other elements are not excluded from the claim as a whole.

[0023] When an equivalent, concentration, or other value or parameter is expressed as a range, a preferred range, or a range defined by a series of upper preferred values and lower preferred values, this should be understood to specifically disclose all ranges formed by any pairing of any range upper limit or preferred value with any range lower limit or preferred value, regardless of whether the range is disclosed individually. For example, when the range "1 to 5" is disclosed, the described range should be interpreted to include ranges "1 to 4", "1 to 3", "1 to 2", "1 to 2 and 4 to 5", "1 to 3 and 5", etc. When a numerical range is described herein, unless otherwise stated, the range is intended to include its end values and all integers and fractions within the range.

[0024] In these examples, unless otherwise specified, the parts and percentages are by mass.

[0025] "Part by mass" refers to the basic measurement unit representing the mass ratio relationship of multiple components. 1 part can represent any unit mass, such as 1 g or 2.689 g, etc. If we say that the mass part of component A is a parts and the mass part of component B is b parts, it means the mass ratio of component A to component B is a:b. Or, it means the mass of component A is aK and the mass of component B is bK (K is any number representing a multiple factor). It should not be misunderstood that, different from the number of mass parts, the sum of the mass parts of all components is not limited to 100 parts.

[0026] "And / or" is used to indicate that either or both of the stated situations may occur. For example, A and / or B includes (A and B) and (A or B).

[0027] To better explain the technical solution provided by this application, before the examples, the technical solution will be explained as a whole.

[0028] In a first aspect, this application provides a supported manganese tantalate catalyst with crystal plane regulation. The supported manganese tantalate catalyst includes manganese tantalate and an activated alumina carrier, and the manganese tantalate is loaded on the activated alumina carrier; the structure of the manganese tantalate includes at least one of an octahedral structure, a nanosheet sphere structure, and a nanoflower sphere structure.

[0029] In an alternative embodiment, the crystal planes (621), (211), and (200) of the manganese tantalate are exposed at least one of them.

[0030] In a second aspect, this application also provides a preparation method of a supported manganese tantalate catalyst with crystal plane regulation, and this method includes: Perform a first mixing of water and glycerol to obtain a mixed solution; Perform a second mixing of the mixed solution with a manganese salt, an amino acid, a chloropyridine compound, and activated alumina to obtain a reaction precursor; The reaction precursor and tantalum pentoxide are subjected to a third mixing and then heat treatment to obtain the manganese tantalate.

[0031] In an optional embodiment, the volume ratio of the water to the glycerol is 1:0.5 - 1.

[0032] Optionally, the volume ratio of the water to the glycerol can be 1:0.5, 1:0.55, 1:0.6, 1:0.65, 1:0.7, 1:0.75, 1:0.8, 1:0.85, 1:0.9, 1:0.95, 1:1, or any value between 1:0.5 - 1.

[0033] In an optional embodiment, the manganese salt includes at least one of manganese chloride, manganese sulfate, and manganese acetate.

[0034] In an optional embodiment, the amino acid includes alanine family amino acids.

[0035] In an optional embodiment, the activated alumina includes activated alumina balls.

[0036] In an optional embodiment, the alanine family amino acids include at least one of L-2-chlorophenylalanine, L-4-fluorophenylalanine, and Z-L-alanine.

[0037] In an optional embodiment, the chloropyridine compounds include at least one of 6-chloro-2-hydroxymethylpyridine, dodecylpyridinium chloride, and 2-chloro-3-hydroxypyridine.

[0038] In an optional embodiment, the dosage relationship of the manganese salt, the amino acid, the chloropyridine compounds, and the activated alumina is 0.5 - 1.0 mmol: 0.2 - 0.4 g: 0.1 - 0.2 g: 0.3 - 0.5 g.

[0039] Optionally, the dosage relationship among the manganese salt, the amino acid, the chloropyridine compound and the activated alumina can be 0.5 mmol: 0.2 g: 0.1 g: 0.3 g, 0.6 mmol: 0.2 g: 0.1 g: 0.3 g, 0.7 mmol: 0.2 g: 0.1 g: 0.3 g, 0.8 mmol: 0.2 g: 0.1 g: 0.3 g, 0.9 mmol: 0.2 g: 0.1 g: 0.3 g, 1.0 mmol: 0.2 g: 0.1 g: 0.3 g, 0.5 mmol: 0.3 g: 0.1 g: 0.3 g, 0.5 mmol: 0.4 g: 0.1 g: 0.3 g, 0.5 mmol: 0.2 g: 0.2 g: 0.3 g, 0.5 mmol: 0.2 g: 0.1 g: 0.4 g, 0.5 mmol: 0.2 g: 0.1 g: 0.5 g, 0.6 mmol: 0.3 g: 0.2 g: 0.4 g, 0.7 mmol: 0.3 g: 0.2 g: 0.4 g, 0.8 mmol: 0.3 g: 0.2 g: 0.4 g, 0.9 mmol: 0.3 g: 2 g: 0.4 g, 1.0 mmol: 0.3 g: 0.2 g: 0.4 g, 1.0 mmol: 0.3 g: 0.2 g: 0.5 g, 1.0 mmol: 0.4 g: 0.2 g: 0.5 g, or any value between 0.5 - 1.0 mmol: 0.2 - 0.4 g: 0.1 - 0.2 g: 0.3 - 0.5 g.

[0040] In an alternative embodiment, the dosage relationship between the mixed solution and tantalum pentoxide is 15 mL: 1 - 2 mmol.

[0041] Optionally, the dosage relationship between the mixed solution and tantalum pentoxide can be 15 mL: 1 mmol, 15 mL: 1.2 mmol, 15 mL: 1.4 mmol, 15 mL: 1.6 mmol, 15 mL: 1.8 mmol, 15 mL: 2 mmol, or any value between 15 mL: 1 - 2 mmol.

[0042] In an alternative embodiment, the heat treatment is carried out under airtight conditions, the temperature of the heat treatment is 100 - 140 °C, and the time is 4 - 8 hours.

[0043] Optionally, the temperature of the heat treatment can be 100 °C, 115 °C, 120 °C, 125 °C, 130 °C, 135 °C, 140 °C, or any value between 100 - 140 °C. The time of the heat treatment can be 4 hours, 5 hours, 6 hours, 7 hours, 8 hours, or any value between 4 - 8 hours.

[0044] It is understandable that this application is based on the theory of regulating the geometric configuration by the rotation of amino acid-metal coordination bonds and the electronic interaction between bridged metal ions, and develops a simple and efficient new preparation method. In this application, alanine family amino acids and chloropyridine solution are selected as precursor raw materials, and the directional arrangement of lattice atoms is realized through solvothermal synthesis technology, and manganese tantalate with a specific morphology structure is accurately loaded on the activated alumina carrier. This manganese tantalate with a specific morphology can expose different highly active crystal planes, significantly increasing the number and availability of active sites, thereby greatly improving the activation efficiency of persulfate. Therefore, the crystal plane-regulated supported manganese tantalate catalyst prepared in this application not only has high intrinsic activity and abundant active sites, but also exhibits excellent catalytic performance, providing an efficient and practical innovative solution for the field of persulfate activation treatment of ore dressing wastewater. On the one hand, this method can efficiently realize the batch preparation of manganese tantalate with high intrinsic catalytic activity and abundant active sites; on the other hand, through the loading of activated alumina spheres, not only the stability of manganese tantalate is significantly improved, but also it is easy to recycle. This innovation effectively solves the technical bottlenecks of low catalytic efficiency and difficult recovery commonly existing in existing persulfate nanocatalysts, and shows broad application prospects in the fields of ore dressing wastewater treatment and other catalytic materials.

[0045] The following will describe the implementation scheme of this application in detail with specific examples. However, those skilled in the art will understand that the following examples are only used to illustrate this application and should not be regarded as limiting the scope of this application. Those not specified in the examples are carried out under conventional conditions or conditions recommended by the manufacturer. Those reagents or instruments not specified by the manufacturer can be obtained as conventional products through commercial purchase.

[0046] Example 1 This example provides a crystal plane-regulated supported manganese tantalate catalyst.

[0047] Figure 1 is the scanning electron micrograph of the crystal plane-regulated supported manganese tantalate catalyst; as Figure 1 shown, the structure of the crystal plane-regulated supported manganese tantalate catalyst is an octahedral structure.

[0048] This example also provides a preparation method for the crystal plane-regulated supported manganese tantalate catalyst, and the specific steps are as follows: Mix 10 mL of water and 5 mL of glycerol to obtain a mixed solution.

[0049] Mix the mixed solution with MnCl2·4H2O, L-2-chlorophenylalanine, 6-chloro-2-hydroxymethylpyridine and activated alumina balls to obtain a reaction precursor. Among them, the dosage relationship of MnCl2·4H2O, L-2-chlorophenylalanine, 6-chloro-2-hydroxymethylpyridine and activated alumina balls is 0.6 mmol: 0.25 g: 0.1 g: 0.3 g.

[0050] Add 1.2 mmol of tantalum pentoxide powder to 15 mL of the reaction precursor, and heat-treat it at 110 °C for 4 hours in a closed reaction kettle to obtain a crystal-plane-regulated supported manganese tantalate catalyst.

[0051] Example 2 This example provides a crystal-plane-regulated supported manganese tantalate catalyst: Figure 2 It is the scanning electron micrograph of the crystal-plane-regulated supported manganese tantalate catalyst; as Figure 2 shown, the structure of the crystal-plane-regulated supported manganese tantalate catalyst is a nanosheet sphere structure.

[0052] This example also provides a preparation method of the crystal-plane-regulated supported manganese tantalate catalyst, and the specific steps are as follows: Mix 10 mL of water and 6 mL of glycerol to obtain a mixed solution.

[0053] Mix the mixed solution with MnSO4·4H2O, L-2-chlorophenylalanine, dodecylpyridinium chloride and activated alumina balls to obtain a reaction precursor. Among them, the dosage relationship of MnSO4·4H2O, L-2-chlorophenylalanine, dodecylpyridinium chloride and activated alumina balls is 0.7 mmol: 0.3 g: 0.1 g: 0.5 g.

[0054] Add 1.4 mmol of tantalum pentoxide powder to 16 mL of the reaction precursor, and heat-treat it at 120 °C for 7 hours in a closed reaction kettle to obtain a crystal-plane-regulated supported manganese tantalate catalyst.

[0055] Example 3 This example provides a crystal-plane-regulated supported manganese tantalate catalyst: Figure 3 It is the scanning electron micrograph of the crystal-plane-regulated supported manganese tantalate catalyst; as Figure 3 shown, the structure of the crystal-plane-regulated supported manganese tantalate catalyst is a nanoflower sphere structure.

[0056] This example also provides a preparation method of the crystal-plane-regulated supported manganese tantalate catalyst, and the specific steps are as follows: Mix 7 mL of water and 7 mL of glycerol to obtain a mixed solution.

[0057] Mix the mixed solution with (CH3COO)2Mn, Z-L-alanine, 2-chloro-3-hydroxypyridine and activated alumina balls to obtain a reaction precursor. Among them, the dosage relationship of (CH3COO)2Mn, Z-L-alanine, 2-chloro-3-hydroxypyridine and activated alumina balls is 1 mmol: 0.25 g: 0.2 g: 0.4 g.

[0058] Add 1.4 mmol of tantalum pentoxide powder to 14 mL of the reaction precursor, and heat-treat it at 140 °C for 8 hours in a sealed reaction kettle to obtain a crystal plane-regulated supported manganese tantalate catalyst.

[0059] Comparative Example 1 This comparative example provides a preparation method of a conventional manganese tantalate catalyst, and the specific steps are as follows: Mix 0.3 g of commercially available tantalum pentoxide powder with 1 mL of hydrofluoric acid, prepare it into a suspension and heat it to 120 °C until it is completely dissolved to obtain a clear solution. After the solution is cooled to room temperature, slowly add ammonia water with the same volume as hydrofluoric acid until the reaction is completed. At this time, a white precipitate will be formed, and this white precipitate is amorphous tantalum pentoxide.

[0060] Mix amorphous tantalum pentoxide, 0.4 g of MnCl2·4H2O, 15 mL of ethanol and 0.4 g of activated alumina balls to obtain a reaction precursor.

[0061] Heat-treat the reaction precursor in a sealed reaction kettle at 160 °C for 6 hours to obtain a supported manganese tantalate catalyst.

[0062] Comparative Example 2 This comparative example provides a preparation method of a manganese tantalate catalyst, and the specific steps are as follows: Mix 10 mL of water and 5 mL of glycerol to obtain a mixed solution.

[0063] Mix the mixed solution with MnCl2·4H2O, 2-mercapto-3-pyridinecarboxylic acid, 6-chloro-2-hydroxymethylpyridine and activated alumina balls to obtain a reaction precursor. Among them, the dosage relationship of MnCl2·4H2O, 2-mercapto-3-pyridinecarboxylic acid, 6-chloro-2-hydroxymethylpyridine and activated alumina balls is 0.6 mmol: 0.25 g: 0.1 g: 0.3 g.

[0064] Add 1.2 mmol of tantalum pentoxide powder to 15 mL of the reaction precursor, and heat-treat it at 110 °C for 4 hours in a sealed reaction kettle to obtain a crystal plane-regulated supported manganese tantalate catalyst.

[0065] Comparative Example 3 This comparative example provides a preparation method of a manganese tantalate catalyst, and the specific steps are as follows: Mix 10 mL of water and 5 mL of glycerol to obtain a mixed solution.

[0066] Mix the mixed solution with MnCl2·4H2O, DL-glutamic acid, 6-chloro-2-hydroxymethylpyridine, and activated alumina balls to obtain a reaction precursor. Among them, the dosage relationship of MnCl2·4H2O, DL-glutamic acid, 6-chloro-2-hydroxymethylpyridine, and activated alumina balls is 0.6 mmol: 0.25 g: 0.1 g: 0.3 g.

[0067] Add 1.2 mmol of tantalum pentoxide powder to 15 mL of the reaction precursor, and heat-treat it at 110 °C for 4 hours in a sealed reaction kettle to obtain a crystal plane-regulated supported manganese tantalate catalyst.

[0068] Comparative Example 4 This comparative example provides a method for preparing a manganese tantalate catalyst, and the specific steps are as follows: Mix 10 mL of water and 5 mL of glycerol to obtain a mixed solution.

[0069] Mix the mixed solution with MnCl2·4H2O, L-2-chlorophenylalanine, acetamide, and activated alumina balls to obtain a reaction precursor. Among them, the dosage relationship of MnCl2·4H2O, L-2-chlorophenylalanine, acetamide, and activated alumina balls is 0.6 mmol: 0.25 g: 0.1 g: 0.3 g.

[0070] The XRD patterns of the manganese tantalate prepared in Examples 1, 2, and 3 are as Figure 4 shown. It can be seen that the manganese tantalate crystal provided in Example 1 exposes the (621) crystal plane, the manganese tantalate crystal provided in Example 2 exposes the (211) crystal plane, and the manganese tantalate crystal provided in Example 3 exposes the (200) crystal plane. Figure 5 is the XRD pattern of the manganese tantalate prepared in Comparative Example 1, Figure 6 is the XRD pattern of the manganese tantalate prepared in Comparative Examples 2, 3, and 4. According to Figure 5 , Figure 6 it can be seen that the manganese tantalate crystals prepared in Comparative Examples 1, 2, 3, and 4 expose the (311) crystal plane and do not expose any of the (621) crystal plane, (211) crystal plane, and (200) crystal plane; this indicates that the supported manganese tantalate catalyst prepared by the technical solution provided in this application contains more reaction steps, kinks, and defect sites and has extremely high catalytic activity.

[0071] Taking 151 mg / L of actual ore dressing COD wastewater as an example, the dosage relationship between the manganese tantalate prepared in Examples 1, 2, 3, and Comparative Example 1 and the aqueous solution of sodium persulfate is 1:1 (m). The performance curve of manganese tantalate for activating sodium persulfate to oxidize COD is as Figure 7As shown. After reacting for 30 minutes in Comparative Example 1, the COD concentration in the solution was only reduced to 86 mg / L. In Examples 1, 2, and 3, all had good treatment effects on COD, and the COD concentrations were reduced to 46, 43, and 40 mg / L respectively. It can be seen that the manganese carbonate exposing the (200) crystal plane in Example 3 had the best effect.

[0072] Finally, it should be noted that the above embodiments are only used to illustrate the technical solutions of the present application, and not to limit them; although the present application has been described in detail with reference to the foregoing embodiments, those of ordinary skill in the art should understand that they can still modify the technical solutions recorded in the foregoing embodiments, or perform equivalent replacements on some or all of the technical features; and these modifications or replacements do not cause the essence of the corresponding technical solutions to deviate from the scope of the technical solutions of the embodiments of the present application.

[0073] In addition, those skilled in the art can understand that although some of the embodiments herein include certain features included in other embodiments rather than other features, the combination of the features of different embodiments means that it is within the scope of the present application and forms different embodiments. For example, in the above claims, any one of the claimed embodiments can be used in any combination. The information disclosed in this background art section is only intended to deepen the understanding of the overall background art of the present application, and should not be regarded as an admission or any form of implication that this information constitutes the prior art known to those skilled in the art.

Claims

1. A supported manganese tantalate catalyst with crystal plane regulation, characterized in that, The supported manganese tantalate catalyst comprises manganese tantalate and an activated alumina support, and the manganese tantalate is supported on the activated alumina support; the structure of the manganese tantalate includes at least one of an octahedral structure, a nanosheet sphere structure, and a nanoflower sphere structure.

2. The supported manganese tantalate catalyst with crystal plane regulation according to claim 1, wherein The crystal planes of the manganese tantalate expose at least one of the crystal planes (621), (211), and (200).

3. A method for preparing a facet-controlled supported manganese tantalate catalyst according to claim 1 or 2, characterized in that, Comprising: Performing a first mixing of water and glycerol to obtain a mixed solution; Performing a second mixing of the mixed solution with a manganese salt, an amino acid, a chloropyridine compound, and activated alumina to obtain a reaction precursor; Performing a third mixing of the reaction precursor and tantalum pentoxide and then performing a heat treatment to obtain the manganese tantalate.

4. The preparation method according to claim 3, wherein The volume ratio of the water to the glycerol is 1:0.5 - 1.

5. The preparation method according to claim 3, wherein The manganese salt includes at least one of manganese chloride, manganese sulfate, and manganese acetate.

6. The preparation method according to claim 3, characterized in that, Satisfying at least one of the following conditions: a. The amino acid includes alanine family amino acids; b. The activated alumina includes activated alumina spheres.

7. The preparation method according to claim 6, characterized in that, The alanine family amino acids include at least one of L-2-chlorophenylalanine, L-4-fluorophenylalanine, and Z-L-alanine.

8. The preparation method according to claim 3, characterized in that, The chloropyridine compound includes at least one of 6-chloro-2-hydroxymethylpyridine, dodecylpyridinium chloride, and 2-chloro-3-hydroxypyridine.

9. The preparation method according to claim 3, characterized in that, Satisfying at least one of the following conditions: c. The dosage relationship of the manganese salt, the amino acid, the chloropyridine compound, and the activated alumina is 0.5 - 1.0 mmol: 0.2 - 0.4 g: 0.1 - 0.2 g: 0.3 - 0.5 g; d. The dosage relationship of the mixed solution and the tantalum pentoxide is 15 mL: 1 - 2 mmol.

10. The preparation method according to any one of claims 3-9, characterized in that, The heat treatment is carried out under a closed condition, the temperature of the heat treatment is 100 - 140 °C, and the time is 4 - 8 hours.

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