Manganese oxide positive electrode material regulated and controlled by dianion-doped synergistic structure and preparation method of manganese oxide positive electrode material

Abstract

The invention discloses a manganese oxide positive electrode material regulated and controlled by a dianion-doped synergistic structure and a preparation method of the manganese oxide positive electrode material, and belongs to the technical field of battery materials. The method comprises the following steps: dissolving a manganese source in deionized water containing or not containing acid to obtain a solution A; dissolving a fluorine source and a nitrogen source in deionized water to obtain a solution B; adding the solution B into the solution A to obtain a solution C; transferring the solution C into a high-temperature reaction kettle, and carrying out hydrothermal reaction under the condition of 120-180 DEG C; after the reaction is finished, cooling to room temperature, and collecting and drying a product after suction filtration and cleaning. According to the invention, a one-step hydrothermal method is adopted to realize multi-strategy cooperative regulation, a Mn-N bond formed by doping weakens the interaction between Zn < 2 + > and lattice oxygen, and a Mn-F bond stabilizes a manganese oxide structure; the NH4 < + > intercalation expands the lattice spacing, the oxygen vacancy increases the Zn < 2 + > storage site and enhances the conductivity, the barrier of structure collapse caused by the high diffusion demand in the manganese oxide material is broken through the multi-strategy cooperation, and the high diffusion dynamics and the structure stability of the manganese oxide material are synchronously realized.

Description

TECHNICAL FIELD

[0001] The application belongs to the technical field of battery materials, and particularly relates to a positive electrode material of an aqueous zinc-ion battery, and in particular to a manganese oxide positive electrode material doped with two anions and synergistically regulated by a structure and a preparation method thereof. BACKGROUND

[0002] An aqueous zinc-ion battery (AZIB) is a secondary battery taking zinc (or zinc alloy) as a negative electrode, a transition metal compound (such as manganese-based / vanadium-based oxide, Prussian blue, etc.) as a positive electrode, and a neutral or weak acid zinc salt aqueous solution as an electrolyte. The core working principle is to realize the conversion between electric energy and chemical energy through the reversible intercalation / deintercalation of zinc ions (Zn 2+ ) between the positive and negative electrodes during charging and discharging. The aqueous zinc-ion battery has become a research focus for future large-scale energy storage applications due to the high natural abundance, high theoretical specific capacity, relatively low redox potential and high safety of zinc element.

[0003] Compared with the current commercial lithium-ion battery, the aqueous zinc-ion battery has the advantages of safety and low cost, and becomes an important supplement to the new power battery taking lithium resources as the core. The positive electrode material is an important factor determining the electrochemical performance of the aqueous zinc-ion battery. Among various positive electrode materials, the manganese oxide positive electrode material, especially the layered manganese oxide, is considered as one of the most potential positive electrode candidate materials due to the advantages of high theoretical capacity, suitable working voltage and adjustable interlayer spacing structure. However, in practical applications, Zn 2+ has a strong interaction with the main layer lattice oxygen of MnO2, resulting in large ion diffusion resistance and easy collapse of the structure; the small lattice spacing makes the Zn 2+ intercalation / deintercalation process difficult; in addition, the small number of active sites and poor conductivity result in low zinc storage capacity and low cycle life.

[0004] Existing modification strategies, such as single doping, simple intercalation and compounding, cannot simultaneously solve the synergistic optimization between ion diffusion rate, structural stability, active site and conductivity. Even the double doping strategy also only regulates the electronic structure of manganese oxide, ignoring the correlation between ion diffusion channels and active sites. Although various ion intercalation can expand the lattice spacing to a certain extent and improve the ion diffusion rate, it has little contribution to the structural stability, and the simple intercalation strategy cannot effectively increase the active sites and improve the conductivity. Therefore, it is of great significance to develop a manganese oxide positive electrode material with multiple strategies for synergistic optimization. SUMMARY

[0005] In view of the shortcomings of the existing technology, the purpose of the present invention is to provide a manganese oxide positive electrode material with double anion doping and synergistic structure regulation and a preparation method thereof. The material has the advantages of cheap raw materials, simple and easy preparation process, and mass production. By constructing the multi-synergistic effects of Mn-N bonds, Mn-F bonds, oxygen vacancies and expanding the interlayer spacing, the structure of the manganese oxide material is modified and used as the positive electrode of aqueous zinc ion batteries, significantly improving the material's specific capacity, rate performance and cycle stability.

[0006] In order to achieve the above technical objectives, the inventors innovatively synthesized N and F co-doped layered manganese oxide (N / F-MnO2) by a one-step hydrothermal method based on the electronegativity gradient to regulate the ionic bonding strength. The Mn-N bond formed by low electronegativity N doping weakens the covalent nature of the Mn-O bond, which can reduce the Zn 2+ Electrostatic interaction with lattice oxygen helps Zn 2+ Deintercalation; the strong polar Mn-F bond formed by high electronegativity F doping can suppress Jahn-Teller distortion and Mn 3+ dissolve, improve structural stability. At the same time, the synthesis process introduces more oxygen vacancies and expands the lattice spacing, increasing the Zn 2+ storage sites, enhanced material conductivity and Zn 2+ Diffusion dynamics. The synergistic advantages of multiple dimensions help improve the zinc storage performance of N / F-MnO2.

[0007] Specifically, the technical purpose of the present invention is achieved as follows: a manganese oxide positive electrode material with double anion doping and coordinated structure regulation, and a preparation method and application thereof, the method comprising the following steps:

[0008] Step 1: adding a manganese source consisting of potassium permanganate and a divalent manganese salt into deionized water or deionized water containing an acid, stirring and dissolving at room temperature to obtain a solution A;

[0009] Step 2: dissolving a fluorine source and a nitrogen source in deionized water, wherein the molar ratio of fluorine in the fluorine source to nitrogen in the nitrogen source is (0.8-1.2): (0.8-1.2), and stirring at room temperature to dissolve to obtain solution B;

[0010] Step 3: Add solution B to solution A to obtain solution C; transfer solution C to a high-temperature reactor and perform a hydrothermal reaction at 120-180°C for 12-36 hours;

[0011] Step 4: After the reaction is completed, the reactor is naturally cooled to room temperature, the product is filtered and washed, and dried to obtain a double anion-doped manganese oxide positive electrode material.

[0012] Further preferably, in the above method for preparing a manganese oxide positive electrode material with double anion doping and coordinated structure regulation, the divalent manganese salt in step 1 is selected from one or more of the following: manganese chloride, manganese sulfate, manganese nitrate, and manganese acetate; and the acid is selected from one or more of the following: hydrochloric acid, sulfuric acid, nitric acid, and acetic acid.

[0013] Further preferably, in the method for preparing the manganese oxide positive electrode material with double anion doping and coordinated structure regulation as described above, the molar ratio of potassium permanganate to divalent manganese salt in step 1 is (4-10):1.

[0014] Further preferably, in the method for preparing the manganese oxide positive electrode material with double anion doping and coordinated structure regulation as described above, the molar ratio of the hydrogen content of the acid to potassium permanganate in step 1 is (0.1-4):1.

[0015] Further preferably, in the method for preparing a manganese oxide positive electrode material with double anion doping and coordinated structural regulation as described above, the fluorine source in step 2 is selected from one or more of the following: ammonium fluoride, sodium fluoride, potassium fluoride; and the nitrogen source is selected from one or more of the following: ammonium fluoride, ammonium chloride, and ammonium sulfate.

[0016] Still further preferably, in the method for preparing the manganese oxide positive electrode material with double anion doping and coordinated structure regulation as described above, the molar ratio of the fluorine source, nitrogen source and manganese source in step 2 is (0.8-1.2): (0.8-1.2): (12-30).

[0017] Further preferably, in the above-mentioned method for preparing manganese oxide positive electrode materials with double anion doping and coordinated structure regulation, the temperature of the hydrothermal reaction in step 3 is 150-180° C., and the reaction time is 12-24 h.

[0018] Further preferably, in the above-mentioned method for preparing manganese oxide positive electrode materials with double anion doping and coordinated structure regulation, the reactor described in step 3 is a high-temperature reactor lined with polytetrafluoroethylene.

[0019] Further preferably, in the method for preparing the manganese oxide positive electrode material with double anion doping and coordinated structure regulation as described above, the filtration in step 4 is performed with alternate washing with deionized water and ethanol for 2 to 6 times.

[0020] Further preferably, in the method for preparing the manganese oxide positive electrode material with coordinated structure regulation by double anion doping as described above, the product obtained after filtration and washing in step 4 is dried in a vacuum drying oven at a drying temperature of 50 to 70°C, a drying time of 6 to 18 hours, and a vacuum degree of approximately -70 to -90 kPa.

[0021] In addition, the present invention also provides a manganese oxide positive electrode material with double anion doping and coordinated structure regulation prepared by the above method.

[0022] Compared with the existing manganese oxide positive electrode materials for aqueous zinc ion batteries, the manganese oxide positive electrode material with double anion doping and coordinated structure regulation prepared by the present invention and its preparation method have the following advantages and progress:

[0023] (1) The manganese oxide prepared by the present invention is a double anion (N, F) doped manganese oxide, and NH4 is introduced between the layers. + intercalation, and the introduction of oxygen vacancies in the layer.

[0024] (2) The Mn-N bond formed by low electronegativity N doping weakens the Zn 2+ Interaction with the lattice oxygen of the main layer of manganese oxide; the strong Mn-F bond formed by the highly electronegative F doping stabilizes the manganese oxide structure; NH4 + Intercalation expands the lattice spacing and slows down the Zn 2+ Diffusion resistance; increased oxygen vacancies not only provide Zn 2+ storage sites and enhance their conductivity.

[0025] (3) The coordinated regulation of multiple strategies optimized the zinc storage performance of manganese oxide materials, broke the barrier of structural collapse caused by high diffusion demand, and established a balance between high diffusion dynamics and structural stability.

[0026] (4) Compared with other synthetic methods, the one-step hydrothermal method used in the present invention has the advantages of cheap and readily available raw materials, simple and easy preparation process, and scalable production.

[0027] (5) The manganese oxide positive electrode material synthesized by the present invention with double anion doping and synergistic structure regulation has high rate performance and good cycle stability as the positive electrode of aqueous zinc ion batteries. It can provide a technical reference for the development of manganese oxide positive electrode materials and the modification of other layered materials, and has important research significance and application value. BRIEF DESCRIPTION OF THE DRAWINGS

[0028] Figure 1 This is an XRD pattern of a manganese oxide positive electrode material with double anion doping and coordinated structure regulation prepared in Example 1 of the present invention;

[0029] Figure 2 This is an SEM image of a manganese oxide positive electrode material with double anion doping and coordinated structure regulation prepared in Example 1 of the present invention;

[0030] Figure 3 This is a TEM-EDS mapping image of a manganese oxide positive electrode material with double anion doping and coordinated structure regulation prepared in Example 1 of the present invention;

[0031] Figure 4This is the F 1s XPS spectrum of a manganese oxide positive electrode material with double anion doping and coordinated structure regulation prepared in Example 1 of the present invention and an undoped manganese oxide material prepared in Comparative Example 1;

[0032] Figure 5 The N 1s XPS spectra of a manganese oxide positive electrode material with double anion doping and coordinated structure regulation prepared in Example 1 of the present invention and an undoped manganese oxide material prepared in Comparative Example 1;

[0033] Figure 6 HRTEM images of a manganese oxide positive electrode material with double anion doping and coordinated structure regulation prepared in Example 1 of the present invention and an undoped manganese oxide material prepared in Comparative Example 1;

[0034] Figure 7 This is an EPR graph of a manganese oxide positive electrode material with double anion doping and coordinated structure regulation prepared in Example 1 of the present invention and an undoped manganese oxide material prepared in Comparative Example 1;

[0035] Figure 8 GCD curves of a manganese oxide positive electrode material with double anion doping and coordinated structure regulation prepared in Example 1 of the present invention and an undoped manganese oxide material prepared in Comparative Example 1;

[0036] Figure 9 This is a comparison chart of the rate performance of a manganese oxide positive electrode material with double anion doping and coordinated structure regulation prepared in Example 1 of the present invention and an undoped manganese oxide material prepared in Comparative Example 1;

[0037] Figure 10 The impedance spectra of a manganese oxide positive electrode material with double anion doping and coordinated structure regulation prepared in Example 1 of the present invention and an undoped manganese oxide material prepared in Comparative Example 1;

[0038] Figure 11 GITT curves of a manganese oxide positive electrode material with double anion doping and coordinated structure regulation prepared in Example 1 of the present invention and an undoped manganese oxide material prepared in Comparative Example 1;

[0039] Figure 12 The double anion doped manganese oxide positive electrode material prepared in Example 1 of the present invention and the undoped manganese oxide material prepared in Comparative Example 1 are 1 A g –1 Cycling performance diagram under current density.

[0040] The present invention proposes a one-step hydrothermal method to prepare a manganese oxide positive electrode material with double anion doping and coordinated structure regulation, which is used as the positive electrode material of aqueous zinc ion battery. The Mn-N bond and Mn-F bond constructed by double anion doping effectively regulate the Zn 2+ Interaction with lattice oxygen and stability of manganese oxide structure.+ The introduction of and the increase of oxygen vacancy content not only expand the lattice spacing and slow down the Zn 2+ The invention reduces diffusion resistance, provides more zinc storage sites, and enhances conductivity. This multi-strategy synergistic regulation improves the rate capability and cycling stability of the manganese oxide positive electrode material. The preparation method of the present invention is described in detail below with reference to the accompanying drawings and specific examples, but the scope of protection of the present invention is not limited to the following examples.

[0041] Example 1:

[0042] A method for preparing a manganese oxide positive electrode material with double anion doping and coordinated structure regulation is specifically carried out according to the following steps:

[0043] In step 1, 0.1900 g (1.2 mmol) of potassium permanganate and 0.0340 g (0.2 mmol) of manganese sulfate monohydrate were dissolved in 20 mL of deionized water and stirred at room temperature to obtain solution A.

[0044] Step 2: Weigh 3.0 mg (0.08 mmol) of ammonium fluoride and dissolve it in 20 mL of deionized water. Stir and dissolve at room temperature to obtain Solution B.

[0045] Step 3: Add solution B to solution A to obtain solution C. Transfer solution C to a 50 mL polytetrafluoroethylene high-temperature reactor and perform a hydrothermal reaction at 160 °C for 12 h.

[0046] Step 4: After the reaction is completed, the reactor is naturally cooled to room temperature, and the product is washed alternately with deionized water and ethanol three times. The product is collected and dried in a vacuum drying oven at 60°C for 12 h with a vacuum degree of approximately -75 kPa to obtain a manganese oxide positive electrode material with a double anion doped and synergistic structure regulation.

[0047] Example 2:

[0048] A method for preparing a manganese oxide positive electrode material with double anion doping and coordinated structure regulation is specifically carried out according to the following steps:

[0049] In step 1, 0.1900 g (1.2 mmol) of potassium permanganate and 0.0340 g (0.2 mmol) of manganese sulfate monohydrate were dissolved in 20 mL of deionized water and stirred at room temperature to obtain solution A.

[0050] In step 2, 5.8 mg (0.1 mmol) of potassium fluoride and 6.6 mg (0.05 mmol) of ammonium sulfate were weighed and dissolved in 20 mL of deionized water. The mixture was stirred at room temperature to obtain solution B.

[0051] Step 3: Add solution B to solution A to obtain solution C. Transfer solution C to a 50 mL polytetrafluoroethylene high-temperature reactor and perform a hydrothermal reaction at 150 °C for 24 h.

[0052] Step 4: After the reaction is completed, the reactor is naturally cooled to room temperature, and the product is washed alternately with deionized water and ethanol three times. The product is collected and dried in a vacuum drying oven at 60°C for 12 h with a vacuum degree of approximately -80 kPa to obtain a manganese oxide positive electrode material with a double anion doped and synergistic structure regulation.

[0053] Example 3:

[0054] A method for preparing a manganese oxide positive electrode material with double anion doping and coordinated structure regulation is specifically carried out according to the following steps:

[0055] In step 1, 0.1900 g (1.2 mmol) of potassium permanganate, 0.0340 g (0.2 mmol) of manganese sulfate monohydrate, and 200 µL of 12 mol / L concentrated hydrochloric acid were dissolved in 20 mL of deionized water and stirred at room temperature to obtain solution A.

[0056] In step 2, 5.8 mg (0.1 mmol) of potassium fluoride and 7.9 mg (0.06 mmol) of ammonium sulfate were weighed and dissolved in 20 mL of deionized water. The mixture was stirred at room temperature to obtain solution B.

[0057] Step 3: Add solution B to solution A to obtain solution C. Transfer solution C to a 50 mL polytetrafluoroethylene high-temperature reactor and perform a hydrothermal reaction at 180 °C for 12 h.

[0058] Step 4: After the reaction is completed, the reactor is naturally cooled to room temperature, and the product is washed alternately with deionized water and ethanol three times. The product is collected and dried in a vacuum drying oven at 60°C for 12 h with a vacuum degree of approximately -75 kPa to obtain a manganese oxide positive electrode material with a double anion doped and synergistic structure regulation.

[0059] Example 4:

[0060] A method for preparing a manganese oxide positive electrode material with double anion doping and coordinated structure regulation is specifically carried out according to the following steps:

[0061] Step 1. Weigh 0.2530 g (1.6 mmol) of potassium permanganate, 0.0340 g (0.2 mmol) of manganese sulfate monohydrate, and 34 µL of 18 mol / L concentrated sulfuric acid and dissolve them in 20 mL of deionized water. Stir and mix at room temperature to obtain Solution A.

[0062] Step 2, 3.0 mg (0.08 mmol) of ammonium fluoride was weighed and dissolved in 20 mL of deionized water, and after stirring and dissolving at room temperature, solution B was obtained.

[0063] Step 3, solution B was added to solution A to obtain solution C. Solution C was transferred to a 50 mL polytetrafluoroethylene high-temperature reaction kettle, and a hydrothermal reaction was carried out at 150°C for 24 h.

[0064] Step 4, after the reaction was completed, the reaction kettle was naturally cooled to room temperature, and deionized water and ethanol were alternately washed 3 times, the product was collected, and dried in a vacuum drying box at 60°C for 12 h, with a vacuum degree of about -75 kPa, to obtain a dianion-doped synergistically-structured manganese oxide positive electrode material.

[0065] Example 5:

[0066] A preparation method of a dianion-doped synergistically-structured manganese oxide positive electrode material, specifically according to the following steps:

[0067] Step 1, 0.1900 g (1.2 mmol) of potassium permanganate, 0.0324 g (0.2 mmol) of manganese chloride, and 200 μL of 12 mol / L concentrated hydrochloric acid were dissolved in 20 mL of deionized water, and the mixture was stirred at room temperature to obtain solution A.

[0068] Step 2, 3.0 mg (0.08 mmol) of ammonium fluoride was weighed and dissolved in 20 mL of deionized water, and after stirring and dissolving at room temperature, solution B was obtained.

[0069] Step 3, solution B was added to solution A to obtain solution C. Solution C was transferred to a 50 mL polytetrafluoroethylene high-temperature reaction kettle, and a hydrothermal reaction was carried out at 160°C for 12 h.

[0070] Step 4, after the reaction was completed, the reaction kettle was naturally cooled to room temperature, and deionized water and ethanol were alternately washed 3 times, the product was collected, and dried in a vacuum drying box at 60°C for 12 h, with a vacuum degree of about -75 kPa, to obtain a dianion-doped synergistically-structured manganese oxide positive electrode material.

[0071] Comparative Example 1

[0072] A preparation method of a dianion-doped synergistically-structured manganese oxide positive electrode material, specifically according to the following steps:

[0073] Step 1, 0.1900 g (1.2 mmol) of potassium permanganate, 0.0340 g (0.2 mmol) of manganese sulfate monohydrate was dissolved in 40 mL of deionized water, and the mixture was stirred at room temperature.

[0074] Step 2: The obtained mixed solution was transferred to a 50 mL polytetrafluoroethylene high-temperature reactor and subjected to a hydrothermal reaction at 160 °C for 12 h.

[0075] Step 3: After the reaction is completed, the reactor is naturally cooled to room temperature, and the product is washed alternately with deionized water and ethanol three times. The product is collected and dried in a vacuum drying oven at 60°C for 12 h with a vacuum degree of about -75 kPa to obtain an undoped manganese oxide positive electrode material.

[0076] like Figure 1 : The figure shows the XRD pattern of a manganese oxide positive electrode material with double anion doping and coordinated structure control prepared in Example 1 of the present invention. From the spectrum analysis, it can be seen that the synthesized manganese oxide material can be clearly classified as δ-type layered manganese oxide.

[0077] like Figure 2 The figure shows an SEM image of a manganese oxide cathode material with double anion doping and coordinated structure regulation prepared in Example 1 of the present invention. As can be seen from the figure, its rich hierarchical porous structure increases the effective utilization of the material and shortens the diffusion path of ions.

[0078] like Figure 3 The figure shows a TEM-EDS mapping image of a manganese oxide cathode material with double anion doping and coordinated structure regulation prepared in Example 1 of the present invention. As can be seen from the figure, the sample contains five elements, K, Mn, O, N, and F, and their distribution is uniform, confirming the successful doping of N and F elements.

[0079] like Figure 4 As shown, the F 1s XPS spectra of a manganese oxide positive electrode material with double anion doping and coordinated structure regulation prepared in Example 1 of the present invention and the undoped manganese oxide material prepared in Comparative Example 1 further confirm the successful doping of the F element.

[0080] like Figure 5 As shown, the N 1s XPS spectra of a manganese oxide positive electrode material with double anion doping and coordinated structure regulation prepared in Example 1 of the present invention and the undoped manganese oxide material prepared in Comparative Example 1 further confirm the successful doping of the N element.

[0081] like Figure 6 The following are HRTEM images of a manganese oxide positive electrode material with double anion doping and coordinated structure regulation prepared in Example 1 of the present invention and an undoped manganese oxide material prepared in Comparative Example 1. As can be seen from the figure, the lattice spacing of the doped sample increases, confirming that the interlayer NH4 + The introduction of .

[0082] like Figure 7Figure 2 shows the EPR patterns of a manganese oxide cathode material with a double anion doping and coordinated structure regulation prepared in Example 1 of the present invention and an undoped manganese oxide material prepared in Comparative Example 1. As can be seen from the figure, the EPR signal at g = 2.002 is stronger in the doped sample, indicating a significant increase in oxygen vacancy concentration after doping.

[0083] like Figure 8 As shown in FIG1 , the GCD curves of a manganese oxide positive electrode material with double anion doping and coordinated structure regulation prepared in Example 1 of the present invention and the undoped manganese oxide material prepared in Comparative Example 1 are shown. As can be seen from the figure, at 0.1 A g –1 After 20 cycles of activation at the same current density, the capacity of the doped sample reached 496 mAh g –1 , which is significantly higher than that of the undoped sample (356 mAh g –1 ).

[0084] like Figure 9 Figure 2 shows a comparison of the rate performance of a manganese oxide cathode material with a double anion doping and coordinated structure control prepared in Example 1 of the present invention and an undoped manganese oxide material prepared in Comparative Example 1. As can be seen from the figure, at different current densities, the capacity of the doped sample is significantly higher than that of the undoped sample.

[0085] like Figure 10 Figure 2 shows the impedance spectra of a manganese oxide cathode material with a double anion doped and coordinated structure, prepared in Example 1 of the present invention, and an undoped manganese oxide material, prepared in Comparative Example 1. As can be seen from the figure, the charge transfer resistance of the doped sample is lower than that of the undoped sample, and the ion diffusion rate is higher than that of the undoped sample.

[0086] like Figure 11 The figure shows the GITT curves of a manganese oxide cathode material with double anion doping and coordinated structure regulation prepared in Example 1 of the present invention and an undoped manganese oxide material prepared in Comparative Example 1. It further confirms that the ion diffusion rate of the doped sample is higher than that of the undoped sample.

[0087] like Figure 12 As shown, the double anion doped manganese oxide positive electrode material prepared in Example 1 of the present invention and the undoped manganese oxide material prepared in Comparative Example 1 are shown in FIG. –1 Cycling performance diagram under current density. The doped sample cycled 600 times and the capacity was still as high as 181.8 mAh g –1 , which is better than the undoped sample (129.9 mAh g –1 ), showing good rate capacity and cycle stability, indicating that the manganese oxide positive electrode material with double anion doping and synergistic structure regulation has significant zinc storage advantages for zinc ion batteries.

Claims

1. A method for preparing a manganese oxide positive electrode material with double anion doping and coordinated structural regulation, characterized in that: The method comprises the following steps: Step 1: adding a manganese source consisting of potassium permanganate and a divalent manganese salt into deionized water or deionized water containing an acid, stirring and dissolving at room temperature to obtain a solution A; Step 2: dissolving a fluorine source and a nitrogen source in deionized water, wherein the molar ratio of fluorine in the fluorine source to nitrogen in the nitrogen source is (0.8-1.2): (0.8-1.2), and stirring at room temperature to dissolve to obtain solution B; Step 3: Add solution B to solution A to obtain solution C; transfer solution C to a high-temperature reactor and perform a hydrothermal reaction at 120-180°C for 12-36 hours; Step 4: After the reaction is completed, cool to room temperature, filter and wash the product, and dry it to obtain a double anion-doped manganese oxide positive electrode material.

2. The method for preparing a manganese oxide cathode material with double anion doping and coordinated structure regulation according to claim 1, characterized in that: The divalent manganese salt in step 1 is selected from one or more of the following: manganese chloride, manganese sulfate, manganese nitrate, and manganese acetate; and the acid is selected from one or more of the following: hydrochloric acid, sulfuric acid, nitric acid, and acetic acid.

3. The method for preparing a manganese oxide cathode material with double anion doping and coordinated structure regulation according to claim 1, characterized in that: In step 1, the molar ratio of potassium permanganate to divalent manganese salt is (4-10):

1.

4. The method for preparing a manganese oxide cathode material with double anion doping and coordinated structure regulation according to claim 1, characterized in that: The molar ratio of the hydrogen content of the acid to potassium permanganate in step 1 is (0.1-4):

1.

5. The method for preparing a manganese oxide cathode material with double anion doping and coordinated structure regulation according to claim 1, characterized in that: In step 2, the fluorine source is selected from one or more of the following: ammonium fluoride, sodium fluoride, and potassium fluoride; and the nitrogen source is selected from one or more of the following: ammonium fluoride, ammonium chloride, and ammonium sulfate.

6. The method for preparing a manganese oxide cathode material with double anion doping and coordinated structure regulation according to claim 5, characterized in that: The molar ratio of the fluorine source, nitrogen source and manganese source in step 2 is (0.8-1.2): (0.8-1.2): (12-30).

7. The method for preparing a manganese oxide cathode material with double anion doping and coordinated structure regulation according to claim 1, characterized in that: The temperature of the hydrothermal reaction in step 3 is 150-180°C, and the reaction time is 12-24 hours.

8. The method for preparing a manganese oxide cathode material with double anion doping and coordinated structure regulation according to claim 1, characterized in that: During the filtration in step 4, the product is washed alternately with deionized water and ethanol 2 to 6 times.

9. The method for preparing a manganese oxide cathode material with double anion doping and coordinated structure regulation according to claim 1, characterized in that: The product obtained after filtration and washing in step 4 is dried in a vacuum drying oven at a drying temperature of 50 to 70° C., a drying time of 6 to 18 h, and a vacuum degree of -70 to -90 kPa.

10. A double anion doped manganese oxide positive electrode material prepared according to the method according to any one of claims 1 to 9.

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