Preparation method of Nb2O5@Ag3PO4 composite material

Abstract

The application belongs to the technical field of photocatalytic nanomaterials, and relates to a preparation method of Nb2O5@Ag3PO4 composite material, which comprises the following steps: a. dissolving niobium oxalate in a mixed solution of deionized water and hydrogen peroxide, and magnetically stirring to obtain solution A; b. adding ammonia water into solution A, magnetically stirring, and hydrothermally reacting, and then treating the product after the reaction to obtain white powder B; c. dissolving powder B in anhydrous ethanol, and ultrasonically and stirring to mix to form a uniform mixed solution C; d. respectively dissolving silver nitrate and sodium phosphate in deionized water to form solutions D and E for standby; e. dropping solution D into solution C at a certain rate to obtain solution F; f. dropping solution E into solution F at a certain rate, and then centrifuging, cleaning and drying at a constant temperature for a certain time to obtain the Nb2O5@Ag3PO4 composite material. The application has the advantages of simple process, low cost, short reaction period, no pollution to the environment, and visible light photocatalytic performance.

Description

Technical Field

[0001] This invention belongs to the field of photocatalytic nanomaterials and their preparation process technology and application, and relates to a method for preparing Nb2O5@Ag3PO4 composite material. Background Technology

[0002] Silver phosphate, as a powerful photocatalyst, possesses unparalleled advantages in solar energy conversion and photocatalytic degradation of water pollutants. Its quantum efficiency can reach 90% under visible light irradiation, surpassing most semiconductor photocatalytic materials. Furthermore, silver phosphate exhibits diverse morphologies, commonly including hierarchical porous structures, dendritic structures, nanorods, tetrapods, and spherical particles. With its wide bandgap (approximately 2.4 eV), silver phosphate can absorb visible light below 520 nm, and its low valence band position results in strong oxidation capabilities from photogenerated holes, thus demonstrating high activity in pollutant degradation.

[0003] Nb2O5 is a typical wide-bandgap n-type transition metal oxide semiconductor with low toxicity, resistance to photocorrosion, excellent chemical stability, and high specific surface area with specific surface acidic sites. These characteristics are beneficial for its application in the photocatalytic degradation of organic pollutants. Furthermore, it exhibits high stability and recyclability in most solvents. Summary of the Invention

[0004] The primary technical problem to be solved by this invention is to provide a method for preparing Nb2O5@Ag3PO4 composite material that is simple in process, low in cost, short in reaction cycle, uniform, and has good photocatalytic performance.

[0005] The present invention provides a technical solution comprising: a method for preparing Nb2O5@Ag3PO4 composite material, comprising the following steps: a. dissolving niobium oxalate in a mixed solution of deionized water and hydrogen peroxide, and stirring magnetically to dissolve it, obtaining solution A; b. adding ammonia to solution A, stirring magnetically, and performing a hydrothermal reaction. After the reaction is complete, the mixture is naturally cooled to room temperature, centrifuged, and the precipitate is washed with water and alcohol several times. The product is dried at a constant temperature, and the dried powder is then annealed in a muffle furnace to obtain white powder B; c. dissolving powder B in anhydrous ethanol, and mixing it by sonication and stirring to form a homogeneous solution C; d. dissolving silver nitrate and sodium phosphate in deionized water respectively to form solutions D and E for later use; e. adding solution D dropwise to solution C at a certain rate to obtain solution F; f. adding solution E dropwise to solution F at a certain rate, centrifuging after the reaction is complete, washing, and drying at a constant temperature for a certain time to obtain Nb2O5@Ag3PO4 composite material.

[0006] Furthermore, in step a, the amount of niobium oxalate is 0.403g-1.614g, the amount of deionized water is 15ml-60ml, and the stirring time is 15min-60min;

[0007] Further, in step b, the amount of ammonia is 0.05-0.5 ml, the stirring time is 15-60 min, the hydrothermal reaction temperature is 160-200℃, the hydrothermal reaction time is 10-14 h, the drying temperature is 50-70℃, the drying time is 6-14 h, the annealing temperature is 400-700℃, and the annealing time is 2-6 h;

[0008] Further, in step c, the amount of powder B is 26.6mg-79.8mg, the amount of ethanol is 50-200ml, the sonication time is 10-30min, and the stirring time is 10-30min;

[0009] Furthermore, in step d, the amount of silver nitrate is 12.7 mg-51 mg, the amount of sodium phosphate is 3 mg-16.3 mg, and the amount of deionized water is 5-20 ml;

[0010] Furthermore, the dropping rate in step e is 3-10 seconds / drop;

[0011] Furthermore, in step f, the dropping rate is 3-10 seconds / drop, followed by three washes with water and alcohol, drying at a temperature of 50-70℃, and drying time of 10-14 hours.

[0012] Beneficial effects:

[0013] This invention features a simple process, low cost, short reaction cycle, and no environmental pollution. It also exhibits visible light photocatalytic performance and has wide applications in the energy and environmental protection industries. The Nb₂O₅@Ag₃PO₄ composite material of this invention is a 1-3 micrometer cluster, composed of several stacked lamellar structures. The lamellar structures support granular structures, resulting in a large specific surface area for the Nb₂O₅@Ag₃PO₄ composite material. The radius of the electrochemical impedance spectroscopy spectrum of the Nb₂O₅@Ag₃PO₄ composite material is smaller than that of Nb₂O₅ and Ag₃PO₄, and the electrical properties of the Nb₂O₅@Ag₃PO₄ composite material are superior to those of Nb₂O₅ and Ag₃PO₄. Attached Figure Description

[0014] Figure 1 Scanning electron microscope image of Nb2O5@Ag3PO4 composite material.

[0015] Figure 2 Transmission electron microscope image of Nb2O5@Ag3PO4 composite material.

[0016] Figure 3 Electrochemical impedance spectroscopy (EIS) spectra of Nb2O5, Ag3PO4, and Nb2O5@Ag3PO4 composites. Detailed Implementation

[0017] The following specific embodiments are used to further illustrate the methods described in this invention, but it is not intended that this invention is limited to these embodiments.

[0018] Example 1:

[0019] A method for preparing a Nb2O5@Ag3PO4 composite material includes the following steps: a. Dissolving 0.807 g of niobium oxalate in 30 ml of a mixed solution (H2O:H2O2 = 1:1), and stirring magnetically for 30 min to ensure complete dissolution, obtaining solution A; b. Adding 0.1 ml of ammonia water to solution A, and stirring magnetically for 30 min to ensure complete dissolution, transferring the solution to a hydrothermal reactor, and reacting at 180 °C for 12 h. After the reaction is complete, allowing it to cool naturally to room temperature, centrifuging, and washing the precipitate three times with water and alcohol, placing the resulting precipitate in a drying oven, and drying at 60 °C for 12 h, then annealing the dried powder in a muffle furnace at 500 °C for 2 h, and cooling to room temperature after annealing to obtain white powder B; c. Dissolving 53.2 mg of powder B in 100 ml of anhydrous... d. In ethanol, sonicate and stir for 15 min to form a homogeneous mixed solution C; d. Dissolve 34 mg of silver nitrate and 10.86 mg of sodium phosphate in 13.6 ml and 6.6 ml of deionized water, respectively, and stir for 15 min to form solutions D and E for later use; e. Add solution D dropwise to solution C at a rate of 5 s / drop, while maintaining vigorous stirring. After solution D is completely added, continue vigorous stirring for 30 min to obtain solution F; f. Add the prepared solution E dropwise to solution F at a rate of 5 s / drop, while maintaining vigorous stirring. After solution E is completely added, continue vigorous stirring for 30 min. Centrifuge the mixed solution, wash the precipitate three times with water and alcohol, and place the resulting precipitate in a drying oven to dry at 60℃ for 12 h to obtain the Nb2O5@Ag3PO4 composite material. Figure 1 The image shown is a scanning electron microscope image of the Nb2O5@Ag3PO4 composite material obtained in this invention. As can be seen from the image, the obtained Nb2O5@Ag3PO4 composite material is in the form of 1-3 micrometer clusters, and the clustered Nb2O5@Ag3PO4 composite material is composed of several stacked plate-like structures. Figure 2 As shown, the sheet-like structure of the present invention supports a particulate structure, resulting in a large specific surface area for the Nb2O5@Ag3PO4 composite material. Figure 3The figure shows the electrochemical impedance spectroscopy of Nb2O5, Ag3PO4 and Nb2O5@Ag3PO4 composite materials of the present invention. As can be seen from the figure, the radius of the electrochemical impedance spectroscopy of the Nb2O5@Ag3PO4 composite material of the present invention is smaller than that of Nb2O5 and Ag3PO4, which makes the electrical performance of the Nb2O5@Ag3PO4 composite material better than that of Nb2O5 and Ag3PO4.

[0020] Example 2:

[0021] The difference between this embodiment and Example 1 is that the amounts of niobium oxalate and deionized water in step a are changed to 1.614 g and 60 ml, respectively. Everything else is the same as in Example 1, as follows: a. Dissolve 1.614 g of niobium oxalate in 60 ml of a mixed solution (H2O:H2O2 = 1:1), and stir magnetically for 30 min to ensure complete dissolution, obtaining solution A; b. Add 0.1 ml of ammonia water to solution A, stir magnetically for 30 min to ensure complete dissolution, transfer the solution to a hydrothermal reactor, and react at 180°C for 12 h. After the reaction is complete, allow it to cool naturally to room temperature, centrifuge, and wash the precipitate three times with water and alcohol. Place the precipitate in a drying oven and dry at 60°C for 12 h. Then, place the dried powder in a muffle furnace and anneal at 500°C for 2 h. After annealing, cool to room temperature to obtain white powder B; c. Take 53.2 mg of powder B... d. Dissolve 34 mg of silver nitrate and 10.86 mg of sodium phosphate in 13.6 ml and 6.6 ml of deionized water, respectively, and stir for 15 min to form solutions D and E for later use; e. Add solution D dropwise to solution C at 5 s / drop while maintaining vigorous stirring. After the addition of solution D is complete, continue vigorous stirring for 30 min to obtain solution F; f. Add the prepared solution E dropwise to solution F at 5 s / drop while maintaining vigorous stirring. After the addition of solution E is complete, continue vigorous stirring for 30 min. Centrifuge the mixed solution, wash the precipitate three times with water and alcohol, and place the resulting precipitate in a drying oven to dry at 60 °C for 12 h to obtain the Nb2O5@Ag3PO4 composite material.

[0022] The structure and properties of the Nb2O5@Ag3PO4 composite material of the present invention are similar to those of Example 1, and will not be repeated here.

[0023] Example 3:

[0024] The difference between this embodiment and Embodiment 1 is that the time in step a is halved to 15 minutes. Otherwise, it is the same as Embodiment 1, specifically as follows: a. Dissolve 0.807 g of niobium oxalate in 30 ml of a mixed solution (H2O:H2O2 = 1:1), and stir magnetically for 15 minutes to ensure complete dissolution, obtaining solution A; b. Add 0.1 ml of ammonia water to solution A, and stir magnetically for 30 minutes to ensure complete dissolution. Transfer the solution to a hydrothermal reactor and react at 180°C for 12 hours. After the reaction is complete, allow it to cool naturally to room temperature, centrifuge, and wash the precipitate three times with water and alcohol. Place the resulting precipitate in a dry place. Inside the oven, dry at 60℃ for 12 hours, then place the dried powder in a muffle furnace and anneal at 500℃ for 2 hours. After annealing, cool to room temperature to obtain white powder B; c. Dissolve 53.2 mg of powder B in 100 ml of anhydrous ethanol, sonicate and stir for 15 min to fully mix to form a homogeneous mixed solution C; d. Dissolve 34 mg of silver nitrate and 10.86 mg of sodium phosphate in 13.6 ml and 6.6 ml of deionized water respectively, stir for 15 min to form solution D. e. Add solution D dropwise to solution C at 5s / drop, while maintaining vigorous stirring. After solution D is completely added, continue vigorous stirring for 30 minutes to obtain solution F; f. Add the reserved solution E dropwise to solution F at 5s / drop, while maintaining vigorous stirring. After solution E is completely added, continue vigorous stirring for 30 minutes. Centrifuge the mixed solution, wash the precipitate three times with water and alcohol, and place the resulting precipitate in a drying oven to dry at 60°C for 12 hours to obtain the Nb2O5@Ag3PO4 composite material. The structure and properties of the Nb2O5@Ag3PO4 composite material of the present invention are similar to those of Example 1, and will not be described again here.

[0025] Example 4:

[0026] The difference between this embodiment and Embodiment 1 is that the amount of ammonia in step b is changed to 0.5 ml. Everything else is the same as in Embodiment 1, specifically as follows: a. Dissolve 0.807 g of niobium oxalate in 30 ml of a mixed solution (H2O:H2O2 = 1:1), and stir magnetically for 30 min to ensure complete dissolution, obtaining solution A; b. Add 0.5 ml of ammonia to solution A, and stir magnetically for 30 min to ensure complete dissolution. Transfer the solution to a hydrothermal reactor and react at 180°C for 12 h. After the reaction is complete, allow it to cool naturally to room temperature, centrifuge, and wash the precipitate three times with water and alcohol. Place the resulting precipitate in a dry place. Inside the oven, dry at 60℃ for 12 hours, then place the dried powder in a muffle furnace and anneal at 500℃ for 2 hours. After annealing, cool to room temperature to obtain white powder B; c. Dissolve 53.2 mg of powder B in 100 ml of anhydrous ethanol, sonicate and stir for 15 min to fully mix to form a homogeneous mixed solution C; d. Dissolve 34 mg of silver nitrate and 10.86 mg of sodium phosphate in 13.6 ml and 6.6 ml of deionized water respectively, stir for 15 min to form solution D. e. Add solution D dropwise to solution C at 5s / drop, while maintaining vigorous stirring. After solution D is completely added, continue vigorous stirring for 30 minutes to obtain solution F; f. Add the reserved solution E dropwise to solution F at 5s / drop, while maintaining vigorous stirring. After solution E is completely added, continue vigorous stirring for 30 minutes. Centrifuge the mixed solution, wash the precipitate three times with water and alcohol, and place the resulting precipitate in a drying oven to dry at 60°C for 12 hours to obtain the Nb2O5@Ag3PO4 composite material. The structure and properties of the Nb2O5@Ag3PO4 composite material of the present invention are similar to those of Example 1, and will not be described again here.

[0027] Example 5:

[0028] The difference between this embodiment and Embodiment 1 is that the stirring time in step b is changed to 15 min, while the rest is the same as in Embodiment 1, as follows: a. Dissolve 0.807 g of niobium oxalate in 30 ml of a mixed solution (H2O:H2O2 = 1:1), and stir magnetically for 30 min to ensure complete dissolution, obtaining solution A; b. Add 0.1 ml of ammonia water to solution A, and stir magnetically for 15 min to ensure complete dissolution. Transfer the solution to a hydrothermal reactor and react at 180°C for 12 h. After the reaction is complete, allow it to cool naturally to room temperature, centrifuge, and wash the precipitate three times with water and alcohol. Place the resulting precipitate in a dry place. Inside the oven, dry at 60℃ for 12 hours, then place the dried powder in a muffle furnace and anneal at 500℃ for 2 hours. After annealing, cool to room temperature to obtain white powder B; c. Dissolve 53.2 mg of powder B in 100 ml of anhydrous ethanol, sonicate and stir for 15 min to fully mix to form a homogeneous mixed solution C; d. Dissolve 34 mg of silver nitrate and 10.86 mg of sodium phosphate in 13.6 ml and 6.6 ml of deionized water respectively, stir for 15 min to form solution D. e. Add solution D dropwise to solution C at 5s / drop, while maintaining vigorous stirring. After solution D is completely added, continue vigorous stirring for 30 minutes to obtain solution F; f. Add the reserved solution E dropwise to solution F at 5s / drop, while maintaining vigorous stirring. After solution E is completely added, continue vigorous stirring for 30 minutes. Centrifuge the mixed solution, wash the precipitate three times with water and alcohol, and place the resulting precipitate in a drying oven to dry at 60°C for 12 hours to obtain the Nb2O5@Ag3PO4 composite material. The structure and properties of the Nb2O5@Ag3PO4 composite material of the present invention are similar to those of Example 1, and will not be described again here.

[0029] Example 6:

[0030] The difference between this embodiment and Embodiment 1 is that the reaction temperature in step b is 200℃. Everything else is the same as in Embodiment 1, specifically as follows: a. Dissolve 0.807g of niobium oxalate in 30ml of a mixed solution (H2O:H2O2 = 1:1), and stir magnetically for 30min to ensure complete dissolution, obtaining solution A; b. Add 0.1ml of ammonia water to solution A, and stir magnetically for 30min to ensure complete dissolution. Transfer the solution to a hydrothermal reactor and react at 200℃ for 12h. After the reaction is complete, allow it to cool naturally to room temperature, centrifuge, and collect the precipitate. Wash three times with alcohol, and place the resulting precipitate in a drying oven to dry at 60°C for 12 hours. Then, place the dried powder in a muffle furnace and anneal at 500°C for 2 hours. After annealing, cool to room temperature to obtain white powder B; c. Dissolve 53.2 mg of powder B in 100 ml of anhydrous ethanol, and sonicate and stir for 15 minutes to form a homogeneous mixed solution C; d. Dissolve 34 mg of silver nitrate and 10.86 mg of sodium phosphate in 13.6 ml and 6.6 ml of deionized water, respectively, and stir for 15 minutes to form solution D. e. Add solution D dropwise to solution C at 5s / drop, while maintaining vigorous stirring. After solution D is completely added, continue vigorous stirring for 30 minutes to obtain solution F; f. Add the reserved solution E dropwise to solution F at 5s / drop, while maintaining vigorous stirring. After solution E is completely added, continue vigorous stirring for 30 minutes. Centrifuge the mixed solution, wash the precipitate three times with water and alcohol, and place the resulting precipitate in a drying oven to dry at 60°C for 12 hours to obtain the Nb2O5@Ag3PO4 composite material. The structure and properties of the Nb2O5@Ag3PO4 composite material of the present invention are similar to those of Example 1, and will not be described again here.

[0031] Example 7:

[0032] The difference between this embodiment and Embodiment 1 is that the reaction time in step b is 14 hours. Everything else is the same as in Embodiment 1, as follows: a. Dissolve 0.807 g of niobium oxalate in 30 ml of a mixed solution (H₂O:H₂O₂ = 1:1), and stir magnetically for 30 minutes until fully dissolved to obtain solution A; b. Add 0.1 ml of ammonia water to solution A, and stir magnetically for 30 minutes until fully dissolved. Transfer the solution to a hydrothermal reactor and react at 180°C for 14 hours. After the reaction is complete, allow it to cool naturally to room temperature, centrifuge, and wash the precipitate with water. a. Wash the powder three times with alcohol, place the resulting precipitate in a drying oven and dry it at 60℃ for 12 hours. Then, anneal the dried powder in a muffle furnace at 500℃ for 2 hours. After annealing, cool it to room temperature to obtain white powder B; c. Dissolve 53.2 mg of powder B in 100 ml of anhydrous ethanol, sonicate and stir for 15 minutes to fully mix it to form a homogeneous mixed solution C; d. Dissolve 34 mg of silver nitrate and 10.86 mg of sodium phosphate in 13.6 ml and 6.6 ml of deionized water, respectively, and stir for 15 minutes to form solutions D and E. e. Add solution D dropwise to solution C at 5s / drop, while maintaining vigorous stirring. After solution D is completely added, continue vigorous stirring for 30 minutes to obtain solution F; f. Add the prepared solution E dropwise to solution F at 5s / drop, while maintaining vigorous stirring. After solution E is completely added, continue vigorous stirring for 30 minutes. Centrifuge the mixed solution, wash the precipitate three times with water and alcohol, and place the resulting precipitate in a drying oven to dry at 60°C for 12 hours to obtain the Nb2O5@Ag3PO4 composite material. The structure and properties of the Nb2O5@Ag3PO4 composite material of the present invention are similar to those of Example 1, and will not be described again here.

[0033] Example 8:

[0034] The difference between this embodiment and Embodiment 1 is that the drying temperature in step b is 70℃. Everything else is the same as in Embodiment 1, specifically as follows: a. Dissolve 0.807g of niobium oxalate in 30ml of a mixed solution (H2O:H2O2 = 1:1), and stir magnetically for 30min to ensure complete dissolution, obtaining solution A; b. Add 0.1ml of ammonia water to solution A, and stir magnetically for 30min to ensure complete dissolution. Transfer the solution to a hydrothermal reactor and react at 180℃ for 12h. After the reaction is complete, allow it to cool naturally to room temperature, centrifuge, and wash the precipitate with water. a. Wash the powder three times with alcohol, place the resulting precipitate in a drying oven and dry it at 70℃ for 12 hours. Then, anneal the dried powder in a muffle furnace at 500℃ for 2 hours. After annealing, cool it to room temperature to obtain white powder B; c. Dissolve 53.2 mg of powder B in 100 ml of anhydrous ethanol, sonicate and stir for 15 minutes to fully mix it to form a homogeneous mixed solution C; d. Dissolve 34 mg of silver nitrate and 10.86 mg of sodium phosphate in 13.6 ml and 6.6 ml of deionized water, respectively, and stir for 15 minutes to form solutions D and E. e. Add solution D dropwise to solution C at 5s / drop, while maintaining vigorous stirring. After solution D is completely added, continue vigorous stirring for 30 minutes to obtain solution F; f. Add the prepared solution E dropwise to solution F at 5s / drop, while maintaining vigorous stirring. After solution E is completely added, continue vigorous stirring for 30 minutes. Centrifuge the mixed solution, wash the precipitate three times with water and alcohol, and place the resulting precipitate in a drying oven to dry at 60°C for 12 hours to obtain the Nb2O5@Ag3PO4 composite material. The structure and properties of the Nb2O5@Ag3PO4 composite material of the present invention are similar to those of Example 1, and will not be described again here.

[0035] Example 9:

[0036] The difference between this embodiment and Embodiment 1 is that the drying time in step b is 14 hours. Everything else is the same as in Embodiment 1, specifically as follows: a. Dissolve 0.807 g of niobium oxalate in 30 ml of a mixed solution (H2O:H2O2 = 1:1), and stir magnetically for 30 minutes to ensure complete dissolution, obtaining solution A; b. Add 0.1 ml of ammonia water to solution A, and stir magnetically for 30 minutes to ensure complete dissolution. Transfer the solution to a hydrothermal reactor and react at 180°C for 12 hours. After the reaction is complete, allow it to cool naturally to room temperature, centrifuge, and wash the precipitate with water. a. Wash the powder three times with alcohol, place the resulting precipitate in a drying oven and dry it at 60℃ for 14 hours. Then, place the dried powder in a muffle furnace and anneal it at 500℃ for 2 hours. After annealing, cool it to room temperature to obtain white powder B; c. Dissolve 53.2 mg of powder B in 100 ml of anhydrous ethanol, sonicate and stir for 15 min to fully mix it to form a homogeneous mixed solution C; d. Dissolve 34 mg of silver nitrate and 10.86 mg of sodium phosphate in 13.6 ml and 6.6 ml of deionized water, respectively, and stir for 15 min to form solutions D and E. e. Add solution D dropwise to solution C at 5s / drop, while maintaining vigorous stirring. After solution D is completely added, continue vigorous stirring for 30 minutes to obtain solution F; f. Add the prepared solution E dropwise to solution F at 5s / drop, while maintaining vigorous stirring. After solution E is completely added, continue vigorous stirring for 30 minutes. Centrifuge the mixed solution, wash the precipitate three times with water and alcohol, and place the resulting precipitate in a drying oven to dry at 60°C for 12 hours to obtain the Nb2O5@Ag3PO4 composite material. The structure and properties of the Nb2O5@Ag3PO4 composite material of the present invention are similar to those of Example 1, and will not be described again here.

[0037] Example 10:

[0038] The difference between this embodiment and Embodiment 1 is that the annealing temperature in step b is 600℃. Everything else is the same as in Embodiment 1, specifically as follows: a. Dissolve 0.807g of niobium oxalate in 30ml of a mixed solution (H2O:H2O2 = 1:1), and stir magnetically for 30min to ensure complete dissolution, obtaining solution A; b. Add 0.1ml of ammonia water to solution A, and stir magnetically for 30min to ensure complete dissolution. Transfer the solution to a hydrothermal reactor and react at 180℃ for 12h. After the reaction is complete, allow it to cool naturally to room temperature, centrifuge, and collect the precipitate. Wash three times with alcohol, and place the resulting precipitate in a drying oven to dry at 60°C for 12 hours. Then, place the dried powder in a muffle furnace and anneal at 600°C for 2 hours. After annealing, cool to room temperature to obtain white powder B; c. Dissolve 53.2 mg of powder B in 100 ml of anhydrous ethanol, and sonicate and stir for 15 minutes to form a homogeneous mixed solution C; d. Dissolve 34 mg of silver nitrate and 10.86 mg of sodium phosphate in 13.6 ml and 6.6 ml of deionized water, respectively, and stir for 15 minutes to form solution D. e. Add solution D dropwise to solution C at 5s / drop, while maintaining vigorous stirring. After solution D is completely added, continue vigorous stirring for 30 minutes to obtain solution F; f. Add the reserved solution E dropwise to solution F at 5s / drop, while maintaining vigorous stirring. After solution E is completely added, continue vigorous stirring for 30 minutes. Centrifuge the mixed solution, wash the precipitate three times with water and alcohol, and place the resulting precipitate in a drying oven to dry at 60°C for 12 hours to obtain the Nb2O5@Ag3PO4 composite material. The structure and properties of the Nb2O5@Ag3PO4 composite material of the present invention are similar to those of Example 1, and will not be described again here.

[0039] Example 11:

[0040] The difference between this embodiment and Embodiment 1 is that the annealing time in step b is 4 hours. Everything else is the same as in Embodiment 1, specifically as follows: a. Dissolve 0.807 g of niobium oxalate in 30 ml of a mixed solution (H2O:H2O2 = 1:1), and stir magnetically for 30 minutes until fully dissolved to obtain solution A; b. Add 0.1 ml of ammonia water to solution A, and stir magnetically for 30 minutes until fully dissolved. Transfer the solution to a hydrothermal reactor and react at 180°C for 12 hours. After the reaction is complete, allow it to cool naturally to room temperature, centrifuge, and wash the precipitate with water. Wash the powder three times with alcohol, place the resulting precipitate in a drying oven and dry it at 60°C for 12 hours. Then, anneal the dried powder in a muffle furnace at 500°C for 4 hours. After annealing, cool it to room temperature to obtain white powder B; c. Dissolve 53.2 mg of powder B in 100 ml of anhydrous ethanol, sonicate and stir for 15 minutes to fully mix it to form a homogeneous mixed solution C; d. Dissolve 34 mg of silver nitrate and 10.86 mg of sodium phosphate in 13.6 ml and 6.6 ml of deionized water, respectively, and stir for 15 minutes to form solutions D and E. e. Add solution D dropwise to solution C at 5s / drop, while maintaining vigorous stirring. After solution D is completely added, continue vigorous stirring for 30 minutes to obtain solution F; f. Add the prepared solution E dropwise to solution F at 5s / drop, while maintaining vigorous stirring. After solution E is completely added, continue vigorous stirring for 30 minutes. Centrifuge the mixed solution, wash the precipitate three times with water and alcohol, and place the resulting precipitate in a drying oven to dry at 60°C for 12 hours to obtain the Nb2O5@Ag3PO4 composite material. The structure and properties of the Nb2O5@Ag3PO4 composite material of the present invention are similar to those of Example 1, and will not be described again here.

[0041] Example 12:

[0042] The difference between this embodiment and Embodiment 1 is that the amount of powder B in step c is changed to 79.8 mg. Everything else is the same as in Embodiment 1, specifically as follows: a. Dissolve 0.807 g of niobium oxalate in 30 ml of a mixed solution (H2O:H2O2 = 1:1), and stir magnetically for 30 min to ensure complete dissolution, obtaining solution A; b. Add 0.1 ml of ammonia water to solution A. In the middle, magnetically stir for 30 minutes to fully dissolve it, transfer the solution to a hydrothermal reactor, react at 180℃ for 12 hours, after the reaction is complete, allow it to cool naturally to room temperature, centrifuge, wash the precipitate with water and alcohol three times, place the precipitate in a drying oven, dry at 60℃ for 12 hours, then place the dried powder in a muffle furnace and anneal at 500℃ for 2 hours, after annealing is complete and cool to room temperature to obtain white powder B; c. Dissolve 79.8 mg of powder B in 100 ml of anhydrous ethanol, sonicate and stir for 15 minutes to fully mix to form a homogeneous mixed solution C; d. Add 34 mg of silver nitrate and 10.86 mg of phosphoric acid respectively. Sodium was dissolved in 13.6 ml and 6.6 ml of deionized water and stirred for 15 min to form solutions D and E for later use. e. Solution D was added dropwise to solution C at 5 s / drop while maintaining vigorous stirring. After the addition of solution D was complete, vigorous stirring was continued for 30 min to obtain solution F. f. The prepared solution E was added dropwise to solution F at 5 s / drop while maintaining vigorous stirring. After the addition of solution E was complete, vigorous stirring was continued for 30 min. The mixed solution was centrifuged, and the precipitate was washed three times with water and alcohol. The resulting precipitate was placed in a drying oven and dried at 60°C for 12 h to obtain the Nb2O5@Ag3PO4 composite material. The structure and properties of the Nb2O5@Ag3PO4 composite material of the present invention are similar to those of Example 1, and will not be described again here.

[0043] Example 13:

[0044] The difference between this embodiment and Embodiment 1 is that the amount of ethanol in step c is changed to 200 ml. Everything else is the same as in Embodiment 1, as follows: a. Dissolve 0.807 g of niobium oxalate in 30 ml of a mixed solution (H2O:H2O2 = 1:1), and stir magnetically for 30 min to ensure complete dissolution, obtaining solution A; b. Add 0.1 ml of ammonia water to solution A, and stir magnetically for 30 min to ensure complete dissolution. Transfer the solution to a hydrothermal reactor and react at 180°C for 12 h. After the reaction is complete, allow it to cool naturally to room temperature, centrifuge, and wash the precipitate three times with water and alcohol. Place the precipitate in a drying oven and dry at 60°C for 12 h. Then, place the dried powder in a muffle furnace and anneal at 500°C for 2 h. After annealing, cool to room temperature to obtain white powder B; c. Dissolve 53.2 mg of powder B in 200 ml of anhydrous ethanol, and sonicate and stir for 1 minute. d. Mix thoroughly for 5 minutes to form a homogeneous mixed solution C; d. Dissolve 34 mg of silver nitrate and 10.86 mg of sodium phosphate in 13.6 ml and 6.6 ml of deionized water, respectively, and stir for 15 minutes to form solutions D and E for later use; e. Add solution D dropwise to solution C at 5 s / drop while maintaining vigorous stirring. After the addition of solution D is complete, continue vigorous stirring for 30 minutes to obtain solution F; f. Add the prepared solution E dropwise to solution F at 5 s / drop while maintaining vigorous stirring. After the addition of solution E is complete, continue vigorous stirring for 30 minutes. Centrifuge the mixed solution, wash the precipitate three times with water and alcohol, and place the resulting precipitate in a drying oven to dry at 60°C for 12 hours to obtain the Nb2O5@Ag3PO4 composite material. The structure and properties of the Nb2O5@Ag3PO4 composite material of the present invention are similar to those of Example 1, and will not be described again here.

[0045] Example 14:

[0046] The difference between this embodiment and Embodiment 1 is that the ultrasonic and stirring time in step c is changed to 30 min. The rest is the same as Embodiment 1, as follows: a. Dissolve 0.807 g of niobium oxalate in 30 ml of a mixed solution (H2O:H2O2 = 1:1), and stir magnetically for 30 min to ensure complete dissolution, obtaining solution A; b. Add 0.1 ml of ammonia water to solution A, and stir magnetically for 30 min to ensure complete dissolution. Transfer the solution to a hydrothermal reactor and react at 180°C for 12 h. After the reaction is complete, allow it to cool naturally to room temperature, centrifuge, and wash the precipitate three times with water and alcohol. Place the precipitate in a drying oven and dry at 60°C for 12 h. Then, place the dried powder in a muffle furnace and anneal at 500°C for 2 h. After annealing, cool to room temperature to obtain white powder B; c. Dissolve 53.2 mg of powder B in 100 ml of anhydrous ethanol, and ultrasonically and stir for 30 min to ensure thorough mixing, forming a homogeneous mixed solution C; d. Dissolve 34 mg of... Silver nitrate and 10.86 mg sodium phosphate were dissolved in 13.6 ml and 6.6 ml of deionized water, respectively, and stirred for 15 min to form solutions D and E for later use. e. Solution D was added dropwise to solution C at 5 s / drop, while maintaining vigorous stirring. After the addition of solution D was completed, vigorous stirring was continued for 30 min to obtain solution F. f. The prepared solution E was added dropwise to solution F at 5 s / drop, while maintaining vigorous stirring. After the addition of solution E was completed, vigorous stirring was continued for 30 min. The mixed solution was centrifuged, and the precipitate was washed three times with water and alcohol. The resulting precipitate was placed in a drying oven and dried at 60 °C for 12 h to obtain the Nb2O5@Ag3PO4 composite material. The structure and properties of the Nb2O5@Ag3PO4 composite material of the present invention are similar to those of Example 1, and will not be described again here.

[0047] Example 15:

[0048] The difference between this embodiment and Example 1 is that the amounts of silver nitrate and sodium phosphate in step d are changed to 51 mg and 16.3 mg, respectively. The rest is the same as in Example 1, as follows: a. Dissolve 0.807 g of niobium oxalate in 30 ml of a mixed solution (H2O:H2O2 = 1:1), and stir magnetically for 30 min to ensure complete dissolution, obtaining solution A; b. Add 0.1 ml of ammonia water to solution A, stir magnetically for 30 min to ensure complete dissolution, transfer the solution to a hydrothermal reactor, and react at 180°C for 12 h. After the reaction is complete, allow it to cool naturally to room temperature, centrifuge, and wash the precipitate three times with water and alcohol. Place the precipitate in a drying oven and dry at 60°C for 12 h. Then, place the dried powder in a muffle furnace and anneal at 500°C for 2 h. After annealing, cool to room temperature to obtain white powder B; c. Take 53.2 mg of powder B... Dissolve in 100 ml of anhydrous ethanol, sonicate and stir for 15 min to form a homogeneous mixed solution C; d. Dissolve 51 mg of silver nitrate and 16.3 mg of sodium phosphate in 13.6 ml and 6.6 ml of deionized water respectively, stir for 15 min to form solutions D and E for later use; e. Add solution D dropwise to solution C at 5 s / drop, while maintaining vigorous stirring. After solution D is completely added, continue vigorous stirring for 30 min to obtain solution F; f. Add the prepared solution E dropwise to solution F at 5 s / drop, while maintaining vigorous stirring. After solution E is completely added, continue vigorous stirring for 30 min. Centrifuge the mixed solution, wash the precipitate three times with water and alcohol, place the precipitate in a drying oven and dry at 60 °C for 12 h to obtain the Nb2O5@Ag3PO4 composite material. The structure and properties of the Nb2O5@Ag3PO4 composite material of the present invention are similar to those of Example 1, and will not be described again here.

[0049] Example 16:

[0050] The difference between this embodiment and Example 1 is that the amount of deionized water used to prepare silver nitrate and sodium phosphate in step d is changed to 20 ml and 10 mg, respectively. Everything else is the same as in Example 1, specifically as follows: a. Dissolve 0.807 g of niobium oxalate in 30 ml of a mixed solution (H2O:H2O2 = 1:1), and stir magnetically for 30 min to ensure complete dissolution, obtaining solution A; b. Add 0.1 ml of ammonia water to solution A, and stir magnetically for 30 min to ensure complete dissolution. Transfer the solution to a hydrothermal reactor and react at 180°C for 12 h. After the reaction is complete, allow it to cool naturally to room temperature, centrifuge, and wash the precipitate three times with water and alcohol. Place the precipitate in a drying oven and dry at 60°C for 12 h. Then, place the dried powder in a muffle furnace and anneal at 500°C for 2 h. After annealing, cool to room temperature to obtain white powder B; c. Add 53.2 mg Powder B was dissolved in 100 ml of anhydrous ethanol and ultrasonically stirred for 15 min to form a homogeneous mixed solution C; d. 34 mg of silver nitrate and 10.86 mg of sodium phosphate were dissolved in 20 ml and 10 ml of deionized water, respectively, and stirred for 15 min to form solutions D and E for later use; e. Solution D was added dropwise to solution C at 5 s / drop while maintaining vigorous stirring. After the addition of solution D was completed, vigorous stirring was continued for 30 min to obtain solution F; f. The prepared solution E was added dropwise to solution F at 5 s / drop while maintaining vigorous stirring. After the addition of solution E was completed, vigorous stirring was continued for 30 min. The mixed solution was centrifuged, and the precipitate was washed three times with water and alcohol. The resulting precipitate was placed in a drying oven and dried at 60 °C for 12 h to obtain the Nb2O5@Ag3PO4 composite material. The structure and properties of the Nb2O5@Ag3PO4 composite material of the present invention are similar to those of Example 1, and will not be described again here.

[0051] Example 17:

[0052] The difference between this embodiment and Embodiment 1 is that the dropping rate of the solution in step e is changed to 10 s / drop. Everything else is the same as in Embodiment 1, as follows: a. Dissolve 0.807 g of niobium oxalate in 30 ml of a mixed solution (H2O:H2O2 = 1:1), and stir magnetically for 30 min to ensure complete dissolution, obtaining solution A; b. Add 0.1 ml of ammonia water to solution A, and stir magnetically for 30 min to ensure complete dissolution. Transfer the solution to a hydrothermal reactor and react at 180°C for 12 h. After the reaction is complete, allow it to cool naturally to room temperature, centrifuge, and wash the precipitate three times with water and alcohol. Place the precipitate in a drying oven and dry at 60°C for 12 h. Then, place the dried powder in a muffle furnace and anneal at 500°C for 2 h. After annealing, cool to room temperature to obtain white powder B; c. Dissolve 53.2 mg of powder B in 100 ml of... d. In anhydrous ethanol, the solution was sonicated and stirred for 15 min to form a homogeneous mixed solution C; d. 34 mg of silver nitrate and 10.86 mg of sodium phosphate were dissolved in 13.6 ml and 6.6 ml of deionized water, respectively, and stirred for 15 min to form solutions D and E for later use; e. Solution D was added dropwise to solution C at 10 s / drop while maintaining vigorous stirring. After the addition of solution D was completed, vigorous stirring was continued for 30 min to obtain solution F; f. The prepared solution E was added dropwise to solution F at 5 s / drop while maintaining vigorous stirring. After the addition of solution E was completed, vigorous stirring was continued for 30 min. The mixed solution was centrifuged, and the precipitate was washed three times with water and alcohol. The resulting precipitate was placed in a drying oven and dried at 60 °C for 12 h to obtain the Nb2O5@Ag3PO4 composite material. The structure and properties of the Nb2O5@Ag3PO4 composite material of the present invention are similar to those of Example 1, and will not be described again here.

[0053] Example 18:

[0054] The difference between this embodiment and Embodiment 1 is that the dropping rate of the solution in step f is changed to 10 s / drop. Everything else is the same as in Embodiment 1, as follows: a. Dissolve 0.807 g of niobium oxalate in 30 ml of a mixed solution (H2O:H2O2 = 1:1), and stir magnetically for 30 min to ensure complete dissolution, obtaining solution A; b. Add 0.1 ml of ammonia water to solution A, stir magnetically for 30 min to ensure complete dissolution, transfer the solution to a hydrothermal reactor, and react at 180°C for 12 h. After the reaction is complete, allow it to cool naturally to room temperature, centrifuge, and wash the precipitate three times with water and alcohol. Place the precipitate in a drying oven and dry at 60°C for 12 h. Then, place the dried powder in a muffle furnace and anneal at 500°C for 2 h. After annealing, cool to room temperature to obtain white powder B; c. Dissolve 53.2 mg of powder B in 100 ml of... d. In anhydrous ethanol, the solution was sonicated and stirred for 15 min to form a homogeneous mixed solution C; d. 34 mg of silver nitrate and 10.86 mg of sodium phosphate were dissolved in 13.6 ml and 6.6 ml of deionized water, respectively, and stirred for 15 min to form solutions D and E for later use; e. Solution D was added dropwise to solution C at 5 s / drop, while maintaining vigorous stirring. After the addition of solution D was completed, vigorous stirring was continued for 30 min to obtain solution F; f. The prepared solution E was added dropwise to solution F at 10 s / drop, while maintaining vigorous stirring. After the addition of solution E was completed, vigorous stirring was continued for 30 min. The mixed solution was centrifuged, and the precipitate was washed three times with water and alcohol. The resulting precipitate was placed in a drying oven and dried at 60 °C for 12 h to obtain the Nb2O5@Ag3PO4 composite material. The structure and properties of the Nb2O5@Ag3PO4 composite material of the present invention are similar to those of Example 1, and will not be described again here.

[0055] Example 19:

[0056] The difference between this embodiment and Embodiment 1 is that the drying temperature in step f is 70℃, while the rest is the same as in Embodiment 1, as follows: a. Dissolve 0.807g of niobium oxalate in 30ml of a mixed solution (H2O:H2O2 = 1:1), and stir magnetically for 30min to ensure complete dissolution, obtaining solution A; b. Add 0.1ml of ammonia water to solution A, and stir magnetically for 30min to ensure complete dissolution. Transfer the solution to a hydrothermal reactor and react at 180℃ for 12h. After the reaction is complete, allow it to cool naturally to room temperature, centrifuge, and remove the precipitate water. Wash three times with alcohol, and place the resulting precipitate in a drying oven to dry at 60°C for 12 hours. Then, place the dried powder in a muffle furnace and anneal at 500°C for 2 hours. After annealing, cool to room temperature to obtain white powder B; c. Dissolve 53.2 mg of powder B in 100 ml of anhydrous ethanol, and sonicate and stir for 15 minutes to form a homogeneous mixed solution C; d. Dissolve 34 mg of silver nitrate and 10.86 mg of sodium phosphate in 13.6 ml and 6.6 ml of deionized water, respectively, and stir for 15 minutes to form solution D. e. Add solution D dropwise to solution C at 5s / drop, while maintaining vigorous stirring. After solution D is completely added, continue vigorous stirring for 30 minutes to obtain solution F; f. Add the reserved solution E dropwise to solution F at 5s / drop, while maintaining vigorous stirring. After solution E is completely added, continue vigorous stirring for 30 minutes. Centrifuge the mixed solution, wash the precipitate three times with water and alcohol, and place the resulting precipitate in a drying oven to dry at 70°C for 12 hours to obtain the Nb2O5@Ag3PO4 composite material. The structure and properties of the Nb2O5@Ag3PO4 composite material of the present invention are similar to those of Example 1, and will not be described again here.

[0057] Example 20:

[0058] The difference between this embodiment and Embodiment 1 is that the drying time in step f is 14 hours. Everything else is the same as in Embodiment 1, specifically as follows: a. Dissolve 0.807 g of niobium oxalate in 30 ml of a mixed solution (H2O:H2O2 = 1:1), and stir magnetically for 30 minutes to ensure complete dissolution, obtaining solution A; b. Add 0.1 ml of ammonia water to solution A, and stir magnetically for 30 minutes to ensure complete dissolution. Transfer the solution to a hydrothermal reactor and react at 180°C for 12 hours. After the reaction is complete, allow it to cool naturally to room temperature, centrifuge, and collect the precipitate. Wash three times with alcohol, and place the resulting precipitate in a drying oven to dry at 60°C for 12 hours. Then, place the dried powder in a muffle furnace and anneal at 500°C for 2 hours. After annealing, cool to room temperature to obtain white powder B; c. Dissolve 53.2 mg of powder B in 100 ml of anhydrous ethanol, and sonicate and stir for 15 minutes to form a homogeneous mixed solution C; d. Dissolve 34 mg of silver nitrate and 10.86 mg of sodium phosphate in 13.6 ml and 6.6 ml of deionized water, respectively, and stir for 15 minutes to form solution D. e. Add solution D dropwise to solution C at 5s / drop, while maintaining vigorous stirring. After solution D is completely added, continue vigorous stirring for 30 minutes to obtain solution F; f. Add the reserved solution E dropwise to solution F at 5s / drop, while maintaining vigorous stirring. After solution E is completely added, continue vigorous stirring for 30 minutes. Centrifuge the mixed solution, wash the precipitate three times with water and alcohol, and place the resulting precipitate in a drying oven to dry at 60°C for 14 hours to obtain the Nb2O5@Ag3PO4 composite material. The structure and properties of the Nb2O5@Ag3PO4 composite material of the present invention are similar to those of Example 1, and will not be described again here.

[0059] Example 21:

[0060] The difference between this embodiment and Embodiment 1 is that the H2O:H2O2 ratio in step a is 2:1. Everything else is the same as in Embodiment 1, specifically as follows: a. Dissolve 0.807g of niobium oxalate in 30ml of a mixed solution (H2O:H2O2 = 2:1), and stir magnetically for 30min to ensure complete dissolution, obtaining solution A; b. Add 0.1ml of ammonia water to solution A, and stir magnetically for 30min to ensure complete dissolution. Transfer the solution to a hydrothermal reactor and react at 180℃ for 12h. After the reaction is complete, allow it to cool naturally to room temperature, centrifuge, and collect the sediment. The precipitate was washed three times with water and alcohol. It was then placed in a drying oven and dried at 60°C for 12 hours. The dried powder was then annealed in a muffle furnace at 500°C for 2 hours. After annealing, it was cooled to room temperature to obtain white powder B. c. 53.2 mg of powder B was dissolved in 100 ml of anhydrous ethanol and sonicated and stirred for 15 minutes to form a homogeneous solution C. d. 34 mg of silver nitrate and 10.86 mg of sodium phosphate were dissolved in 13.6 ml and 6.6 ml of deionized water, respectively, and stirred for 15 minutes to form solution D. e. Add solution D dropwise to solution C at a rate of 5 drops / second, while maintaining vigorous stirring. After solution D is completely added, continue vigorous stirring for 30 minutes to obtain solution F; f. Add the reserved solution E dropwise to solution F at a rate of 5 drops / second, while maintaining vigorous stirring. After solution E is completely added, continue vigorous stirring for 30 minutes. Centrifuge the mixed solution, wash the precipitate three times with water and alcohol, and place the resulting precipitate in a drying oven to dry at 60°C for 12 hours to obtain the Nb2O5@Ag3PO4 composite material. The structure and properties of the Nb2O5@Ag3PO4 composite material of the present invention are similar to those of Example 1, and will not be described again here.

Claims

1. A method for preparing Nb2O5@Ag3PO4 composite material, characterized in that, Includes the following steps: a. Dissolve niobate in a mixed solution of deionized water and hydrogen peroxide, and stir magnetically to dissolve it, to obtain solution A; b. Add ammonia water to solution A, stir magnetically, and initiate a hydrothermal reaction. After the reaction is complete, allow it to cool naturally to room temperature, centrifuge, and wash the precipitate several times with water and alcohol. Dry the product at a constant temperature, and then anneal the dried powder in a muffle furnace to obtain white powder B; c. Dissolve powder B in anhydrous ethanol, sonicate and stir to form a homogeneous solution C; d. Dissolve silver nitrate and sodium phosphate in deionized water to form solutions D and E for later use; e. Add solution D dropwise to solution C at a certain rate to obtain solution F; f. Solution E is added dropwise to solution F at a certain rate. After the process is completed, the solution is centrifuged, washed, and dried at a constant temperature for a certain period of time to obtain the Nb2O5@Ag3PO4 composite material. The Nb2O5@Ag3PO4 composite material is a 1-3 micrometer cluster, which is composed of several sheet-like structures stacked together, and the sheet-like structures support the granular structures.

2. The method for preparing the Nb2O5@Ag3PO4 composite material as described in claim 1, characterized in that: In step a, the amount of niobium oxalate is 0.403-1.614 g, and the ratio of H2O to H2O2 is 5:1-1:2; the magnetic stirring time in step a is 15-60 min.

3. The method for preparing the Nb2O5@Ag3PO4 composite material as described in claim 1, characterized in that: In step b, the amount of ammonia is 0.05-0.5 ml, the stirring time is 15-60 min, the hydrothermal reaction temperature is 160-200℃, the hydrothermal reaction time is 10-14 h, the drying temperature is 50-70℃, the annealing temperature is 400-700℃, and the annealing time is 2-6 h.

4. The method for preparing the Nb2O5@Ag3PO4 composite material as described in claim 1, characterized in that: In step c, the amount of powder B is 26.6mg-79.8mg, the amount of ethanol is 50-200ml, the sonication time is 10-30min, and the stirring time is 10-30min.

5. The method for preparing the Nb2O5@Ag3PO4 composite material as described in claim 1, characterized in that: In step d, the amount of silver nitrate is 12.7-51 mg, the amount of sodium phosphate is 3-16.3 mg, and the amount of H2O is 5-20 ml.

6. The method for preparing the Nb2O5@Ag3PO4 composite material as described in claim 1, characterized in that: The dripping rate in step e is 3-10 seconds / drop.

7. The method for preparing the Nb2O5@Ag3PO4 composite material as described in claim 1, characterized in that: In step f, the dropping rate is 3-10 seconds / drop, the drying temperature is 50-70℃, and the drying time is 10-14 hours.

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