Preparation method and application of polyacrylamide-based monatomic oxygen reduction catalyst

Abstract

The application discloses a preparation method and application of a polyacrylamide-based monatomic oxygen reduction catalyst, and comprises the following steps: (1) taking FeCl3, 1,10-phenanthroline, ultrapure water, acrylamide, N,N'-methylenebisacrylamide, potassium carbonate, zinc chloride and ammonium persulfate as raw materials, and performing a free radical polymerization reaction to obtain (ZnCl2+[Fe(Phen)3 3+ )@PAM; (2) sequentially performing vacuum drying, high-temperature annealing and pickling on the (ZnCl2+[Fe(Phen)3 3+ )@PAM prepared in the step (1) to obtain the polyacrylamide-based monatomic oxygen reduction catalyst. The application takes an iron (III)-o-phenanthroline complex (denoted as [Fe(Phen)3 3+ ) as an iron precursor, takes ZnCl2 as a high-temperature volatile salt template to modify a pore structure and prevent the occurrence of metal aggregation, takes APS as an initiator, and promotes the synthesis of a polyacrylamide hydrogel in a [Fe(Phen)3 3+ and ZnCl2 mixed solution through an in-situ polymerization method, and finally, the prepared catalyst can be used for electrocatalytic oxygen reduction reaction.

Description

Technical Field

[0001] This invention belongs to the field of catalyst technology, specifically relating to a method for preparing a polyacrylamide-based single-atom oxygen reduction catalyst and its application. Background Technology

[0002] In today's era, global warming, energy depletion, and the massive consumption of fossil fuels have attracted widespread attention, leading to extensive research focused on developing sustainable and green energy technologies. As a promising alternative to traditional fossil fuels, fuel cells have garnered significant interest due to their high energy density and environmental friendliness. The energy conversion efficiency of fuel cells is primarily limited by the oxygen reduction reaction (ORR) at the cathode. Therefore, designing a rational and effective catalyst is crucial for addressing the crisis caused by fossil fuel consumption. Furthermore, high-performance OORR catalysts demonstrate immense application value and market potential in new energy vehicles, portable smart devices, and biomedical equipment.

[0003] Atomically dispersed transition metal-based catalysts (MNCs, M = Fe, Co, Ni, Zn, Cu, Mn) possess high atom utilization and excellent catalytic activity, making them the most promising candidates to replace noble metal-based catalysts. Among previously reported transition metal-based single-atom catalysts (SACs), Fe-NC catalysts exhibit the highest catalytic activity. Over the past decade, extensive research has focused on tuning the coordination environment and optimizing the pore structure of Fe-NC catalysts to further improve their performance. Metal-organic frameworks (MOFs), as an emerging type of crystalline porous material, possess ordered structures, controllable composition and porosity, and high specific surface area, and have been widely used as precursors / templates for Fe-NC catalysts. In particular, carbon-, nitrogen-rich, and microporous imidazolidinyl zeolite frameworks (ZIFs) have been widely used in the synthesis of Fe SACs.

[0004] However, the active centers of MOF-derived Fe-NC catalysts are typically in a four-coordinate structure of Fe-N4. The strong electronegativity of nitrogen affects the electronic properties of the active metal centers, thereby increasing the catalyst's free energy and hindering the adsorption and activation of oxygen reduction intermediates. Furthermore, the predominantly microporous structure of catalysts obtained from the pyrolysis of MOFs restricts the contact between active sites and accessible substances, significantly impacting mass transport and utilization at the active sites. Using MOFs as precursors / templates makes it difficult to achieve high performance by precisely tuning the local coordination environment and pore structure while easily preparing Fe SAC. Therefore, developing an excellent precursor capable of simultaneously altering electronic configuration and pore structure and easily synthesizing atomically dispersed oxygen reduction catalysts is highly attractive. Summary of the Invention

[0005] The purpose of this invention is to overcome the shortcomings of the prior art and provide a polyacrylamide-based single-atom oxygen reduction catalyst and its application.

[0006] The technical solution of the present invention is as follows:

[0007] A method for preparing a polyacrylamide-based single-atom oxygen reduction catalyst includes the following steps:

[0008] (1) Using FeCl3, 1,10-phenanthroline, ultrapure water, acrylamide, N,N'-methylenebisacrylamide, potassium carbonate, zinc chloride, and ammonium persulfate as raw materials, a free radical polymerization reaction was carried out to prepare (ZnCl2+[Fe(Phen)3)) 3+ @PAM;

[0009] (2) The (ZnCl2+[Fe(Phen)3) obtained in step (1) 3+ The polyacrylamide-based single-atom oxygen reduction catalyst was prepared by sequentially vacuum drying, high-temperature annealing (one-step pyrolysis) and acid washing of PAM.

[0010] In a preferred embodiment of the present invention, in step (1), the mass ratio of FeCl3, 1,10-phenanthroline, ultrapure water, acrylamide, N,N'-methylenebisacrylamide, potassium carbonate, zinc chloride and ammonium persulfate is 0.1-0.2:0.5-0.6:70-80:4-6:0.04-0.06:0.3-0.5:10-20:0.2-1.4.

[0011] More preferably, in step (1), the mass ratio of FeCl3, 1,10-phenanthroline, ultrapure water, acrylamide, N,N'-methylenebisacrylamide, potassium carbonate, zinc chloride and ammonium persulfate is 0.15:0.5055:75:5:0.05:0.4:15:0.2-1.4.

[0012] In a preferred embodiment of the present invention, the vacuum drying temperature is 75-85°C and the time is 90-100 hours.

[0013] More preferably, the vacuum drying temperature is 80°C and the time is 96 hours.

[0014] In a preferred embodiment of the present invention, the high-temperature annealing is: (ZnCl2+[Fe(Phen)3]) after vacuum drying 3+ PAM is heated to 480-520℃ in an argon atmosphere at a heating rate of 4-6℃ / min, annealed for 0.8-1.2h, then heated to 880-920℃ and held for 1.8-2.2h, and then cooled naturally.

[0015] More preferably, the high-temperature annealing is: (ZnCl2+[Fe(Phen)3]) after vacuum drying 3+ PAM was heated to 500°C in an argon atmosphere at a heating rate of 5°C / min, annealed for 1 hour, then heated to 900°C and held for 2 hours, and then cooled naturally.

[0016] In a preferred embodiment of the present invention, the pickling is performed by: pickling the material after high-temperature annealing with 1M hydrochloric acid for 8 hours, followed by thorough washing with a large amount of deionized water, and then drying at 80°C for 8 hours.

[0017] The application of the polyacrylamide-based single-atom oxygen reduction catalyst prepared by the above method in the preparation of energy storage and conversion devices.

[0018] A method for preparing energy storage and conversion devices comprising a polyacrylamide-based single-atom oxygen reduction catalyst prepared by the above method.

[0019] The beneficial effects of this invention are:

[0020] 1. This invention utilizes an iron(III)-o-phenanthroline complex (denoted as [Fe(Phen)3]). 3+ As an iron precursor, ZnCl2 is used as a high-temperature volatile salt template to modify the pore structure and prevent metal agglomeration. APS is used as an initiator to promote the formation of [Fe(Phen)3]... 3+ Polyacrylamide hydrogels were synthesized in situ via polymerization in a mixed solution of polyacrylamide and ZnCl2. The resulting catalyst can be used for electrocatalytic oxygen reduction reactions.

[0021] 2. This invention employs a simple and easy-to-implement APS-initiated acrylamide free radical polymerization and (ZnCl2+[Fe(Phen)3]) 3+ The PAM one-step pyrolysis strategy yielded an electrocatalyst with high oxygen reduction catalytic performance.

[0022] 3. This invention utilizes transition metal single atoms supported on carbon materials as active sites, giving them excellent electrocatalytic performance and achieving a highly efficient electrocatalytic oxygen reduction reaction. This enables them to be directly applied in fields such as electrochemical catalysis and fuel cells, and has great potential application prospects in energy storage and conversion devices.

[0023] Figure caption

[0024] Figure 1 The oxygen reduction catalyst FeZS-PDC-APS obtained in Examples 1 to 4 of this invention 0.2 FeZS-PDC-APS 0.6 FeZS-PDC-APS 1.0 and FeZS-PDC-APS1.4 LSV curve measured in oxygen-saturated 0.1M KOH solution.

[0025] Figure 2 a is the oxygen reduction catalyst FeZS-PDC-APS obtained in Example 1 of this invention. 0.6 TEM image, Figure 2 b is the oxygen reduction catalyst FeZS-PDC-APS obtained in Example 1 of this invention. 0.6 The spherical aberration corrected HAADF-STEM test image.

[0026] Figure 3 The oxygen reduction catalyst FeZS-PDC-APS obtained in Example 2 of this invention 0.2 TEM image.

[0027] Figure 4 The oxygen reduction catalyst FeZS-PDC-APS obtained in Example 3 of this invention 1.0 TEM image.

[0028] Figure 5 The oxygen reduction catalyst FeZS-PDC-APS obtained in Example 4 of this invention 1.4 TEM image.

[0029] Figure 6 The figure shows the experimental results of Example 5 of the present invention, where a is the oxygen reduction catalyst FeZS-PDC-APS obtained in Example 1. 0.6 The polarization curve measured as the positive electrode of an aqueous zinc-air battery, b is the oxygen reduction catalyst FeZS-PDC-APS obtained in Example 1. 0.6 Practical applications of aqueous zinc-air batteries as positive electrodes.

[0030] Figure 7 The figure shows the experimental results of Example 6 of the present invention, where a is the oxygen reduction catalyst FeZS-PDC-APS obtained in Example 1. 0.6 The polarization curves measured as the positive electrode of a solid-state zinc-air battery are shown in Figure b, which represents the oxygen reduction catalyst FeZS-PDC-APS obtained in Example 1. 0.6 Practical applications of solid-state zinc-air batteries as positive electrodes. Detailed Implementation

[0031] The technical solution of the present invention will be further explained and described below with reference to specific embodiments and figures.

[0032] Example 1: Polyacrylamide-based iron single-atom oxygen reduction catalyst -- FeZS-PDC-APS 0.6

[0033] The preparation process in this embodiment consists of four steps: preparation of polyacrylamide gel, vacuum drying, high-temperature annealing, and acid washing.

[0034] (1) First, 0.15 g FeCl3 and 0.5055 g 1,10-phenanthroline (FeCl3:1,10-phenanthroline = 1:3 molar ratio) were added to 75 ml of ultrapure water and stirred until a brownish-yellow solution was formed. Next, under continuous magnetic stirring, 5 g acrylamide, 0.05 g N,N′-methylenebisacrylamide (crosslinking agent), 0.4 g potassium carbonate, 15 g zinc chloride, and 0.6 g initiator (APS) were added to the brownish-yellow solution in sequence. Then, under continuous magnetic stirring, the mixture was heated in an oil bath at 55 °C for 3 h, and then the temperature was raised to 80 °C for 1 h to form a polyacrylamide hydrogel.

[0035] (2) The polyacrylamide hydrogel was dried in a vacuum oven at 80°C for 96 hours to obtain a dry brown colloid.

[0036] (3) The dry brown colloid was heated to 500°C in an argon atmosphere at a heating rate of 5°C / min, annealed for 1 hour, then heated to 900°C and held for 2 hours, and then cooled naturally to obtain the catalyst.

[0037] (4) The obtained catalyst was acid-washed with 1M hydrochloric acid for 8 hours and washed three times with a large amount of deionized water. Then it was dried at 80°C for 8 hours to obtain polyacrylamide-based iron single-atom oxygen reduction catalyst.

[0038] like Figure 1 As shown, this is the oxygen reduction catalyst FeZS-PDC-APS obtained in this embodiment. 0.6 LSV curve determined in oxygen-saturated 0.1 MkOH solution. From Figure 1 It can be seen that the oxygen reduction catalyst FeZS-PDC-APS 0.6 The half-wave potential in an oxygen-saturated 0.1M KOH solution is 0.93V (vs. RHE), indicating that this catalyst possesses extremely high oxygen reduction catalytic performance. Figure 2 Figure a shows the oxygen reduction catalyst FeZS-PDC-APS obtained in this embodiment. 0.6 TEM image. From Figure 2 As can be seen from a, the Fe single-atom oxygen reduction catalyst FeZS-PDC-APS 0.6 The absence of metal particles on the surface proves that Fe single atoms were successfully anchored in the carbon material. Figure 2 As shown in b, this is the oxygen reduction catalyst FeZS-PDC-APS obtained in this embodiment. 0.6 The spherical aberration corrected HAADF-STEM test plot. From Figure 2The aberration-corrected HAADF-STEM test image of b allows direct observation of the presence of iron single atoms in the catalyst.

[0039] Example 2: Polyacrylamide-based iron single-atom oxygen reduction catalyst -- FeZS-PDC-APS 0.2

[0040] The preparation process in this embodiment consists of four steps: polyacrylamide gel preparation, vacuum drying, high-temperature annealing, and acid washing.

[0041] (1) First, 0.15 g FeCl3 and 0.5055 g 1,10-phenanthroline (FeCl3:1,10-phenanthroline = 1:3 molar ratio) were added to 75 ml of ultrapure water and stirred until homogeneous, forming a brownish-yellow solution. Next, under continuous magnetic stirring, 5 g acrylamide, 0.05 g N,N′-methylenebisacrylamide (crosslinking agent), 0.4 g potassium carbonate, 15 g zinc chloride, and 0.2 g initiator (APS) were added sequentially to the brownish-yellow solution. Then, under continuous magnetic stirring, the mixture was heated in an oil bath at 55 °C for 3 h, and then the temperature was increased to 80 °C for 1 h to form a polyacrylamide hydrogel.

[0042] (2) The polyacrylamide hydrogel was dried in a vacuum oven at 80°C for 96 hours to obtain a dry brown colloid.

[0043] (3) The dry brown colloid was heated to 500°C in an argon atmosphere at a heating rate of 5°C / min, annealed for 1 hour, then heated to 900°C and held for 2 hours, and then cooled naturally to obtain the catalyst.

[0044] (4) The obtained catalyst was acid-washed with 1M hydrochloric acid for 8 hours and washed three times with a large amount of deionized water. Then it was dried at 80°C for 8 hours to obtain polyacrylamide-based iron single-atom oxygen reduction catalyst.

[0045] like Figure 1 As shown, this is the oxygen reduction catalyst FeZS-PDC-APS obtained in this embodiment. 0.2 LSV curve determined in oxygen-saturated 0.1 MkOH solution. From Figure 1 It can be seen that the oxygen reduction catalyst FeZS-PDC-APS 0.2 The half-wave potential in an oxygen-saturated 0.1M KOH solution is 0.92V (vs. RHE), indicating that this catalyst possesses extremely high oxygen reduction catalytic performance. Figure 3 The image shows the oxygen reduction catalyst FeZS-PDC-APS obtained in this embodiment. 0.2 TEM image. From Figure 3 It can be seen that the Fe single-atom oxygen reduction catalyst FeZS-PDC-APS 0.2The absence of metal particles on the surface proves that Fe single atoms were successfully anchored in the carbon material.

[0046] Example 3: Polyacrylamide-based iron single-atom oxygen reduction catalyst -- FeZS-PDC-APS 1.0

[0047] The preparation process in this embodiment consists of four steps: polyacrylamide gel preparation, vacuum drying, high-temperature annealing, and acid washing.

[0048] (1) First, 0.15 g FeCl3 and 0.5055 g 1,10-phenanthroline (FeCl3:1,10-phenanthroline = 1:3 molar ratio) were added to 75 ml of ultrapure water and stirred until homogeneous, forming a brownish-yellow solution. Next, under continuous magnetic stirring, 5 g acrylamide, 0.05 g N,N′-methylenebisacrylamide (crosslinking agent), 0.4 g potassium carbonate, 15 g zinc chloride, and 1.0 g initiator (APS) were added sequentially to the brownish-yellow solution. Then, under continuous magnetic stirring, the mixture was heated in an oil bath at 55 °C for 3 h, and then the temperature was increased to 80 °C for 1 h to form a polyacrylamide hydrogel.

[0049] (2) The polyacrylamide hydrogel was dried in a vacuum oven at 80°C for 96 hours to obtain a dry brown colloid.

[0050] (3) The dry brown colloid was heated to 500°C in an argon atmosphere at a heating rate of 5°C / min, annealed for 1 hour, then heated to 900°C and held for 2 hours, and then cooled naturally to obtain the catalyst.

[0051] (4) The obtained catalyst was acid-washed with 1M hydrochloric acid for 8 hours and washed three times with a large amount of deionized water. Then it was dried at 80°C for 8 hours to obtain polyacrylamide-based iron single-atom oxygen reduction catalyst.

[0052] like Figure 1 The figure shows the LSV curve of the oxygen reduction catalyst FeZS-PDC-APS10 obtained in this embodiment, measured in an oxygen-saturated 0.1 MkOH solution. From... Figure 1 It can be seen that the oxygen reduction catalyst FeZS-PDC-APS10 has a half-wave potential of 0.90 V (vs. RHE) in an oxygen-saturated 0.1 M KOH solution, indicating that this catalyst has extremely high oxygen reduction catalytic performance. Figure 4 The image shown is a TEM image of the oxygen reduction catalyst FeZS-PDC-APS10 obtained in this embodiment. From... Figure 4 It can be seen that no metal particles are generated on the surface of the Fe single-atom oxygen reduction catalyst FeZS-PDC-APS10, proving that the Fe single atoms are successfully anchored in the carbon material.

[0053] Example 4: Polyacrylamide-based iron single-atom oxygen reduction catalyst -- FeZS-PDC-APS 1.4

[0054] The preparation process in this embodiment consists of four steps: polyacrylamide gel preparation, vacuum drying, high-temperature annealing, and acid washing.

[0055] (1) First, 0.15 g FeCl3 and 0.5055 g 1,10-phenanthroline (FeCl3:1,10-phenanthroline = 1:3 molar ratio) were added to 75 ml of ultrapure water and stirred until a brownish-yellow solution was formed. Next, under continuous magnetic stirring, 5 g acrylamide, 0.05 g N,N′-methylenebisacrylamide (crosslinking agent), 0.4 g potassium carbonate, 15 g zinc chloride, and 1.4 g initiator (APS) were added to the brownish-yellow solution in sequence. Then, under continuous magnetic stirring, the mixture was heated in an oil bath at 55 °C for 3 h, and then the temperature was raised to 80 °C for 1 h to form a polyacrylamide hydrogel.

[0056] (2) The polyacrylamide hydrogel was dried in a vacuum oven at 80°C for 96 hours to obtain a dry brown colloid.

[0057] (3) The dry brown colloid was heated to 500°C in an argon atmosphere at a heating rate of 5°C / min, annealed for 1 hour, then heated to 900°C and held for 2 hours, and then cooled naturally to obtain the catalyst.

[0058] (4) The obtained catalyst was acid-washed with 1M hydrochloric acid for 8 hours and washed three times with a large amount of deionized water. Then it was dried at 80°C for 8 hours to obtain polyacrylamide-based iron single-atom oxygen reduction catalyst.

[0059] like Figure 1 As shown, this is the oxygen reduction catalyst FeZS-PDC-APS obtained in this embodiment. 1.4 LSV curve determined in oxygen-saturated 0.1 MkOH solution. From Figure 1 It can be seen that the oxygen reduction catalyst FeZS-PDC-APS 1.4 The half-wave potential in an oxygen-saturated 0.1M KOH solution is 0.90 V (vs. RHE), indicating that this catalyst possesses extremely high oxygen reduction catalytic performance. Figure 5 The image shows the oxygen reduction catalyst FeZS-PDC-APS obtained in this embodiment. 1.4 TEM image. From Figure 5 It can be seen that the Fe single-atom oxygen reduction catalyst FeZS-PDC-APS 1.4 The absence of metal particles on the surface proves that Fe single atoms were successfully anchored in the carbon material.

[0060] Example 5: Aqueous Zinc-Air Battery

[0061] The negative electrode of the zinc-air battery is made of a polished 0.5mm thick zinc plate. The positive electrode consists of nickel foam, a waterproof layer, and a catalyst with a loading of 1mg / cm³. -2 The electrode sheet is composed of a catalyst layer. 5 mg of FeZS-PDC-APS was used. 0.6 1.5 mg of carbon black was dispersed in 250 μL of isopropanol and 700 μL of water, and sonicated for 30 minutes to obtain the catalyst ink. Then, 50 μL of Nation was added dropwise to the ink and sonicated continuously for 90 minutes. The electrolyte for the aqueous primary zinc-air battery contained 0.2 M Zn(Ac)₂ and 6 M KOH. Room temperature polarization curves were tested using a CHI 760E workstation. For comparison, the results were obtained according to the FeZS-PDC-APS model. 0.6 The same procedure was used to assemble a control zinc-air battery using a cathode loaded with a commercially available 20% Pt / C catalyst.

[0062] Figure 6 Figure a shows the oxygen reduction catalyst FeZS-PDC-APS from Example 1. 0.6 Polarization curves measured as the positive electrode in an aqueous zinc-air battery. From Figure 6 It can be seen that the oxygen reduction catalyst is FeZS-PDC-APS 0.6 It exhibits extremely excellent oxygen reduction catalytic performance, with a peak power density reaching 215.3 mW·cm⁻¹. -2 It is significantly higher than that of commercial 20% Pt / C catalysts. Figure 6 b shows the oxygen reduction catalyst FeZS-PDC-APS in Example 1. 0.6 The practical application of aqueous zinc-air batteries as positive electrodes demonstrates the significant potential advantages of polyacrylamide-based iron single-atom oxygen reduction catalysts in energy storage and conversion devices.

[0063] Example 6: Solid-state zinc-air battery

[0064] Solid-state zinc-air batteries use a zinc plate (0.08 mm thick) as the negative electrode, with FeZS-PDC-APS coated on carbon cloth. 0.6 (Catalyst loading is 1 mg cm) -2The positive electrode is a zinc plate, and the solid electrolyte is a polymer electrolyte gel. Before use, the zinc plate is polished to a smooth surface, and the carbon cloth is treated with PTFE (60 wt.%, Alfa) to prevent diffusion during the casting of the catalyst ink. The steps for preparing the polymer electrolyte gel are as follows: 5 g of polyvinyl alcohol is added to 45 mL of deionized water at 95 °C under vigorous stirring until a homogeneous solution is formed. Next, 5 mL of 18 M KOH containing 0.2 M Zn(Ac)₂ is injected into the solution. Stirring continues for 40 minutes. Finally, the gel solution is transferred to a rectangular mold and stored at -25 °C for later use.

[0065] Figure 7 Figure a shows the oxygen reduction catalyst FeZS-PDC-APS from Example 1. 0.6 Polarization curves measured as the positive electrode in a solid-state zinc-air battery. From... Figure 7 It can be seen that the oxygen reduction catalyst is FeZS-PDC-APS 0.6 It exhibits excellent oxygen reduction catalytic performance, with a peak power density reaching 76.3 mW·cm⁻¹. -2 It is higher than that of commercially available 20% Pt / C catalysts. Figure 7 b shows the oxygen reduction catalyst FeZS-PDC-APS in Example 1. 0.6 The practical application of solid-state zinc-air batteries as positive electrodes demonstrates the significant potential advantages of polyacrylamide-based iron single-atom oxygen reduction catalysts in portable smart devices.

[0066] The above description is merely a preferred embodiment of the present invention, and therefore should not be construed as limiting the scope of the present invention. All equivalent changes and modifications made in accordance with the scope of the patent and the contents of the specification should still fall within the scope of the present invention.

Claims

1. A method for preparing a polyacrylamide-based single-atom oxygen reduction catalyst, characterized in that: Includes the following steps: (1) Using FeCl3, 1,10-phenanthroline, ultrapure water, acrylamide, N,N'-methylenebisacrylamide, potassium carbonate, zinc chloride, and ammonium persulfate in a mass ratio of 0.1-0.2: 0.5-0.6: 70-80: 4-6: 0.04-0.06: 0.3-0.5: 10-20:0.2-1.4 as raw materials, a free radical polymerization reaction was carried out to obtain (ZnCl2 + [Fe(Phen)3] 3+ @PAM; (2) Take the (ZnCl2 + [Fe(Phen)3] obtained in step (1) 3+ The polyacrylamide-based single-atom oxygen reduction catalyst was prepared by sequentially vacuum drying at 75-85℃ for 90-100h, high-temperature annealing, and acid washing. The high-temperature annealing process involves annealing the vacuum-dried (ZnCl2 + [Fe(Phen)3]) 3+ @PAM is heated to 480-520℃ in an argon atmosphere at a heating rate of 4-6℃ / min, annealed for 0.8-1.2h, then heated to 880-920℃ and held for 1.8-2.2h, and then cooled naturally.

2. The preparation method according to claim 1, characterized in that: In step (1), the mass ratio of FeCl3, 1,10-phenanthroline, ultrapure water, acrylamide, N,N'-methylenebisacrylamide, potassium carbonate, zinc chloride and ammonium persulfate is 0.15:0.5055: 75: 5: 0.05: 0.4: 15: 0.2-1.

4.

3. The preparation method according to claim 1, characterized in that: The vacuum drying temperature is 80℃ and the time is 96 hours.

4. The preparation method according to claim 1, characterized in that: The high-temperature annealing is performed by annealing (ZnCl2 + [Fe(Phen)3]) under vacuum drying. 3+ PAM was heated to 500°C in an argon atmosphere at a heating rate of 5°C / min, annealed for 1 hour, then heated to 900°C and held for 2 hours, and then cooled naturally.

5. The preparation method according to any one of claims 1 to 4, characterized in that: The pickling process involves pickling the material after high-temperature annealing with 1M hydrochloric acid for 8 hours, followed by thorough washing with a large amount of deionized water, and then drying at 80°C for 8 hours.

6. The application of the polyacrylamide-based single-atom oxygen reduction catalyst prepared by the preparation method according to any one of claims 1 to 5 in the preparation of energy storage and conversion devices.

7. A method for fabricating an energy storage and conversion device, characterized in that: It comprises a polyacrylamide-based single-atom oxygen reduction catalyst prepared by the preparation method described in any one of claims 1 to 5.

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