Platinum cluster-nitrogen-doped graphitized carbon electrocatalytic material and preparation and application thereof

By confining platinum clusters at a two-dimensional interface using a platinum cluster-nitrogen-doped graphitized carbon electrocatalytic material to form a coplanar structure, the problems of metal ion loss and catalyst instability in electro-Fenton technology are solved, achieving efficient and stable pollutant degradation.

CN117680179BActive Publication Date: 2026-02-03ZHEJIANG OCEAN UNIV
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Patent Information

Application Number
CN202311607764.2
Authority / Receiving Office
CN · China
Patent Type
Patents(China)
Current Assignee / Owner
Filing Date
2023-11-29
Publication Date
2026-02-03
Estimated Expiration
2043-11-29

AI Technical Summary

Technical Problem

In existing electro-Fenton technology, the conversion efficiency of high-valence metals to low-valence metals is low, the catalyst is unstable, and the loss of metal ions leads to a decrease in catalytic efficiency, which limits its application in high-precision fields.

Method used

A platinum cluster-nitrogen-doped graphitized carbon electrocatalytic material is used. By confining platinum clusters at the interface of two-dimensional nitrogen-doped graphitized carbon, a coplanar structure is formed, which promotes the generation of H2O2 intermediate and HO•, avoids the loss of metal ions, and improves catalytic stability and activity.

Benefits of technology

It achieves highly efficient catalytic oxidation of pollutants, improves the stability of catalytic materials, avoids metal loss, enhances reaction activity, and reduces energy consumption and cost.

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Abstract

The present application relates to the technical field of electrocatalytic materials, in particular to a platinum cluster-nitrogen-doped graphitized carbon electrocatalytic material and its preparation and application.A platinum cluster-nitrogen-doped graphitized carbon electrocatalytic material, the material uses potassium chloride as a template, and two-dimensional nitrogen-doped graphitized carbon with platinum clusters is generated on the template; wherein the platinum clusters are confined in the interface of the two-dimensional nitrogen-doped graphitized carbon and form a coplanar structure with the nitrogen-doped graphitized carbon.The electrocatalytic material provided by the present application has a unique two-dimensional confined structure, which inhibits the loss of platinum species in the coplanar platinum clusters, and can expose more catalytic sites, and the stability of the catalytic material is higher.
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Description

Technical Field

[0001] This invention relates to the field of electrocatalytic materials technology, specifically to a platinum cluster-nitrogen-doped graphitized carbon electrocatalytic material and its preparation and application. Background Technology

[0002] With the continuous and rapid development of modern industry, water pollution has become increasingly serious. Currently, my country's annual industrial wastewater production exceeds 200 billion tons, and the organic pollutants contained in this wastewater, such as dyes, phenols, and antibiotics, are mostly structurally stable and difficult to degrade. Mainstream treatment technologies include chemical catalytic oxidation, physical adsorption, and biodegradation, but these methods have limitations such as secondary pollution, long treatment cycles, and high costs. Therefore, providing an efficient and economical water treatment technology has become one of the important research topics. Electrocatalysis technology, due to its green and environmentally friendly characteristics, simple operation, and high efficiency, has become a research hotspot in energy and environmental fields.

[0003] Electro-Fenton technology, a promising electrocatalytic water treatment technology, utilizes a system dominated by variable-valence metals such as iron, cobalt, and nickel. It generates H₂O₂ at the cathode via a two-electron oxygen reduction reaction, eliminating the risks associated with the storage, transportation, and dilution of concentrated H₂O₂. The electrogenerated H₂O₂ then reacts with homogeneous metal ions to produce reactive oxygen species, such as hydroxyl radicals (HO). • ), peroxyhydrogen radical ( • OOH) and singlet oxygen ( 1 (O2). Compared with traditional chemical oxidation methods, electro-Fenton technology does not require the addition of additional oxidants or catalysts, reducing the use of chemical agents and the generation of chemical waste, which helps to reduce the impact on the environment.

[0004] However, the limitation of this type of electro-Fenton process lies in the fact that low-valence metal ions are oxidized to high-valence metal ions after completing one electro-Fenton reaction. The conversion rate of high-valence metals to low-valence metals is very slow, which is actually the rate-limiting step of the electro-Fenton reaction. This situation means that variable-valence metal ions cannot be recycled, thus reducing the catalytic efficiency and cost-effectiveness of the electro-Fenton process. In addition, the in-situ generation of H2O2 and subsequent unidirectional enhancement of activation during the electro-Fenton process, the loss of metal ions in strongly acidic solutions, and the poor recyclability of transition metal-based catalysts also contribute to the low catalytic efficiency. These factors limit the application of electro-Fenton technology in high-precision fields. Summary of the Invention

[0005] This invention aims to overcome the defects in the existing technology of unstable overall catalytic performance in the Fenton reaction due to the low conversion efficiency of high-valence metals to low-valence metals, as well as the instability of the catalyst and the decrease in catalytic efficiency caused by the loss of metal ions during the catalytic process. It provides platinum cluster-nitrogen-doped graphitized carbon electrocatalytic materials and their preparation and application to overcome the above defects.

[0006] To achieve the above objectives, the present invention provides the following technical solution:

[0007] A platinum cluster-nitrogen-doped graphitized carbon electrocatalytic material is provided, wherein a two-dimensional nitrogen-doped graphitized carbon with platinum clusters is generated in situ on potassium chloride as a template; wherein the platinum clusters are confined in the interface of the two-dimensional nitrogen-doped graphitized carbon and form a coplanar structure with the nitrogen-doped graphitized carbon.

[0008] The platinum cluster-nitrogen-doped graphite carbon electrocatalytic material designed by the inventors of this application induces the formation of the *H2O2 intermediate through the two-electron oxygen reduction reaction promoted by graphitized nitrogen-doped carbon. Simultaneously, atomic hydrogen (H*) generated by the electroreduction of platinum clusters confined at the interface of the two-dimensional nitrogen-doped graphitized carbon network is used for the in-situ reduction of the *HOOH intermediate to generate HO. • Once reactive oxygen species are obtained, catalytic oxidation of pollutants can be achieved. The entire reaction system does not involve the conventional Fenton process dominated by variable-valence metals, resulting in high reactivity.

[0009] Furthermore, the coplanar structure formed by platinum clusters confined at the interface of two-dimensional nitrogen-doped graphitized carbon helps promote electron transfer and interaction between the platinum clusters and nitrogen-doped graphitized carbon, effectively improving the electrocatalytic performance of the catalyst. More importantly, the two-dimensional nitrogen-doped graphitized carbon structure can suppress platinum loss, avoiding the problem of decreased catalytic activity caused by metal ion loss in conventional electro-Fenton technology; at the same time, it exposes more catalytic sites, resulting in a significant increase in catalytic activity, and the catalytic material is more stable and easier to recover.

[0010] Therefore, this scheme not only reduces the loss of catalytically active metal ions by limiting their location, but also avoids the formation of HO by reducing H2O2 from low-valence metal centers. • The conventional Fenton process is used to enhance the catalytic stability of catalytic materials.

[0011] This invention also provides a method for preparing electrocatalytic materials, comprising the following steps:

[0012] S1. Add platinum source, carbon nitrogen source, and potassium chloride to an ethanol aqueous solution, mix well, heat and stir until the solvent is completely evaporated to obtain the precursor;

[0013] S2. After drying the precursor in S1, calcine it under nitrogen and / or an inert atmosphere to obtain the electrocatalytic material.

[0014] This invention utilizes a platinum source, a carbon-nitrogen source, potassium chloride, deionized water, and ethanol to obtain a platinum-based carbon-nitrogen precursor coated on the surface of potassium chloride crystals through stirring and drying. Subsequently, calcination in a N2 and / or inert atmosphere confines the platinum clusters at the interface of two-dimensional nitrogen-doped graphitized carbon, forming a coplanar structure, thus obtaining the final planar platinum cluster-nitrogen-doped graphitized carbon electrocatalytic material in one step. Potassium chloride is used as a template for the two-dimensional material composite formation, providing support and aiding in the construction of the two-dimensional morphology.

[0015] It is noteworthy that when sodium chloride is used instead of potassium chloride as a template, a two-dimensional coplanar structure cannot be constructed; therefore, potassium chloride is irreplaceable and crucial for synthesizing the two-dimensional coplanar material. The reason for this is likely that sodium chloride and potassium chloride differ structurally, leading to different results when using them as templates. Sodium chloride crystals have a face-centered cubic structure, while potassium chloride crystals have a body-centered cubic structure. This means that the arrangement and spatial structure of ions in sodium chloride and potassium chloride crystals are different.

[0016] The entire solution is simple, has a short reaction time, and uses widely available raw materials, making it suitable for large-scale application.

[0017] Preferably, in step S1, the platinum source is selected from one or more of platinum acetylacetonate, platinum chloride, and platinum nitrate, and the carbon and nitrogen source is selected from one or more of melamine and urea.

[0018] There are no special requirements for the choice of platinum source; any readily available raw material that can synthesize the corresponding substance without producing synthetic byproducts is acceptable, and it is not limited to the types mentioned above. The selection of each raw material has no special impact on the properties and morphology of the final synthesized product.

[0019] Melamine and urea are commonly used carbon and nitrogen co-sources. They are composed of clean elements, containing only O and H in addition to C and N. During calcination, C and N can be retained, while O and H are carried away as water vapor, making them ideal sources of carbon and nitrogen.

[0020] Preferably, in step S1, the volume ratio of ethanol to water in the ethanol-water solution is 1:(1~3).

[0021] Ethanol-water solutions with different volume ratios may exhibit varying densities, surface tensions, and viscosities. These variations in physical properties can influence the formation and properties of the synthesized materials. Furthermore, the volume ratio of ethanol to water directly affects the concentrations of ethanol and water in the solution, thereby influencing the solubility of platinum and carbon / nitrogen sources. This can potentially impact the purity and crystal morphology of the electrocatalyst.

[0022] Experiments have shown that when the volume ratio of ethanol to water is 1:(1~3), the dissolution rate of each raw material is faster, and the morphology of the obtained material is also more regular.

[0023] Preferably, in step S1, the heating temperature is 80~100℃.

[0024] At this heating temperature, the solvent evaporation rate can be controlled at a suitable level, preventing the solvent from evaporating too quickly and the evaporation time from being too short, which would affect grain growth. However, if the temperature is too low, the required evaporation time will be prolonged, increasing the experimental time and cost. Furthermore, slow solvent evaporation may affect the purity of the product. Experiments have shown that heating at 800 rpm and 80-100°C for 4 hours is sufficient to completely evaporate the solvent.

[0025] Preferably, in step S1, the molar ratio of platinum in the platinum source, carbon in the carbon-nitrogen source, nitrogen in the carbon-nitrogen source, and potassium chloride is 5:2:1:400.

[0026] In this scheme, the carbon and nitrogen sources are both melamine or urea, and the molar ratio of carbon to nitrogen in both raw materials is 2:1.

[0027] The amounts of platinum and carbon / nitrogen sources affect the amount of platinum clusters and graphitized carbon generated. Since the platinum clusters are confined within the two-dimensional interface of the graphitized carbon, excessive amounts of platinum clusters can result in free platinum not encapsulated by the graphitized carbon interface, thus hindering optimal performance. To ensure that all platinum clusters are confined within the two-dimensional graphitized carbon interface and that both react synergistically for the best effect, theoretical calculations and experimental designs were performed to adjust the specific amounts.

[0028] Furthermore, potassium chloride, as the template material for the entire electrocatalytic material, affects the formation and stability of the layered structure of graphitized carbon in its ratio to the carbon and nitrogen source. Different amounts of template result in different available specific surface areas, which may lead to the formation of graphitized carbon with different interlayer distances and intralayer structures, thereby affecting the electrical conductivity and mechanical properties of graphitized carbon.

[0029] The inventors of this application theoretically calculated and controlled the molar ratio between platinum in the platinum source, carbon in the carbon-nitrogen source, nitrogen in the carbon-nitrogen source, and potassium chloride to be 5:2:1:400, which ultimately yielded a platinum cluster-nitrogen-doped graphite carbon electrocatalytic material.

[0030] Preferably, in step S2, the drying method is freeze drying, and the drying time is 12~24 h.

[0031] The freeze-dried material has a more regular morphology and a looser structure, resulting in a larger specific surface area. When used as an electrocatalytic material, it can increase the number of interaction sites with the electrolyte. Other drying methods can also be used, which, apart from affecting the morphology, do not significantly affect the catalytic activity of the material itself.

[0032] Preferably, in step S2, the inert atmosphere is selected from argon or helium.

[0033] In this situation, choosing argon as the inert atmosphere might be a better option. Argon does not participate in chemical reactions and is therefore considered an ideal inert gas. Its large atomic weight, high stability, and relatively low cost make it a common choice for inert gases in many laboratory and industrial applications.

[0034] Alternatively, a mixture of nitrogen and argon can be used to create an inert atmosphere.

[0035] Preferably, in step S2, the calcination temperature is 250~350℃, the calcination time is 1~3 h, and the heating rate is 3~5 ℃ / min.

[0036] Calcination temperature can affect the formation and stability of the crystal structure of materials, as well as the formation of surface active sites. Higher calcination temperatures may help improve the crystallinity and stability of materials, but may also lead to grain growth and loss of surface active sites. Controlling the calcination temperature within 250–350 °C can yield electrocatalytic materials with stable performance and regular structure.

[0037] Calcination time affects the degree of perfection of the internal structure of the material. Longer calcination time helps to remove impurities and improve the stability of the material, but it may also lead to grain growth and over-sintering. Similarly, controlling the calcination time within 1 to 3 hours can yield electrocatalytic materials with complete and uniform grain growth.

[0038] Excessively high or low heating rates will affect the stability and particle uniformity of the electrocatalytic material obtained after calcination. To ensure high stability and high particle uniformity of the synthesized material, the inventors of this application have discovered that controlling the heating rate during calcination at 3~5 ℃ / min can ensure that the calcined material has good stability and high particle uniformity.

[0039] The present invention also provides an electrocatalytic membrane, which is prepared from the above-mentioned electrocatalytic material.

[0040] The electrocatalytic membrane provided by this invention is obtained directly from the vacuum filtration of powdered materials, thereby constructing a permeable electrochemical membrane system characterized by rapid mass transfer and low energy consumption. This membrane system can effectively promote the transfer of ions or molecules in electrochemical reactions, thereby improving reaction efficiency. Furthermore, due to its rapid mass transfer and low energy consumption, this system can also reduce energy consumption, lower costs, and contribute to improving the sustainability of the reaction process.

[0041] It is noteworthy that the material prepared using sodium chloride as a template loses its coplanar structure and cannot be vacuum filtered to obtain an electrocatalytic membrane, thus preventing its catalytic application. This also demonstrates the structural characteristics of the planar platinum cluster-nitrogen-doped graphitized carbon electrocatalytic material proposed in this scheme.

[0042] The present invention also provides the application of the above-mentioned electrocatalytic membrane in water treatment.

[0043] Due to the electrocatalytic properties of the electrocatalytic material in the membrane, pollutants in water can be specifically treated. Under electrical action, the selective generation of H₂O from oxygen is induced by the synergistic effect of platinum clusters and graphitized doped nitrogen. • And HO • It is a highly oxidizing free radical that can directly oxidize organic pollutants, breaking them down into smaller, harmless substances such as carbon dioxide and water. This oxidation reaction occurs through the reaction of HO• with organic molecules, disrupting their structure and thus degrading the pollutants. Additionally, HO• can also trigger reactions such as hydrogen atom abstraction and hydroxyl addition with organic pollutants, leading to chain breakage and ring opening, ultimately decomposing them into smaller organic or inorganic molecules. It can effectively degrade organic pollutants into harmless small-molecule products.

[0044] To verify the excellent treatment effect of the electrocatalytic membrane on organic pollutants, a simulated water pollution environment was used. A benzimidazole solution was prepared and designated as a pollutant in the water, and treatment was simulated under a current intensity of 2.5 mA. The results showed that the electrocatalytic membrane could achieve nearly 100% degradation of a 10 mg / L benzimidazole solution within 60 min. Furthermore, the circulation filtration rate could be controlled at 0.123 min, and the batch filtration time was 0.017 min, demonstrating highly efficient filtration and separation speed, which can meet the application requirements of different scenarios.

[0045] Therefore, the present invention has the following beneficial effects:

[0046] (1) The electrocatalytic material provided by the present invention has a unique two-dimensional confined structure, which inhibits the loss of platinum species in the coplanar platinum clusters and can expose more catalytic sites, resulting in higher stability of the catalytic material.

[0047] (2) The electrocatalytic material provided by this invention has a synergistic effect between platinum clusters and nitrogen-doped graphitized carbon, which induces the selective generation of HO from oxygen. • It does not involve the Fenton process and has high reactivity.

[0048] (3) The electrocatalytic membrane designed in this invention adopts a permeable electrochemical membrane system, which has fast mass transfer and low energy consumption.

[0049] (4) The electrocatalytic membrane provided by the present invention can be used in water treatment to treat pollutants in water and has broad application prospects. Attached Figure Description

[0050] Figure 1 This is a process diagram for preparation;

[0051] Figure 2 SEM and TEM images of Example 1;

[0052] Figure 3 This is the SEM image of Comparative Example 1;

[0053] Figure 4 Figures showing the effects of benzimidazole treatment under different conditions;

[0054] Figure 5 This is a comparison chart of the filtering effects;

[0055] Figure 6 This is a diagram of the reaction mechanism;

[0056] Figure 7 This is a model diagram of a through-type electrochemical reactor. Detailed Implementation

[0057] The present invention will be further described below with reference to specific embodiments. Those skilled in the art will be able to implement the present invention based on these descriptions. Furthermore, the embodiments of the present invention described below are generally only some, not all, of the embodiments of the present invention. Therefore, all other embodiments obtained by those skilled in the art based on the embodiments of the present invention without inventive effort should fall within the scope of protection of the present invention.

[0058]

Example

[0059] Example 1

[0060] (1) Weigh 10 mL of ethanol and 10 mL of deionized water to prepare an ethanol-water solution.

[0061] (2) Weigh 0.033 mmol acetylacetone platinum, 0.04 mmol melamine and 2.68 mmol potassium chloride and add them in portions to the prepared ethanol aqueous solution. Sonicate for 20 min to mix thoroughly.

[0062] (3) Stir at 800 rpm and 80℃ for 4 h until the solvent is completely evaporated to obtain a pale yellow solid.

[0063] (4) Transfer the pale yellow solid from step (3) into a freeze dryer and dry overnight.

[0064] (5) After drying, the pale yellow solid was transferred to a smooth ceramic crucible, sealed in a tube furnace, and heated to 300°C at a rate of 5 °C / min under a N2 atmosphere (10 mL / min). The temperature was maintained for 2 h, and then cooled to room temperature. A platinum cluster-nitrogen-doped graphite carbon two-dimensional material was obtained.

[0065] Example 2

[0066] (1) Weigh 10 mL of ethanol and 20 mL of deionized water to prepare an ethanol-water solution.

[0067] (2) Weigh 0.033 mmol acetylacetone platinum, 0.04 mmol melamine and 2.68 mmol potassium chloride and add them in portions to the prepared ethanol aqueous solution. Sonicate for 20 min to mix thoroughly.

[0068] (3) Stir at 800 rpm and 100℃ for 4 h until the solvent is completely evaporated to obtain a pale yellow solid.

[0069] (4) Transfer the pale yellow solid from step (3) into a freeze dryer and dry overnight.

[0070] (5) After drying, the pale yellow solid was transferred to a smooth ceramic crucible, sealed in a tube furnace, and heated to 350°C at a rate of 3 °C / min under a N2 atmosphere (10 mL / min). The temperature was maintained for 1 h, and then cooled to room temperature. A platinum cluster-nitrogen-doped graphite carbon two-dimensional material was obtained.

[0071] Example 3

[0072] (1) Weigh 10 mL of ethanol and 30 mL of deionized water to prepare an ethanol-water solution.

[0073] (2) Weigh 0.033 mmol acetylacetone platinum, 0.04 mmol melamine and 2.68 mmol potassium chloride and add them in portions to the prepared ethanol aqueous solution. Sonicate for 20 min to mix thoroughly.

[0074] (3) Stir at 800 rpm and 100℃ for 4 h until the solvent is completely evaporated to obtain a pale yellow solid.

[0075] (4) Transfer the pale yellow solid from step (3) into a freeze dryer and dry overnight.

[0076] (5) After drying, the pale yellow solid was transferred to a smooth ceramic crucible, sealed in a tube furnace, and heated to 250°C at a heating rate of 3 °C / min under a mixed atmosphere of N2 and argon (10 mL / min). The temperature was maintained for 2 h, and then cooled to room temperature. A two-dimensional platinum cluster-nitrogen-doped graphite carbon material was obtained.

[0077] Example 4

[0078] This embodiment is basically the same as Embodiment 1, except that the carbon and nitrogen source used is urea.

[0079] Comparative Example 1

[0080] This comparative example is basically the same as Example 1, except that the template used is sodium chloride.

[0081] [Performance Testing]

[0082] 1. SEM and TEM testing

[0083] The platinum cluster-nitrogen-doped graphite carbon two-dimensional material obtained in Example 1 was subjected to SEM and TEM tests, and Comparative Example 1 was subjected to SEM tests. The results are as follows: Figures 2-3 As shown in the image, SEM images reveal that the generated electrocatalytic material has a planar sheet-like structure with a smooth surface. TEM images show similar results to the SEM images, both indicating a planar sheet-like structure with a large specific surface area. Furthermore, the planar sheet-like nitrogen-doped graphitized carbon network structure contains darker platinum cluster particles, confirming the successful synthesis of a platinum cluster-nitrogen-doped graphitized carbon two-dimensional material.

[0084] like Figure 3 As shown, the electrocatalytic material obtained using sodium chloride as a template loses its coplanar structure, and its surface is rough, uneven, and has large undulations, which is inconsistent with... Figure 2 The planar structure shown is completely different.

[0085] 2. Catalytic performance test

[0086] The platinum cluster-nitrogen-doped graphite carbon two-dimensional material prepared in Example 1 was vacuum filtered into the following form: Figure 7 The electrocatalytic membrane shown in Figure 2, and used with Figure 7 The apparatus shown was used to begin measuring the electrocatalytic performance.

[0087] ① Prepare a benzimidazole solution with a pH of 5.5 and a concentration of 10 mg / L. Pour the prepared benzimidazole solution from the apparatus ( Figure 7The water inlet is slowly fed in through a peristaltic pump, allowing it to flow through the electrocatalytic membrane. The current intensity is set to 2.5 mA, and the electrocatalytic performance test begins. Water samples treated by the electrocatalytic membrane are taken from the outlet every 5 to 10 minutes. The first sample is taken after a 5-minute interval, and the subsequent samples are taken every 10 minutes, for a total of 7 samples. The measurement is completed in 60 minutes; this is the electrocatalytic-oxygen group.

[0088] ② is similar to the steps in ①, except that nitrogen is introduced into the device to isolate oxygen; it is an electroadsorption-nitrogen group.

[0089] ③ is similar to the steps in ①, except that no electricity is applied and nitrogen is introduced into the device to isolate oxygen; this is adsorption-nitrogen.

[0090] ④ is similar to the steps in ①, except that no electricity is applied; it is an adsorption-oxygen group.

[0091] The collected water samples were measured and calculated as follows: Figure 4 The results shown are observed. Figure 4 It is evident that the electrocatalytic membrane in this scheme requires the presence of oxygen, through which oxygen selectively generates H₂O on the cathode catalytic membrane. • Therefore, the catalytic activity of the cathode electrocatalytic membrane cannot be activated after oxygen is isolated, and its benzimidazole removal rate is much lower than that under oxygen conditions. Furthermore, data from group ③ (without electricity) and group ② were compared to observe... Figure 4 As can be seen from the electrocatalysis-oxygen group and the adsorption-oxygen group, without the effect of an external electric field, oxygen cannot be converted into highly reactive H₂O. • Therefore, the removal performance of benzimidazole is mainly dominated by the adsorption of the system, and the removal performance of benzimidazole under adsorption-oxygen and adsorption-nitrogen conditions is similar.

[0092] 3. Filtration test

[0093] According to the conditions tested in "2. Catalytic Performance Test", the actual performance of the electrocatalytic membrane obtained in Example 1 was evaluated under both circulating filtration and batch filtration conditions during water treatment. The results are as follows: Figure 5 As shown, the circulating filtration speed can be controlled at 0.123 min, and the batch filtration time is 0.017 min; this proves that it has a high-efficiency filtration and separation speed, which can meet the application needs of different scenarios.

Claims

1. A method for preparing a platinum cluster-nitrogen-doped graphitized carbon electrocatalytic material for treating benzimidazole pollutants in water, characterized in that, The material uses potassium chloride as a template to generate two-dimensional nitrogen-doped graphitized carbon with platinum clusters in situ; wherein the platinum clusters are confined in the interface of the two-dimensional nitrogen-doped graphitized carbon and form a coplanar structure with the nitrogen-doped graphitized carbon. The preparation method of the electrocatalytic material includes the following steps: S1. Add platinum source, carbon nitrogen source, and potassium chloride to an ethanol aqueous solution, mix well, heat and stir until the solvent is completely evaporated to obtain the precursor; S2. After drying the precursor in S1, calcination is carried out under an inert atmosphere to obtain the electrocatalytic material; In step S2, the calcination temperature is 250~350℃, the calcination time is 1~3 h, and the heating rate is 3~5℃ / min.

2. The method as described in claim 1, characterized in that, In step S1, the platinum source is selected from one or more of platinum acetylacetonate, platinum chloride, and platinum nitrate, and the carbon and nitrogen source is selected from one or more of melamine and urea.

3. The method as described in claim 1, characterized in that, In step S1, the volume ratio of ethanol to water in the ethanol-water solution is 1:(1~3).

4. The method as described in claim 1, characterized in that, In step S1, the heating temperature is 80~100℃.

5. The method according to any one of claims 1-4, characterized in that, In step S1, the molar ratio of platinum in the platinum source, carbon in the carbon-nitrogen source, nitrogen in the carbon-nitrogen source, and potassium chloride is 5:2:1:

400.

6. The method as described in claim 1, characterized in that, In step S2, the inert atmosphere is selected from argon or helium.

7. The electrocatalytic membrane prepared corresponding to the electrocatalytic material prepared by the method according to any one of claims 1 to 6.

8. The application of the electrocatalytic membrane as described in claim 7 in water treatment, characterized in that, The application involves preparing a benzimidazole solution as a pollutant in water and treating it under a current intensity of 2.5 mA.

Citation Information

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