A platinum-based electrocatalyst using nitrogen-doped carbon semitube as carrier and a preparation method thereof

Abstract

The application discloses a platinum-based electrocatalyst using nitrogen-doped carbon half-tube as a carrier and a preparation method thereof. The platinum-based electrocatalyst is prepared by using nitrogen-doped carbon half-tube as a carrier, using platinum-based nanoparticles as catalyst active points, uniformly distributing the platinum-based nanoparticles on the surface of the nitrogen-doped carbon half-tube, and forming the platinum-based electrocatalyst. In the application, a surfactant, an amine compound and an acid are dissolved in water, ammonium persulfate is added to perform oxidative polymerization, and then the polymerization product is filtered, washed and dried. The polymerization product is pyrolyzed in an inert gas at high temperature to obtain the nitrogen-doped carbon half-tube. A platinum compound, a transition metal compound and sodium hydroxide are dissolved in a solvent to perform microwave reaction, and then platinum-based nanoparticles are obtained. Finally, the platinum-based nanoparticles and the nitrogen-doped carbon half-tube carrier are fully mixed to obtain the platinum-based electrocatalyst using the nitrogen-doped carbon half-tube as the carrier. The catalyst prepared by the application has excellent oxygen reduction reaction catalytic activity and good durability, and the preparation method is simple and easy to implement, and is suitable for large-scale production.

Description

Technical Field

[0001] This invention belongs to the field of new energy technology and relates to an electrocatalyst for fuel cell cathodes, specifically to a platinum-based electrocatalyst using nitrogen-doped carbon semiconductors as a support and its preparation method. Background Technology

[0002] Fuel cells are energy conversion devices with advantages such as high energy density, high utilization rate, and clean and quiet operation. Platinum-supported carbon black (Pt / C) remains the most practical commercial catalyst. However, the slow kinetics of the oxygen reduction reaction (ORR) at the fuel cell cathode, the high Pt content, the limited and expensive nature of Pt resources, and the poor electrochemical stability of Pt / C catalysts severely hinder the practical application of fuel cells. Therefore, designing and developing low-cost and high-performance ORR electrocatalysts is an important research topic in the field of fuel cell technology.

[0003] Early fuel cells used platinum black as a catalyst; however, platinum black (Pt) readily agglomerates and dissolves in practice, exhibiting very poor fuel cell performance. Researchers then loaded Pt nanoparticles onto carbon black, which has a high specific surface area and high electrical conductivity, successfully making the Pt nanoparticles smaller. Furthermore, due to their dispersion on the high specific surface area carbon black surface, the stacking of Pt nanoparticles is reduced, improving surface atom utilization. Further, it has been found that heteroatom doping in carbon supports can create active centers and improve catalyst activity. For example, nitrogen (N)-doped carbon materials are widely studied due to their abundant reserves, excellent catalytic activity, and high electronic conductivity. Simultaneously, the N-containing functional groups introduced into carbon materials can bond strongly with metals, facilitating more uniform and stable dispersion of metal catalysts on the carbon material surface. Continuously reducing Pt usage while maintaining fuel cell performance is a persistent pursuit in the industry, and significant progress has been made in recent years. However, further reductions in Pt usage require structural innovation in catalyst technology. Therefore, the preparation of novel carbon supports with heteroatom doping structures is of great significance for improving catalyst activity and stability. Summary of the Invention

[0004] To address the problems of existing technologies, the present invention aims to overcome the shortcomings of existing technologies and provide a platinum-based electrocatalyst using nitrogen-doped carbon semiconductors as a support and its preparation method. A novel carbon support for nitrogen-doped carbon semiconductors is prepared through oxidative polymerization, and platinum-based nanoparticles are synthesized via a one-step microwave method. The two are then combined to prepare the platinum-based electrocatalyst using nitrogen-doped carbon semiconductors as a support. The nitrogen-doped carbon semiconductors of this invention possess a highly open structure, a large specific surface area, abundant micro / mesopores, and good electrical conductivity. The platinum-based electrocatalyst using nitrogen-doped carbon semiconductors as a support in this invention exhibits excellent catalytic activity and high stability.

[0005] To achieve the above-mentioned objectives, the present invention adopts the following technical solution:

[0006] A platinum-based electrocatalyst using nitrogen-doped carbon semiconductors as a support is described. The nitrogen-doped carbon semiconductors are used as the support, and platinum-based nanoparticles are used as the active particles of the catalyst. The platinum-based nanoparticles are uniformly distributed on the surface of the nitrogen-doped carbon semiconductors to form a platinum-based electrocatalyst with a carbon support structured by heteroatoms.

[0007] Preferably, the total atomic percentage of the platinum-based electrocatalyst is 100%, wherein the nitrogen doping amount is 0-20 at%; the carbon half-tube diameter is 1-200 nm and the length is 10 nm-20 μm.

[0008] Preferably, the particle size of the platinum-based nanoparticles is 1-5 nm, wherein the molar ratio of the added transition metal to platinum is (0-10):1.

[0009] A method for preparing a platinum-based electrocatalyst using nitrogen-doped carbon semiconductors as a support, comprising the following steps:

[0010] (1) Dissolve surfactant, amine compound and acid in water, then add ammonium persulfate for oxidative polymerization, filter the product solution, collect the polymerization product, wash and dry the obtained polymerization product, and then place the clean and dry polymerization product in an inert gas for high-temperature pyrolysis to obtain nitrogen-doped carbon half tubes, which can be used as carrier materials for later use.

[0011] (2) Dissolve platinum compounds, transition metal compounds and alkali in ethylene glycol to obtain a reaction mixture. Place the reaction mixture in a microwave reactor and carry out a microwave reaction to obtain platinum-based nanoparticles, which can be used as catalyst active materials for later use.

[0012] (3) The platinum-based nanoparticles prepared in step (2) are thoroughly mixed with the nitrogen-doped carbon half-tubes prepared in step (1) to obtain a platinum-based electrocatalyst with nitrogen-doped carbon half-tubes as the support.

[0013] Preferably, in step (1), the surfactant is at least one of cationic surfactants, anionic surfactants, and nonionic surfactants with different carbon chain lengths;

[0014] Preferably, in step (1), the amine compound is at least one selected from aniline, o-phenylenediamine, m-phenylenediamine, p-phenylenediamine and other amine derivatives;

[0015] Preferably, in step (1), the acid is at least one of inorganic acid and organic acid.

[0016] More preferably, the cationic surfactant is at least one of hexadecyltrimethylammonium bromide and hexadecyltrimethylammonium chloride;

[0017] More preferably, the anionic surfactant is at least one of sodium dodecylbenzenesulfonate and sodium hexadecyl sulfate;

[0018] More preferably, the nonionic surfactant is at least one of polyvinylpyrrolidone and polyoxypropylene-polyoxyethylene copolymer.

[0019] Preferably, in step (1), the molar ratio of the surfactant, amine compound, acid, and ammonium persulfate is (0-10):1:(0-20):(0-2);

[0020] Preferably, in step (1), the oxidative polymerization reaction lasts for at least 24 hours; the pyrolysis temperature is 600–1200°C, and the pyrolysis time is 0.5–5 hours.

[0021] Preferably, in step (2), the platinum compound is at least one of platinum acetylacetonate, chloroplatinic acid, potassium chloroplatinate, and platinum chloride;

[0022] Preferably, in step (2), the transition metal compound is at least one selected from palladium, silver, gold, molybdenum, tungsten, iron, cobalt, nickel, copper, and zinc compounds;

[0023] Preferably, in step (2), the alkali is sodium hydroxide, potassium hydroxide, or other hydroxides that are readily soluble in ethylene glycol solvent.

[0024] Preferably, in step (2), the molar ratio of the platinum compound, the transition metal compound, and the alkali is 1:(0-10):(2.5-40); when the amount of the transition metal compound is 0, pure platinum nanoparticles are synthesized; when the amount of the transition metal compound is not 0, platinum alloy nanoparticles are synthesized.

[0025] Preferably, in step (2), the power of the microwave reaction is 80-800W, the temperature is 120-195℃, and the reaction time is 0.5-30min; the platinum-based nanoparticles are purified using hydrochloric acid with a molar concentration of not less than 1M.

[0026] Preferably, in steps (1) and (2), the molar ratio of surfactant to platinum compound is (0-100):1.

[0027] Preferably, in step (3), the mass ratio of platinum-based nanoparticles to nitrogen-doped carbon semiconductors is (0-1000):1, and the amount of platinum-based nanoparticles added is not 0.

[0028] Compared with the prior art, the present invention has the following obvious and prominent substantive features and significant advantages:

[0029] 1. The support for the electrocatalyst of the present invention is a nitrogen-doped carbon semi-tube, which has a novel semi-tube structure and a highly open morphology that is beneficial for mass transfer;

[0030] 2. The heteroatom nitrogen present in the carbon half-tube support of the electrocatalyst of the present invention can not only create active sites to play a role in catalysis, but also make the platinum nanoparticles more firmly loaded and more uniformly dispersed.

[0031] 3. The electrocatalyst of the present invention uses weakly reducing alcohols as both reducing agents and solvents for the platinum nanoparticles, which inhibits the growth of platinum nanoparticles, keeps the platinum nanoparticles small in size and has high dispersibility.

[0032] 4. The electrocatalyst of this invention is a nitrogen-doped carbon semi-tube supported platinum-based electrocatalyst with a novel and unique structure, exhibiting superior catalytic activity and stability compared to commercial Pt / C. Attached Figure Description

[0033] Figure 1 This is a scanning electron microscope (SEM) image of the nitrogen-doped carbon half-tube carrier prepared in Example 1 of the present invention.

[0034] Figure 2 The powder X-ray diffraction (XRD) spectra of the nitrogen-doped carbon semitube platinum catalyst, Pt / C, and nitrogen-doped carbon semitube support prepared in Example 1 of this invention are shown.

[0035] Figure 3 This is a transmission electron microscope (TEM) image of the nitrogen-doped carbon semi-tube platinum-supported catalyst prepared in Example 1 of the present invention.

[0036] Figure 4 The image shows the Pt 4f X-ray photoelectron spectroscopy (XPS) spectra of the nitrogen-doped carbon semi-tube platinum-supported catalyst prepared in Example 1 of this invention, compared with those of a commercial Pt / C catalyst.

[0037] Figure 5 The graph shows the oxygen reduction reaction polarization curves of the nitrogen-doped carbon semi-tube platinum-supported catalyst prepared in Example 1 of this invention compared with those of a commercial Pt / C catalyst.

[0038] Figure 6 The ORR polarization curves of the nitrogen-doped carbon semi-tube platinum-supported catalyst prepared in Example 1 of this invention are shown before and after 10,000 cycles.

[0039] Figure 7 ORR polarization curves of existing commercial Pt / C catalysts before and after 10,000 cycles. Detailed Implementation

[0040] To better understand the present invention, the following embodiments are further illustrations of the present invention, but the content of the present invention is not limited to the following embodiments.

[0041] The above solution will be further described below with reference to specific embodiments. The preferred embodiments of the present invention are described in detail below:

[0042] Example 1

[0043] In this embodiment, a platinum-based electrocatalyst using nitrogen-doped carbon semiconductors as a support is described. The nitrogen-doped carbon semiconductors are used as the support, and platinum-based nanoparticles are used as the active particles of the catalyst. The platinum-based nanoparticles are uniformly distributed on the surface of the nitrogen-doped carbon semiconductors to form a platinum-based electrocatalyst with a carbon support structure doped with heteroatoms.

[0044] In this embodiment, a method for preparing a platinum-based electrocatalyst using nitrogen-doped carbon semiconductors as a support includes the following steps:

[0045] (1) Weigh 0.016 mol of hexadecyltrimethylammonium bromide and dissolve it in water. Then, dissolve 1 g of m-phenylenediamine, add hydrochloric acid containing 0.1 mol of hydrogen chloride and 0.01 mol of ammonium persulfate, and carry out oxidative polymerization reaction for 24 h. Filter the product solution, collect the polymerization product, wash and dry the obtained polymerization product, and then place the clean and dry polymerization product under argon protection and carry out high-temperature pyrolysis at 900 °C for 3 h to obtain nitrogen-doped carbon half-tubes, which can be used as carrier materials for later use.

[0046] (2) Dissolve 0.0772 mmol of H2PtCl6 and 0.8 mmol of NaOH in ethylene glycol to obtain a reaction mixture. Place the reaction mixture in a microwave reactor and microwave it at 160°C for 2 min with a power of 160 W to obtain platinum nanoparticles. Purify them with 1 M hydrochloric acid and use them as catalyst active materials for later use.

[0047] (3) The platinum-based nanoparticles prepared in step (2) are thoroughly mixed with the nitrogen-doped carbon half-tubes prepared in step (1) to obtain a platinum-based electrocatalyst with nitrogen-doped carbon half-tubes as the support.

[0048] Test characterization:

[0049] The SEM results of the nitrogen-doped carbon semiconductor prepared in step (1) of this embodiment are as follows: Figure 1 As shown, the diameter of the nitrogen-doped carbon half-tube is 80–90 nm. Figure 2As shown, the powder XRD patterns of the prepared nitrogen-doped carbon semitube platinum-supported catalyst, Pt / C, and nitrogen-doped carbon semitube support show that the nitrogen-doped carbon semitube support exhibits only two carbon diffraction peaks at ~24° and 43°, while the nitrogen-doped carbon semitube platinum-supported catalyst and the commercial Pt / C catalyst exhibit typical platinum metal characteristic peaks. The TEM results of the nitrogen-doped carbon semitube platinum-supported catalyst are shown below. Figure 3 As shown, platinum particles are uniformly dispersed on the surface of nitrogen-doped carbon semiconductors, and the size of the platinum nanoparticles is 2-3 nm.

[0050] like Figure 4 As shown, the surface composition of the nitrogen-doped carbon semitube platinum-supported catalyst prepared in this embodiment is compared with that of the commercial Pt / C catalyst using Pt 4fXPS. The binding energy peak position of Pt 4f5 / 2 in the Pt / tube sample is 75 eV, and the peak position of Pt 4f7 / 2 is 71.6 eV. Compared with the corresponding peak positions of commercial Pt / C, the peak positions are shifted to lower energy directions by about 0.3 eV, indicating that less Pt oxide is formed in the Pt / tube compared to Pt / C. 0 The proportion of Pt / tube was 57%, higher than that of Pt / C (52%). Meanwhile, the nitrogen element in the sample included five types: pyridine-N, pyrrole-N, graphitic-N, Pt-N, and nitrogen oxide.

[0051] Next, the electrochemical performance of the nitrogen-doped carbon semi-tube supported platinum catalyst and the commercial Pt / C catalyst were tested. A standard three-electrode system was used, with a platinum sheet as the counter electrode and a saturated calomel electrode as the reference electrode. Oxygen reduction reaction tests were conducted in an oxygen-saturated 0.1M HClO4 electrolyte at an electrode rotation speed of 1600 rpm and a scan rate of 5 mV / s. Figure 5 As shown, the polarization curve results indicate that the half-wave potential of the oxygen reduction reaction of the nitrogen-doped carbon semitube-supported platinum catalyst is 0.89 V (vs. RHE), which is superior to that of commercial Pt / C catalysts.

[0052] Furthermore, the stability of the catalyst was tested: the prepared working electrode was subjected to initial cyclic voltammetry and oxygen reduction polarization curve testing. Then, the working electrode was placed in oxygen-saturated 0.1M HClO4 electrolyte, and a full potential range scan of 0.6–1.1 V (vs. RHE) was performed at a scan rate of 100 mV / s. After 10,000 cycles, the oxygen reduction polarization curve was tested again. Before and after 10,000 cycles: the half-wave potential of the ORR polarization curve of the nitrogen-doped carbon semi-tube platinum catalyst decreased slightly, only by 9 mV. Figure 6 As shown, the ORR polarization curve of the commercial Pt / C catalyst shows a 27 mV decrease in half-wave potential. (See [reference]). Figure 7 The above results demonstrate that the prepared nitrogen-doped carbon semi-tube platinum-supported catalyst exhibits excellent cycling stability.

[0053] Example 2

[0054] This embodiment is basically the same as Embodiment 1, except that:

[0055] In this embodiment, a method for preparing a platinum-based electrocatalyst using nitrogen-doped carbon semiconductors as a support includes the following steps:

[0056] (1) Weigh 0.016 mol of hexadecyltrimethylammonium bromide and dissolve it in water. Then, dissolve 1 g of m-phenylenediamine, add hydrochloric acid containing 0.1 mol of hydrogen chloride and 0.01 mol of ammonium persulfate, and carry out oxidative polymerization reaction for 24 h. Filter the product solution, collect the polymerization product, wash and dry the obtained polymerization product, and then place the clean and dry polymerization product under argon protection and carry out high-temperature pyrolysis at 900 °C for 3 h to obtain nitrogen-doped carbon half-tubes, which can be used as carrier materials for later use.

[0057] (2) Dissolve 0.0772 mmol of H2PtCl6 and 0.8 mmol of NaOH in ethylene glycol to obtain a reaction mixture. Place the reaction mixture in a microwave reactor and microwave it at 160°C for 2 min with a power of 80 W to obtain platinum nanoparticles. Purify them with 1 M hydrochloric acid and use them as catalyst active materials for later use.

[0058] (3) The platinum-based nanoparticles prepared in step (2) are thoroughly mixed with the nitrogen-doped carbon half-tubes prepared in step (1) to obtain a platinum-based electrocatalyst with nitrogen-doped carbon half-tubes as the support.

[0059] Test characterization:

[0060] In this embodiment, a nitrogen-doped carbon semi-tube platinum-supported catalyst was prepared using a microwave reaction power of 80 W. The electrochemical performance of the prepared nitrogen-doped carbon semi-tube platinum-supported catalyst was characterized using a standard three-electrode system, with a platinum sheet as the counter electrode and a saturated calomel electrode as the reference electrode. Oxygen reduction reaction (ORR) tests were conducted in an oxygen-saturated 0.1 M HClO4 electrolyte at an electrode rotation speed of 1600 rpm and a scan rate of 5 mV / s. The results show that the nitrogen-doped carbon semi-tube platinum-supported catalyst exhibits excellent OCR performance.

[0061] Example 3

[0062] This embodiment is basically the same as the above embodiments, except that:

[0063] In this embodiment, a method for preparing a platinum-based electrocatalyst using nitrogen-doped carbon semiconductors as a support includes the following steps:

[0064] (1) Weigh 0.016 mol of hexadecyltrimethylammonium bromide and dissolve it in water. Then, dissolve 1 g of m-phenylenediamine, add hydrochloric acid containing 0.1 mol of hydrogen chloride and 0.01 mol of ammonium persulfate, and carry out oxidative polymerization reaction for 24 h. Filter the product solution, collect the polymerization product, wash and dry the obtained polymerization product, and then place the clean and dry polymerization product under argon protection and carry out high-temperature pyrolysis at 900 °C for 3 h to obtain nitrogen-doped carbon half-tubes, which can be used as carrier materials for later use.

[0065] (2) Dissolve 0.0772 mmol of H2PtCl6 and 0.8 mmol of NaOH in ethylene glycol to obtain a reaction mixture. Place the reaction mixture in a microwave reactor and microwave it at 160°C for 2 min with a power of 800 W to obtain platinum nanoparticles. Purify them with 1 M hydrochloric acid and use them as catalyst active materials for later use.

[0066] (3) The platinum-based nanoparticles prepared in step (2) are thoroughly mixed with the nitrogen-doped carbon half-tubes prepared in step (1) to obtain a platinum-based electrocatalyst with nitrogen-doped carbon half-tubes as the support.

[0067] Test characterization:

[0068] In this embodiment, a nitrogen-doped carbon semi-tube platinum-supported catalyst was prepared using a microwave reaction power of 800 W. The electrochemical performance of the prepared nitrogen-doped carbon semi-tube platinum-supported catalyst was characterized using a standard three-electrode system, with a platinum sheet as the counter electrode and a saturated calomel electrode as the reference electrode. Oxygen reduction reaction (ORR) tests were conducted in an oxygen-saturated 0.1 M HClO4 electrolyte at an electrode rotation speed of 1600 rpm and a scan rate of 5 mV / s. The results show that the nitrogen-doped carbon semi-tube platinum-supported catalyst exhibits excellent OCR performance.

[0069] Example 4

[0070] This embodiment is basically the same as the above embodiments, except that:

[0071] In this embodiment, a method for preparing a platinum-based electrocatalyst using nitrogen-doped carbon semiconductors as a support includes the following steps:

[0072] (1) Weigh 0.016 mol of hexadecyltrimethylammonium bromide and dissolve it in water. Then, dissolve 1 g of m-phenylenediamine, add hydrochloric acid containing 0.1 mol of hydrogen chloride and 0.01 mol of ammonium persulfate, and carry out oxidative polymerization reaction for 24 h. Filter the product solution, collect the polymerization product, wash and dry the obtained polymerization product, and then place the clean and dry polymerization product under argon protection and carry out high-temperature pyrolysis at 900 °C for 3 h to obtain nitrogen-doped carbon half-tubes, which can be used as carrier materials for later use.

[0073] (2) Dissolve 0.0772 mmol of H2PtCl6 and 0.8 mmol of NaOH in ethylene glycol to obtain a reaction mixture. Place the reaction mixture in a microwave reactor and microwave it at 120°C for 2 min with a power of 160 W to obtain platinum nanoparticles. Purify them with 1 M hydrochloric acid and use them as catalyst active materials for later use.

[0074] (3) The platinum-based nanoparticles prepared in step (2) are thoroughly mixed with the nitrogen-doped carbon half-tubes prepared in step (1) to obtain a platinum-based electrocatalyst with nitrogen-doped carbon half-tubes as the support.

[0075] Test characterization:

[0076] In this embodiment, a nitrogen-doped carbon semi-tube platinum-supported catalyst was prepared using microwave reaction at 120℃. The electrochemical performance of the prepared nitrogen-doped carbon semi-tube platinum-supported catalyst was characterized using a standard three-electrode system, with a platinum sheet as the counter electrode and a saturated calomel electrode as the reference electrode. Oxygen reduction reaction (ORR) tests were conducted in an oxygen-saturated 0.1M HClO4 electrolyte at an electrode rotation speed of 1600 rpm and a scan rate of 5 mV / s. The results showed that the nitrogen-doped carbon semi-tube platinum-supported catalyst exhibited excellent OCR performance.

[0077] Example 5

[0078] This embodiment is basically the same as the above embodiments, except that:

[0079] In this embodiment, a method for preparing a platinum-based electrocatalyst using nitrogen-doped carbon semiconductors as a support includes the following steps:

[0080] (1) Weigh 0.016 mol of hexadecyltrimethylammonium bromide and dissolve it in water. Then, dissolve 1 g of m-phenylenediamine, add hydrochloric acid containing 0.1 mol of hydrogen chloride and 0.01 mol of ammonium persulfate, and carry out oxidative polymerization reaction for 24 h. Filter the product solution, collect the polymerization product, wash and dry the obtained polymerization product, and then place the clean and dry polymerization product under argon protection and carry out high-temperature pyrolysis at 900 °C for 3 h to obtain nitrogen-doped carbon half-tubes, which can be used as carrier materials for later use.

[0081] (2) Dissolve 0.0772 mmol of H2PtCl6 and 0.8 mmol of NaOH in ethylene glycol to obtain a reaction mixture. Place the reaction mixture in a microwave reactor and microwave it at 195°C for 2 min with a power of 160 W to obtain platinum nanoparticles. Purify them with 1 M hydrochloric acid and use them as catalyst active materials for later use.

[0082] (3) The platinum-based nanoparticles prepared in step (2) are thoroughly mixed with the nitrogen-doped carbon half-tubes prepared in step (1) to obtain a platinum-based electrocatalyst with nitrogen-doped carbon half-tubes as the support.

[0083] Test characterization:

[0084] In this embodiment, a nitrogen-doped carbon semi-tube platinum-supported catalyst was prepared using microwave reaction at 195℃. The electrochemical performance of the prepared nitrogen-doped carbon semi-tube platinum-supported catalyst was characterized using a standard three-electrode system, with a platinum sheet as the counter electrode and a saturated calomel electrode as the reference electrode. Oxygen reduction reaction (ORR) tests were conducted in an oxygen-saturated 0.1M HClO4 electrolyte at an electrode rotation speed of 1600 rpm and a scan rate of 5 mV / s. The results show that the nitrogen-doped carbon semi-tube platinum-supported catalyst exhibits excellent OCR performance.

[0085] Example 6

[0086] This embodiment is basically the same as the above embodiments, except that:

[0087] In this embodiment, a method for preparing a platinum-based electrocatalyst using nitrogen-doped carbon semiconductors as a support includes the following steps:

[0088] (1) Weigh 0.016 mol of hexadecyltrimethylammonium bromide and dissolve it in water. Then, dissolve 1 g of m-phenylenediamine, add hydrochloric acid containing 0.1 mol of hydrogen chloride and 0.01 mol of ammonium persulfate, and carry out oxidative polymerization reaction for 24 h. Filter the product solution, collect the polymerization product, wash and dry the obtained polymerization product, and then place the clean and dry polymerization product under argon protection and carry out high-temperature pyrolysis at 900 °C for 3 h to obtain nitrogen-doped carbon half-tubes, which can be used as carrier materials for later use.

[0089] (2) Dissolve 0.0772 mmol of H2PtCl6 and 0.8 mmol of NaOH in ethylene glycol to obtain a reaction mixture. Place the reaction mixture in a microwave reactor and microwave it at 160°C for 0.5 min with a power of 160 W to obtain platinum nanoparticles. Purify them with 1 M hydrochloric acid and use them as catalyst active materials for later use.

[0090] (3) The platinum-based nanoparticles prepared in step (2) are thoroughly mixed with the nitrogen-doped carbon half-tubes prepared in step (1) to obtain a platinum-based electrocatalyst with nitrogen-doped carbon half-tubes as the support.

[0091] Test characterization:

[0092] In this embodiment, a nitrogen-doped carbon semi-tube platinum-supported catalyst was prepared using a microwave reaction time of 0.5 min. The electrochemical performance of the prepared nitrogen-doped carbon semi-tube platinum-supported catalyst was characterized using a standard three-electrode system, with a platinum sheet as the counter electrode and a saturated calomel electrode as the reference electrode. Oxygen reduction reaction (ORR) tests were conducted in an oxygen-saturated 0.1 M HClO4 electrolyte at an electrode rotation speed of 1600 rpm and a scan rate of 5 mV / s. The results showed that the nitrogen-doped carbon semi-tube platinum-supported catalyst exhibited excellent OCR performance.

[0093] Example 7

[0094] This embodiment is basically the same as the above embodiments, except that:

[0095] In this embodiment, a platinum-based electrocatalyst using nitrogen-doped carbon semiconductors as a support is described. The nitrogen-doped carbon semiconductors are used as the support, and platinum-based nanoparticles are used as the active particles of the catalyst. The platinum-based nanoparticles are uniformly distributed on the surface of the nitrogen-doped carbon semiconductors to form a platinum-based electrocatalyst with a carbon support structure doped with heteroatoms.

[0096] In this embodiment, a method for preparing a platinum-based electrocatalyst using nitrogen-doped carbon semiconductors as a support includes the following steps:

[0097] (1) Weigh 0.016 mol of hexadecyltrimethylammonium bromide and dissolve it in water. Then, dissolve 1 g of m-phenylenediamine, add hydrochloric acid containing 0.1 mol of hydrogen chloride and 0.01 mol of ammonium persulfate, and carry out oxidative polymerization reaction for 24 h. Filter the product solution, collect the polymerization product, wash and dry the obtained polymerization product, and then place the clean and dry polymerization product under argon protection and carry out high-temperature pyrolysis at 900 °C for 3 h to obtain nitrogen-doped carbon half-tubes, which can be used as carrier materials for later use.

[0098] (2) Dissolve 0.077 mmol of H2PtCl6 and 0.8 mmol of NaOH in ethylene glycol to obtain a reaction mixture. Place the reaction mixture in a microwave reactor and microwave it at 160°C for 30 min with a power of 160 W to obtain platinum nanoparticles. Purify them with 1 M hydrochloric acid and use them as catalyst active materials for later use.

[0099] (3) The platinum-based nanoparticles prepared in step (2) are thoroughly mixed with the nitrogen-doped carbon half-tubes prepared in step (1) to obtain a platinum-based electrocatalyst with nitrogen-doped carbon half-tubes as the support.

[0100] Test characterization:

[0101] In this embodiment, a nitrogen-doped carbon semi-tube platinum-supported catalyst was prepared using a microwave reaction time of 30 min. The electrochemical performance of the prepared nitrogen-doped carbon semi-tube platinum-supported catalyst was characterized using a standard three-electrode system, with a platinum sheet as the counter electrode and a saturated calomel electrode as the reference electrode. Oxygen reduction reaction (ORR) tests were conducted in an oxygen-saturated 0.1 M HClO4 electrolyte at an electrode rotation speed of 1600 rpm and a scan rate of 5 mV / s. The results show that the nitrogen-doped carbon semi-tube platinum-supported catalyst exhibits excellent OCR performance.

[0102] Example 8

[0103] This embodiment is basically the same as the above embodiments, except that:

[0104] In this embodiment, a platinum-based electrocatalyst using nitrogen-doped carbon semiconductors as a support is described. The nitrogen-doped carbon semiconductors are used as the support, and platinum-based nanoparticles are used as the active particles of the catalyst. The platinum-based nanoparticles are uniformly distributed on the surface of the nitrogen-doped carbon semiconductors to form a platinum-based electrocatalyst with a carbon support structure doped with heteroatoms.

[0105] In this embodiment, a method for preparing a platinum-based electrocatalyst using nitrogen-doped carbon semiconductors as a support includes the following steps:

[0106] (1) Weigh 0.016 mol of hexadecyltrimethylammonium bromide and dissolve it in water. Then, dissolve 1 g of m-phenylenediamine, add hydrochloric acid containing 0.1 mol of hydrogen chloride and 0.01 mol of ammonium persulfate, and carry out oxidative polymerization reaction for 24 h. Filter the product solution, collect the polymerization product, wash and dry the obtained polymerization product, and then place the clean and dry polymerization product under argon protection and carry out high-temperature pyrolysis at 900 °C for 3 h to obtain nitrogen-doped carbon half-tubes, which can be used as carrier materials for later use.

[0107] (2) Dissolve 0.0772 mmol of H2PtCl6 and 0.1 mmol of NaOH in ethylene glycol to obtain a reaction mixture. Place the reaction mixture in a microwave reactor and microwave it at 160°C for 2 min with a power of 160 W to obtain platinum nanoparticles. Purify them with 1 M hydrochloric acid and use them as catalyst active materials for later use.

[0108] (3) The platinum-based nanoparticles prepared in step (2) are thoroughly mixed with the nitrogen-doped carbon half-tubes prepared in step (1) to obtain a platinum-based electrocatalyst with nitrogen-doped carbon half-tubes as the support.

[0109] Test characterization:

[0110] In this embodiment, the electrochemical performance of the prepared nitrogen-doped carbon semi-tube platinum catalyst was characterized using a standard three-electrode system with a platinum compound to sodium hydroxide molar ratio of 1:2.5. The counter electrode was a platinum sheet, and the reference electrode was a saturated calomel electrode. Oxygen reduction reaction (ORR) tests were conducted in an oxygen-saturated 0.1M HClO4 electrolyte at an electrode rotation speed of 1600 rpm and a scan rate of 5 mV / s. The results showed that the nitrogen-doped carbon semi-tube platinum catalyst exhibited excellent OCR performance.

[0111] Example 9

[0112] This embodiment is basically the same as the above embodiments, except that:

[0113] In this embodiment, a platinum-based electrocatalyst using nitrogen-doped carbon semiconductors as a support is described. The nitrogen-doped carbon semiconductors are used as the support, and platinum-based nanoparticles are used as the active particles of the catalyst. The platinum-based nanoparticles are uniformly distributed on the surface of the nitrogen-doped carbon semiconductors to form a platinum-based electrocatalyst with a carbon support structure doped with heteroatoms.

[0114] In this embodiment, a method for preparing a platinum-based electrocatalyst using nitrogen-doped carbon semiconductors as a support includes the following steps:

[0115] (1) Weigh 0.016 mol of hexadecyltrimethylammonium bromide and dissolve it in water. Then, dissolve 1 g of m-phenylenediamine, add hydrochloric acid containing 0.1 mol of hydrogen chloride and 0.01 mol of ammonium persulfate, and carry out oxidative polymerization reaction for 24 h. Filter the product solution, collect the polymerization product, wash and dry the obtained polymerization product, and then place the clean and dry polymerization product under argon protection and carry out high-temperature pyrolysis at 900 °C for 3 h to obtain nitrogen-doped carbon half-tubes, which can be used as carrier materials for later use.

[0116] (2) Dissolve 0.0772 mmol of H2PtCl6 and 3.2 mmol of NaOH in ethylene glycol to obtain a reaction mixture. Place the reaction mixture in a microwave reactor and microwave it at 160°C for 2 min with a power of 160 W to obtain platinum nanoparticles. Purify them with 1M hydrochloric acid and use them as catalyst active materials for later use.

[0117] (3) The platinum-based nanoparticles prepared in step (2) are thoroughly mixed with the nitrogen-doped carbon half-tubes prepared in step (1) to obtain a platinum-based electrocatalyst with nitrogen-doped carbon half-tubes as the support.

[0118] Test characterization:

[0119] In this embodiment, a nitrogen-doped carbon semi-tube platinum-supported catalyst was prepared using a platinum compound to sodium hydroxide molar ratio of 1:40. The electrochemical performance of the prepared nitrogen-doped carbon semi-tube platinum-supported catalyst was characterized using a standard three-electrode system, with a platinum sheet as the counter electrode and a saturated calomel electrode as the reference electrode. Oxygen reduction reaction (ORR) tests were conducted in an oxygen-saturated 0.1M HClO4 electrolyte at an electrode rotation speed of 1600 rpm and a scan rate of 5 mV / s. The results show that the nitrogen-doped carbon semi-tube platinum-supported catalyst exhibits excellent OCR performance.

[0120] Example 10

[0121] This embodiment is basically the same as the above embodiments, except that:

[0122] In this embodiment, a platinum-based electrocatalyst using nitrogen-doped carbon semiconductors as a support is described. The nitrogen-doped carbon semiconductors are used as the support, and platinum-based nanoparticles are used as the active particles of the catalyst. The platinum-based nanoparticles are uniformly distributed on the surface of the nitrogen-doped carbon semiconductors to form a platinum-based electrocatalyst with a carbon support structure doped with heteroatoms.

[0123] In this embodiment, a method for preparing a platinum-based electrocatalyst using nitrogen-doped carbon semiconductors as a support includes the following steps:

[0124] (1) Weigh 0.016 mol of hexadecyltrimethylammonium bromide and dissolve it in water. Then, dissolve 1 g of m-phenylenediamine, add hydrochloric acid containing 0.1 mol of hydrogen chloride and 0.01 mol of ammonium persulfate, and carry out oxidative polymerization reaction for 24 h. Filter the product solution, collect the polymerization product, wash and dry the obtained polymerization product, and then place the clean and dry polymerization product under argon protection and carry out high-temperature pyrolysis at 900 °C for 3 h to obtain nitrogen-doped carbon half-tubes, which can be used as carrier materials for later use.

[0125] (2) 0.2316 mmol of FeCl3·6H2O, 0.0772 mmol of H2PtCl6 and 0.8 mmol of NaOH were dissolved in ethylene glycol to obtain a reaction mixture. The reaction mixture was placed in a microwave reactor and microwaved at 160°C for 2 min with a power of 160 W to obtain iron-platinum alloy nanoparticles. The nanoparticles were purified with 1M hydrochloric acid and used as catalyst active materials for later use.

[0126] (3) The platinum-based nanoparticles prepared in step (2) are thoroughly mixed with the nitrogen-doped carbon half-tubes prepared in step (1) to obtain a platinum-based electrocatalyst with nitrogen-doped carbon half-tubes as the support.

[0127] Test characterization:

[0128] In this embodiment, an iron compound was added to prepare a nitrogen-doped carbon semi-tube supported iron-platinum alloy catalyst. The electrochemical performance of the prepared nitrogen-doped carbon semi-tube supported platinum catalyst was characterized using a standard three-electrode system, with a platinum sheet as the counter electrode and a saturated calomel electrode as the reference electrode. Oxygen reduction reaction (ORR) tests were conducted in an oxygen-saturated 0.1M HClO4 electrolyte at an electrode rotation speed of 1600 rpm and a scan rate of 5 mV / s. The results indicate that the prepared nitrogen-doped carbon semi-tube supported iron-platinum catalyst exhibits excellent OCR performance.

[0129] Example 11

[0130] This embodiment is basically the same as the above embodiments, except that:

[0131] In this embodiment, a platinum-based electrocatalyst using nitrogen-doped carbon semiconductors as a support is described. The nitrogen-doped carbon semiconductors are used as the support, and platinum-based nanoparticles are used as the active particles of the catalyst. The platinum-based nanoparticles are uniformly distributed on the surface of the nitrogen-doped carbon semiconductors to form a platinum-based electrocatalyst with a carbon support structure doped with heteroatoms.

[0132] In this embodiment, a method for preparing a platinum-based electrocatalyst using nitrogen-doped carbon semiconductors as a support includes the following steps:

[0133] (1) Weigh 0.016 mol of hexadecyltrimethylammonium bromide and dissolve it in water. Then, dissolve 1 g of m-phenylenediamine, add hydrochloric acid containing 0.1 mol of hydrogen chloride and 0.01 mol of ammonium persulfate, and carry out oxidative polymerization reaction for 24 h. Filter the product solution, collect the polymerization product, wash and dry the obtained polymerization product, and then place the clean and dry polymerization product under argon protection and carry out high-temperature pyrolysis at 900 °C for 3 h to obtain nitrogen-doped carbon half-tubes, which can be used as carrier materials for later use.

[0134] (2) Dissolve 0.1544 mmol of CoCl2·6H2O, 0.0772 mmol of H2PtCl6 and 0.8 mmol of NaOH in ethylene glycol to obtain a reaction mixture. Place the reaction mixture in a microwave reactor and microwave it at 160°C for 2 min with a power of 160 W to obtain platinum-cobalt alloy nanoparticles. Purify them with 1M hydrochloric acid and use them as catalyst active materials for later use.

[0135] (3) The platinum-based nanoparticles prepared in step (2) are thoroughly mixed with the nitrogen-doped carbon half-tubes prepared in step (1) to obtain a platinum-based electrocatalyst with nitrogen-doped carbon half-tubes as the support.

[0136] Test characterization:

[0137] In this embodiment, a nitrogen-doped carbon semi-tube platinum-cobalt alloy catalyst was prepared by adding cobalt compounds. The electrochemical performance of the prepared nitrogen-doped carbon semi-tube platinum-supported catalyst was characterized using a standard three-electrode system, with a platinum sheet as the counter electrode and a saturated calomel electrode as the reference electrode. Oxygen reduction reaction (ORR) tests were conducted in an oxygen-saturated 0.1M HClO4 electrolyte at an electrode rotation speed of 1600 rpm and a scan rate of 5 mV / s. The results indicate that the prepared nitrogen-doped carbon semi-tube platinum-cobalt catalyst exhibits excellent OCR performance.

[0138] Example 12

[0139] This embodiment is basically the same as the above embodiments, except that:

[0140] In this embodiment, a platinum-based electrocatalyst using nitrogen-doped carbon semiconductors as a support is described. The nitrogen-doped carbon semiconductors are used as the support, and platinum-based nanoparticles are used as the active particles of the catalyst. The platinum-based nanoparticles are uniformly distributed on the surface of the nitrogen-doped carbon semiconductors to form a platinum-based electrocatalyst with a carbon support structure doped with heteroatoms.

[0141] In this embodiment, a method for preparing a platinum-based electrocatalyst using nitrogen-doped carbon semiconductors as a support includes the following steps:

[0142] (1) Weigh 0.016 mol of hexadecyltrimethylammonium bromide and dissolve it in water. Then, dissolve 1 g of m-phenylenediamine, add hydrochloric acid containing 0.1 mol of hydrogen chloride and 0.01 mol of ammonium persulfate, and carry out oxidative polymerization reaction for 24 h. Filter the product solution, collect the polymerization product, wash and dry the obtained polymerization product, and then place the clean and dry polymerization product under argon protection and carry out high-temperature pyrolysis at 900 °C for 3 h to obtain nitrogen-doped carbon half-tubes, which can be used as carrier materials for later use.

[0143] (2) Dissolve 0.2316 mmol of NiCl2·6H2O, 0.0772 mmol of H2PtCl6 and 0.8 mmol of NaOH in ethylene glycol to obtain a reaction mixture. Place the reaction mixture in a microwave reactor and microwave it at 160°C for 2 min with a power of 160 W to obtain platinum-nickel alloy nanoparticles. Purify them with 1M hydrochloric acid and use them as catalyst active materials for later use.

[0144] (3) The platinum-based nanoparticles prepared in step (2) are thoroughly mixed with the nitrogen-doped carbon half-tubes prepared in step (1) to obtain a platinum-based electrocatalyst with nitrogen-doped carbon half-tubes as the support.

[0145] Test characterization:

[0146] In this embodiment, a nitrogen-doped carbon semi-tube supported platinum-nickel alloy catalyst was prepared by adding nickel compounds. The electrochemical performance of the prepared nitrogen-doped carbon semi-tube supported platinum catalyst was characterized using a standard three-electrode system, with a platinum sheet as the counter electrode and a saturated calomel electrode as the reference electrode. Oxygen reduction reaction (ORR) tests were conducted in an oxygen-saturated 0.1M HClO4 electrolyte at an electrode rotation speed of 1600 rpm and a scan rate of 5 mV / s. The results indicate that the prepared nitrogen-doped carbon semi-tube supported platinum-nickel catalyst exhibits excellent OCR performance.

[0147] Example 13

[0148] This embodiment is basically the same as the above embodiments, except that:

[0149] In this embodiment, a platinum-based electrocatalyst using nitrogen-doped carbon semiconductors as a support is described. The nitrogen-doped carbon semiconductors are used as the support, and platinum-based nanoparticles are used as the active particles of the catalyst. The platinum-based nanoparticles are uniformly distributed on the surface of the nitrogen-doped carbon semiconductors to form a platinum-based electrocatalyst with a carbon support structure doped with heteroatoms.

[0150] In this embodiment, a method for preparing a platinum-based electrocatalyst using nitrogen-doped carbon semiconductors as a support includes the following steps:

[0151] (1) Weigh 0.016 mol of hexadecyltrimethylammonium bromide and dissolve it in water. Then, dissolve 1 g of m-phenylenediamine, add hydrochloric acid containing 0.1 mol of hydrogen chloride and 0.01 mol of ammonium persulfate, and carry out oxidative polymerization reaction for 24 h. Filter the product solution, collect the polymerization product, wash and dry the obtained polymerization product, and then place the clean and dry polymerization product under argon protection and carry out high-temperature pyrolysis at 900 °C for 3 h to obtain nitrogen-doped carbon half-tubes, which can be used as carrier materials for later use.

[0152] (2) Dissolve 0.0772 mmol of CuCl2·6H2O, 0.0772 mmol of H2PtCl6 and 0.8 mmol of NaOH in ethylene glycol to obtain a reaction mixture. Place the reaction mixture in a microwave reactor and microwave it at 160°C for 2 min with a power of 160 W to obtain platinum-copper alloy nanoparticles. Purify them with 1M hydrochloric acid and use them as catalyst active materials for later use.

[0153] (3) The platinum-based nanoparticles prepared in step (2) are thoroughly mixed with the nitrogen-doped carbon half-tubes prepared in step (1) to obtain a platinum-based electrocatalyst with nitrogen-doped carbon half-tubes as the support.

[0154] Test characterization:

[0155] In this embodiment, a nitrogen-doped carbon semi-tube supported platinum-copper alloy catalyst was prepared by adding copper compounds. The electrochemical performance of the prepared nitrogen-doped carbon semi-tube supported platinum catalyst was characterized using a standard three-electrode system, with a platinum sheet as the counter electrode and a saturated calomel electrode as the reference electrode. Oxygen reduction reaction (ORR) tests were conducted in an oxygen-saturated 0.1M HClO4 electrolyte at an electrode rotation speed of 1600 rpm and a scan rate of 5 mV / s. The results show that the nitrogen-doped carbon semi-tube supported platinum-copper catalyst exhibits excellent OCR performance.

[0156] The present invention relates to a platinum-based electrocatalyst with nitrogen-doped carbon semiconductors as a support and its preparation method. In preparing the nitrogen-doped carbon semiconductor support, a certain amount of surfactant, amine compound, and acid are dissolved in water, followed by the addition of ammonium persulfate for oxidative polymerization. The mixture is then filtered, washed, and dried. The polymerization product is then subjected to high-temperature pyrolysis in an inert gas atmosphere to obtain the nitrogen-doped carbon semiconductor. In preparing the platinum-based nanoparticles, a certain amount of platinum compound, transition metal compound, and sodium hydroxide are dissolved in ethylene glycol and placed in a microwave reactor. The mixture is then subjected to microwave reaction at a specific power and temperature to obtain platinum-based nanoparticles. Finally, the platinum-based nanoparticles are thoroughly mixed with the nitrogen-doped carbon semiconductor support to obtain the platinum-based electrocatalyst with nitrogen-doped carbon semiconductors as a support. The catalyst prepared in the above embodiments of the present invention exhibits excellent oxygen reduction reaction (ORR) catalytic activity and good durability. Furthermore, the preparation method is simple and easy to implement, making it suitable for large-scale production.

[0157] The embodiments of the present invention have been described above in conjunction with the accompanying drawings. However, the present invention is not limited to the above embodiments. Various changes can be made according to the purpose of the invention. Any changes, modifications, substitutions, combinations or simplifications made based on the spirit and principle of the technical solution of the present invention shall be equivalent substitutions. As long as they meet the purpose of the invention and do not deviate from the technical principle and inventive concept of the present invention, they shall fall within the protection scope of the present invention.

Claims

1. A platinum-based electrocatalyst utilizing nitrogen-doped carbon semiconductors as a support, characterized in that: Using nitrogen-doped carbon semitubes as a support, the nitrogen-doped carbon semitubes have a semitube structure, and platinum-based nanoparticles as the catalyst active particles, the platinum-based nanoparticles are uniformly distributed on the surface of the nitrogen-doped carbon semitubes to form a platinum-based electrocatalyst with a heteroatomic doped carbon support. Based on a total atomic percentage of 100% for the platinum-based electrocatalyst, the nitrogen doping amount is 0~20 at%; the nitrogen element in the platinum-based electrocatalyst includes five types: pyridine-N, pyrrole-N, graphitic-N, Pt-N, and nitrogen oxide. The platinum-based electrocatalyst is prepared by the following method, which includes the following steps: (1) Dissolve surfactant, amine compound, and acid in water, then add ammonium persulfate for oxidative polymerization, filter the resulting product solution, collect the polymerization product, wash and dry the obtained polymerization product, and then place the clean and dry polymerization product in an inert gas for high-temperature pyrolysis to obtain nitrogen-doped carbon semiconductor, which can be used as a carrier material for later use; the amine compound is m-phenylenediamine. (2) Dissolve platinum compound and alkali in ethylene glycol, or dissolve platinum compound, transition metal compound and alkali in ethylene glycol to obtain a reaction mixture. Place the reaction mixture in a microwave reactor and carry out a microwave reaction to obtain platinum-based nanoparticles, which can be used as catalyst active materials for later use. (3) The platinum-based nanoparticles prepared in step (2) are thoroughly mixed with the nitrogen-doped carbon half-tubes prepared in step (1) to obtain a platinum-based electrocatalyst with nitrogen-doped carbon half-tubes as the support.

2. The platinum-based electrocatalyst using nitrogen-doped carbon semiconductors as a support according to claim 1, characterized in that: The carbon half-tube has a diameter of 1~200 nm and a length of 10 nm~20 μm.

3. The platinum-based electrocatalyst using nitrogen-doped carbon semiconductors as a support according to claim 1, characterized in that: The platinum-based nanoparticles have a particle size of 1~5 nm, and the molar ratio of the added transition metal to platinum is (0~10):

1.

4. A method for preparing a platinum-based electrocatalyst using nitrogen-doped carbon semiconductors as a support, as described in claim 1, characterized in that, Includes the following steps: (1) Dissolve surfactant, amine compound, and acid in water, then add ammonium persulfate for oxidative polymerization, filter the resulting product solution, collect the polymerization product, wash and dry the obtained polymerization product, and then place the clean and dry polymerization product in an inert gas for high-temperature pyrolysis to obtain nitrogen-doped carbon semiconductor, which can be used as a carrier material for later use; the amine compound is m-phenylenediamine. (2) Dissolve platinum compounds, transition metal compounds and alkali in ethylene glycol to obtain a reaction mixture. Place the reaction mixture in a microwave reactor and carry out a microwave reaction to obtain platinum-based nanoparticles, which can be used as catalyst active materials for later use. (3) The platinum-based nanoparticles prepared in step (2) are thoroughly mixed with the nitrogen-doped carbon half-tubes prepared in step (1) to obtain a platinum-based electrocatalyst with nitrogen-doped carbon half-tubes as the support.

5. The method for preparing a platinum-based electrocatalyst using a nitrogen-doped carbon semiconductor as a support according to claim 4, characterized in that: In step (1), the surfactant is at least one of cationic surfactants, anionic surfactants, and nonionic surfactants with different carbon chain lengths; Alternatively, in step (1), the acid is at least one of inorganic acid and organic acid.

6. The method for preparing a platinum-based electrocatalyst using a nitrogen-doped carbon semiconductor as a support according to claim 4, characterized in that: In step (1), the molar ratio of surfactant, amine compound, acid, and ammonium persulfate is (0~10): 1 : (0~20): (0~2); Alternatively, in step (1), the oxidative polymerization reaction lasts for at least 24 hours; the pyrolysis temperature is 600~1200℃, and the pyrolysis time is 0.5~5 hours.

7. The method for preparing a platinum-based electrocatalyst using a nitrogen-doped carbon semiconductor as a support according to claim 4, characterized in that: In step (2), the platinum compound is at least one of platinum acetylacetonate, chloroplatinic acid, potassium chloroplatinate, and platinum chloride; Alternatively, in step (2), the transition metal compound is at least one of palladium, silver, gold, molybdenum, tungsten, iron, cobalt, nickel, copper, and zinc compounds; Alternatively, in step (2), the base may be sodium hydroxide, potassium hydroxide, or other hydroxides that are readily soluble in ethylene glycol solvent.

8. The method for preparing a platinum-based electrocatalyst using a nitrogen-doped carbon semiconductor as a support according to claim 4, characterized in that: In step (2), the molar ratio of platinum compound, transition metal compound, and alkali is 1:(0-10):(2.5-40); when the amount of transition metal compound is 0, pure platinum nanoparticles are synthesized; when the amount of transition metal compound is not 0, platinum alloy nanoparticles are synthesized. Alternatively, in step (2), the power of the microwave reaction is 80~800 W, the temperature is 120~195℃, and the reaction time is 0.5~30 min; the platinum-based nanoparticles are purified using hydrochloric acid with a molar concentration of not less than 1 M.

9. The method for preparing a platinum-based electrocatalyst using a nitrogen-doped carbon semiconductor as a support according to claim 4, characterized in that: In steps (1) and (2), the molar ratio of surfactant to platinum compound is (0~100):

1.

10. The method for preparing a platinum-based electrocatalyst using a nitrogen-doped carbon semiconductor as a support according to claim 4, characterized in that: In step (3), the mass ratio of platinum-based nanoparticles to nitrogen-doped carbon semiconductors is (0~1000):1, and the amount of platinum-based nanoparticles added is not 0.

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