Method for second-level ultrafast preparation of metal-free element type piezoelectric catalytic material and water treatment application of second-level ultrafast preparation of metal-free element type piezoelectric catalytic material

Abstract

The invention discloses a method for preparing a metal-free element type piezoelectric catalytic material through magnetic induction heating, and particularly relates to research on preparation of a C3N5 material. By optimizing the preparation process, second-level ultra-fast preparation is achieved, the obtained material has excellent piezoelectric catalytic performance, and a new solution is provided for solving the problems that a traditional piezoelectric catalytic material is high in preparation cost, scarce in resources and the like. Meanwhile, the invention also explores the application of the piezoelectric catalytic material in water treatment, which indicates that the piezoelectric catalytic material has potential application value in the aspect of organic pollutant degradation, and provides a new technical approach for protection and treatment of water resources.

Description

[Technical field]

[0001] The present invention belongs to the technical field of catalytic materials, and relates to a second-level ultra-fast preparation of a metal-free piezoelectric catalytic material and its application in the field of water treatment. The present invention aims to provide a method for preparing a metal-free piezoelectric catalytic material by magnetic induction heating, and is particularly aimed at the preparation of C3N5 materials. By optimizing the preparation process, ultra-fast preparation in seconds is achieved, and the obtained material has excellent piezoelectric catalytic performance, which provides a new solution to solve the problems of high preparation cost and scarce resources of traditional piezoelectric catalytic materials. [Background technology]

[0002] As a functional material with excellent catalytic performance, piezoelectric catalytic materials have broad application prospects in environmental governance, energy conversion and other fields. Traditional piezoelectric catalytic materials usually contain rare metal elements, such as palladium and platinum. These materials have high preparation costs, scarce resources, and potential environmental pollution, which limits their development in large-scale applications. Therefore, it is of great significance to develop a piezoelectric catalytic material without metal elements.

[0003] In recent years, carbon-based materials have become one of the research hotspots due to their abundant resources, good chemical stability and tunable structural properties. Among them, carbon nitride materials are widely used in catalysis, photoelectrocatalysis and electrochemistry due to their high specific surface area, excellent electron transport performance and abundant surface active sites.

[0004] Patent CN117756069B discloses a C3N5 material with double defect sites to enhance the piezoelectric effect. Oxygen-doped C3N5 (C3N5-O) was obtained by one-step polymerization in a nitrogen atmosphere at 500°C, and then pyrolyzed again in an air atmosphere to introduce nitrogen vacancies in C3N5-O to obtain C3N 5-x-O oxygen doping and nitrogen vacancies are both defect sites in C3N5, which can enhance the in-plane polarization of C3N5. Then, this material is used to catalyze the degradation of pollutants in sewage through piezoelectric catalysis. The production rate of H2O2 in pure water is only 0.615mM / (g·h). In addition, additional iron-containing reagents need to be added to form a Fenton system for pollutant degradation. Patent CN113210005B discloses a Cl-doped C3N5 and a preparation method thereof, belonging to the field of photocatalysis technology. The preparation method is to fully mix ammonium chloride, 3-amino-1,2,4-triazole and a six-membered nitrogen heterocycle, and heat them at 500-550°C for more than 1.5h through a programmed temperature increase, and then take them out after cooling, wash them, and dry them to obtain Cl-doped C3N5. The calcination is carried out in air or nitrogen atmosphere. The Cl of the present invention is successfully doped into C3N5, and the band gap value is low, which is beneficial to photocatalysis. In addition, the porosity of the Cl-doped C3N5 of the present invention is also increased compared with C3N5. However, the traditional method for preparing carbon nitride materials usually requires high-temperature calcination or a complex synthesis process, and the preparation process is relatively time-consuming, which limits its promotion in practical applications.

[0005] The present invention provides a method for preparing a metal-free piezoelectric catalytic material by magnetic induction heating, and particularly studies the preparation of C3N5 materials. As a new heating method, magnetic induction heating has the advantages of fast heating speed, low energy consumption, and uniform reaction, and is widely used in material preparation, chemical reaction and other fields. [Summary of the invention]

[0006] [Technical issues to be solved]

[0007] The present invention aims to provide a method for preparing metal-free piezoelectric catalytic materials by magnetic induction heating, and is particularly aimed at the preparation of C3N5 materials. By optimizing the preparation process, ultra-fast preparation in seconds is achieved, and the obtained material has excellent piezoelectric catalytic performance, providing a new solution to the problems of high preparation cost and scarce resources of traditional piezoelectric catalytic materials.

[0008] [Technical solution]

[0009] 1. (1) Place 2.0 g to 5 g of 3-amino-1,2,4-triazole and 0.1-2 g of sodium hydroxide in a ball mill reactor and mill at 100-800 rpm for 1-8 hours;

[0010] (2) drying the obtained solid mixture in a vacuum oven at 50° C. to 100° C. for 4 to 12 hours;

[0011] (3) loading the dried substance onto an iron sheet covered with a graphite paper having a thickness of 0.01 mm to 0.05 mm, wherein the size of the iron sheet is 2 cm to 5 cm×2 cm to 5 cm×0.1 mm to 0.5 mm;

[0012] (4) placing the above assembly in a refractory brick in a quartz tube and purging with high-purity inert gas for 5 to 30 minutes;

[0013] (5) placing the quartz tube in a multi-turn induction coil with a diameter of 3 cm to 7 cm and performing magnetic induction heating for 5 seconds to 30 seconds under a controlled current (X = 50 to 800 A);

[0014] (6) After magnetic induction heating, the sample is allowed to cool naturally to room temperature, and finally a tungsten disulfide-based piezoelectric catalytic material is obtained for water treatment applications.

[0015] (7) The prepared piezoelectric catalyst material was added to a water sample containing organic pollutants at a mass concentration of 10-1000 mg / L, and the removal rate of the pollutants was measured after ultrasonic treatment for 1-60 minutes or stirring for 0.1-6 hours to evaluate the piezoelectric catalytic efficiency of the material.

[0016] [Beneficial Effects]

[0017] Compared with the prior art, the advantages and beneficial effects of the present invention are:

[0018] (1) The present invention provides a method for preparing a metal-free piezoelectric catalytic material by magnetic induction heating.

[0019] (2) The material obtained by the preparation method provided by the present invention has excellent piezoelectric catalytic performance, which provides a new solution to solve the problems of high preparation cost and scarce resources of traditional piezoelectric catalytic materials.

Brief Description of the Drawings

[0020] Figure 1 Transmission electron microscopy (TEM) image of the C3N5 piezoelectric catalytic material prepared after Example 1.

[0021] Figure 2 Raman spectrum of the C3N5 piezoelectric catalytic material prepared after Example 1.

[0022] Figure 3 A diagram showing the effect of the C3N5 piezoelectric catalytic material prepared after Example 1 in degrading the rhodamine b organic pollutant. [Specific implementation method]

[0023] Embodiment 1:

[0024] (1) 3-amino-1,2,4-triazole (2.0 g) and sodium hydroxide (0.1 g) were placed in a ball mill reactor, and the ball mill reactor was milled at 200 rpm for 4 hours to achieve sufficient mixing and reaction of the raw materials.

[0025] (2) The solid mixture obtained after ball milling was placed in a vacuum oven and dried at 80° C. for 8 hours to remove moisture therein.

[0026] (3) The dried material is loaded onto an iron sheet with a size of 4 cm×4 cm×0.2 mm. The surface of the iron sheet is covered with a piece of graphite paper with a thickness of 0.03 mm to ensure the uniformity and stability of the loaded material.

[0027] (4) Place the iron sheet in the refractory brick inside the quartz tube and purge it with nitrogen for 15 minutes to keep the reaction environment pure.

[0028] (5) The quartz tube was placed in a multi-turn induction coil with a diameter of 5 cm, and a controlled current (X=500 A) was applied to perform magnetic induction heating for 15 seconds.

[0029] (6) After completing the magnetic induction heating, the sample is allowed to cool naturally to room temperature, and finally a tungsten disulfide-based piezoelectric catalytic material is obtained.

[0030] (7) The prepared piezoelectric catalyst material is added into a water sample containing organic pollutants at a mass concentration of 100 mg / L.

[0031] (8) After 30 minutes of ultrasonic treatment, the removal rate of pollutants was measured and the piezoelectric catalytic efficiency of the material was evaluated. The specific results are shown in the attached Figure 3 .

[0032] Embodiment 2:

[0033] (1) 3-amino-1,2,4-triazole (4.0 g) and sodium hydroxide (1.5 g) were placed in a ball mill reactor, and the ball mill reactor was milled at 300 rpm for 6 hours to ensure that the raw materials were fully mixed and reacted.

[0034] (2) The solid mixture obtained after ball milling was placed in a vacuum oven and dried at 70° C. for 10 hours to remove moisture therein.

[0035] (3) The dried material is loaded onto an iron sheet with a size of 3 cm×3 cm×0.3 mm. The surface of the iron sheet is covered with a piece of graphite paper with a thickness of 0.04 mm to ensure the uniformity and stability of the loaded material.

[0036] (4) Place the iron sheet in a refractory brick inside a quartz tube and purge it with nitrogen for 20 minutes to keep the reaction environment pure.

[0037] (5) The quartz tube was placed in a multi-turn induction coil with a diameter of 6 cm, and a controlled current (X=600 A) was applied to perform magnetic induction heating for 20 seconds.

[0038] (6) After completing the magnetic induction heating, the sample is allowed to cool naturally to room temperature, and finally a tungsten disulfide-based piezoelectric catalytic material is obtained.

[0039] (7) The prepared piezoelectric catalyst material is added into a water sample containing organic pollutants at a mass concentration of 500 mg / L.

[0040] (8) After stirring for 3 hours, the removal rate of pollutants was measured to evaluate the piezoelectric catalytic efficiency of the material.

Claims

1. A method for ultra-fast preparation of metal-free piezoelectric catalytic materials in seconds and water treatment applications thereof, comprising the following steps: (1) Preparation of C3N5 piezoelectric catalytic materials 1) In a ball milling reactor, 3-amino-1,2,4-triazole and sodium hydroxide are subjected to ball milling reaction at 100-800 rpm for 1-8 hours; 2) drying the solid mixture obtained after ball milling in a vacuum oven at 50° C. to 100° C. for 4 to 12 hours; 3) loading the dried substance onto an iron sheet with a size of 2 cm to 5 cm × 2 cm to 5 cm × 0.1 mm to 0.5 mm, the surface of the iron sheet being covered with a piece of graphite paper with a thickness of 0.01 mm to 0.05 mm; 4) Place the iron sheet in the refractory bricks in the quartz tube and purge it with high-purity inert gas for 5 to 30 minutes; 5) placing the quartz tube in the refractory brick in a multi-turn induction coil with a diameter of 3 cm to 7 cm, and applying a controlled current for magnetic induction heating for 5 seconds to 30 seconds; 6) Allow the sample to cool naturally to room temperature to obtain the C3N5 piezoelectric catalytic material.

2. The method according to claim 1, wherein the ball milling time of the ball milling reactor is 2-6 hours.

3. The method according to claim 1, wherein the high purity inert gas is nitrogen.

4. A method for ultra-fast preparation of metal-free piezoelectric catalytic materials in seconds and its water treatment application, characterized in that The prepared piezoelectric catalyst material can be added to a water sample containing organic pollutants; 5. A method for preparing a metal-free piezoelectric catalytic material in seconds and its water treatment application, characterized in that The removal rate of pollutants was measured after ultrasonic treatment for 1-60 min or stirring for 0.1-6 h to evaluate the piezoelectric catalytic efficiency of the materials.

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