阅读说明：本技术 一种片状高催化活性g-C3N4粉体的制备方法 (Flaky high-catalytic-activity g-C3N4Method for preparing powder ) 是由 杨志韬 郭家乐 张宇峰 任彤 梁子寒 刘刚 于 2020-11-30 设计创作，主要内容包括：一种片状高催化活性g-C_3N_4粉体的制备方法,它涉及一种电化学沉积方法制作g-C_3N_4的方法。本方法如下：一、准备好三聚氰胺、乙腈和铂片,以及电桥实验装置；二、称取一定量的三聚氰胺加入乙腈中,利用磁力搅拌器搅拌到澄清,然后将溶液放入电桥实验装置,电桥装置放入超声振荡器的水池中；三、取适当面积的铂片两份,用无水乙醇和丙酮反复清洗若干次；四、两个铂片接通电源的两极后,将超声振荡器打开,开启震动模式；五、打开电源,电压调节到一定值；六、通电一定时间；七、待步骤六的断电之后,再继续使用超声震荡器震荡10分钟,将溶液过滤,得滤渣,即得产物。本发明制备g-C_3N_4粉体微观上呈片状,不仅光催化效果好,而且是在室温条件下进行,具有成本低、制备工艺绿色环保等优点。(Flaky high-catalytic-activity g-C 3 N 4 A method for preparing powder, which relates to a method for preparing g-C by electrochemical deposition 3 N 4 The method of (1). The method comprises the following steps: firstly, preparing melamine, acetonitrile and platinum sheets, and a bridge experiment device; weighing a certain amount of melamine, adding the melamine into acetonitrile, stirring the mixture by using a magnetic stirrer until the mixture is clear, then putting the solution into an electric bridge experimental device, and putting the electric bridge experimental device into ultrasonic vibrationIn the pool of the oscillator; thirdly, taking two parts of platinum sheets with proper areas, and repeatedly cleaning the two parts of platinum sheets with absolute ethyl alcohol and acetone for a plurality of times; after the two platinum sheets are connected with two poles of a power supply, the ultrasonic oscillator is turned on, and a vibration mode is started; fifthly, turning on a power supply, and adjusting the voltage to a certain value; sixthly, electrifying for a certain time; and seventhly, after the power is cut off in the step six, continuing to vibrate for 10 minutes by using the ultrasonic vibrator, and filtering the solution to obtain filter residues, namely obtaining the product. Preparation of g-C according to the invention 3 N 4 The powder is microscopically flaky, has good photocatalytic effect, is carried out at room temperature, and has the advantages of low cost, green and environment-friendly preparation process and the like.)

1. Flaky high-catalytic-activity g-C₃N₄The preparation method of the powder is characterized in that the preparation method is a g-C₃N₄The preparation method of the powder comprises the following steps:

preparing melamine, acetonitrile, a platinum sheet and an electric bridge experimental device, wherein the distance between a positive electrode and a negative electrode in the electric bridge experimental device is 0.1-50 cm;

weighing a certain amount of melamine and adding the melamine into acetonitrile, wherein the mass ratio of the melamine to the acetonitrile is 10: 1-10000, stirring the melamine to be clear by using a magnetic stirrer, and then putting the solution into an electric bridge experimental device which is put into a water tank of an ultrasonic oscillator;

thirdly, taking two parts of platinum sheets with proper areas, and repeatedly cleaning the two parts of platinum sheets with absolute ethyl alcohol and acetone for a plurality of times;

after the two platinum sheets are connected with two poles of a power supply, the ultrasonic oscillator is turned on, and the vibration mode is started, wherein the frequency of ultrasonic waves is 20 kHz-100 MHz;

fifthly, turning on a power supply, and adjusting the voltage to 500-10000V;

sixthly, electrifying for a certain time of 0.1-10000 h;

and seventhly, after the power is cut off in the step six, continuing to vibrate for 1-30 min by using an ultrasonic vibrator, and filtering the solution to obtain filter residues, namely obtaining the product.

2. The flaky high catalytic activity g-C as claimed in claim 1₃N₄The preparation method of the powder is characterized in that in the first step, the distance between a positive electrode and a negative electrode in the bridge device is 1-40 cm.

3. The flaky high catalytic activity g-C as claimed in claim 1₃N₄The preparation method of the powder is characterized in that the mass ratio of the melamine to the acetonitrile in the step two is 10: 1-10000.

4. The flaky high catalytic activity g-C as claimed in claim 1₃N₄The preparation method of the powder is characterized in that in the third step, thePlatinum sheets were used as electrodes.

5. The flaky high catalytic activity g-C as claimed in claim 1₃N₄The preparation method of the powder is characterized in that in the fourth step, the frequency of the ultrasonic wave is 20 kHz-100 MHz.

6. The flaky high catalytic activity g-C as claimed in claim 1₃N₄The preparation method of the powder is characterized in that in the fifth step, the voltage value is 500-10000V.

Technical Field

The invention relates to a method for preparing flaky g-C by electrochemical deposition₃N₄A method for preparing powder.

Background

Graphite phase carbon nitride (g-C)₃N₄) Has unique electronic structure and excellent chemical stability, is used as a catalyst and a catalyst carrier without metals in recent years, is widely used for the selective conversion of organic functional groups, the photocatalytic decomposition of water, the reduction of oxygen and the loading of noble metals such as Au, Pd, Ag, Pt and the like, and is also used as a green energy storage material and a hard template agent for H₂、CO₂The stored nano metal nitrogen oxide is more and more concerned in the related fields of energy, materials and the like. However, how to manufacture in large quantities and make better use of the product, and how to use the product more conveniently, is a constant subject. Therefore, how to develop and conveniently utilize g-C by increasing which substances make it exert more effect₃N₄Photocatalysis, oxygen reduction, organic selective synthesis and the like, and further develops g-C₃N₄The method has great significance in the application of energy and environment fields.

Graphite phase carbon nitride (g-C)₃N₄) Is a typical polymer semiconductor, and CN atoms in the structure form a highly delocalized pi conjugated system through sp2 hybridization. Wherein the Npz orbital component is g-C₃N₄The Highest Occupied Molecular Orbital (HOMO) and the Cpz orbital form the Lowest Unoccupied Molecular Orbital (LUMO), the forbidden bandwidth is 2.7eV, and the blue-violet light with the wavelength less than 475nm in the solar spectrum can be absorbed. It can meet the thermodynamic requirement of photolysis of water to produce hydrogen and oxygen. In recent yearsIt is found to have good photocatalytic property, not only used as a good catalyst carrier of a catalyst without metal components and widely applied to selective conversion of organic functional groups, photocatalytic water decomposition, oxygen reduction and loading of precious metals such as Au, Pd, Ag, Pt and the like, but also used as a green energy storage material and a hard template agent for H₂、CO₂Storage and preparation of nano metal nitrogen (oxide), etc. In addition, with conventional TiO₂Photocatalyst phase ratio, g-C₃N₄Can effectively activate molecular oxygen and generate superoxide radical for the photocatalytic conversion of organic functional groups and the photocatalytic degradation of organic pollutants.

Disclosure of Invention

The invention aims to improve the existing g-C₃N₄The photocatalytic performance is improved, the cost is reduced, and an electrochemical method for preparing g-C is provided₃N₄A method for preparing powder.

Flaky high-catalytic-activity g-C₃N₄The preparation method of the powder comprises the following steps:

preparing melamine, acetonitrile, a platinum sheet and an electric bridge experimental device, wherein the distance between a positive electrode and a negative electrode in the electric bridge experimental device is 0.1-50 cm;

weighing a certain amount of melamine and adding the melamine into acetonitrile, wherein the mass ratio of the melamine to the acetonitrile is 10: 1-10000, stirring the melamine to be clear by using a magnetic stirrer, and then putting the solution into an electric bridge experimental device which is put into a water tank of an ultrasonic oscillator;

thirdly, taking the area of 1-1000 cm²Repeatedly washing the two parts of platinum sheets with absolute ethyl alcohol and acetone for 5-8 times;

after the two platinum sheets are connected with two poles of a power supply, the ultrasonic oscillator is turned on, and the vibration mode is started, wherein the frequency of ultrasonic waves is 20 kHz-100 MHz;

fifthly, turning on a power supply, and adjusting the voltage to 500-10000V;

sixthly, electrifying for a certain time of 0.1-10000 h;

and seventhly, after the power is cut off in the step six, continuing to vibrate for 1-30 min by using an ultrasonic vibrator, and filtering the solution to obtain filter residues, namely obtaining the product.

Drawings

FIG. 1 experiment I graphite phase carbon nitride g-C prepared by electrochemical method₃N₄TEM photograph of (a).

FIG. 2 experiment I graphite phase carbon nitride g-C prepared by electrochemical method₃N₄XRD pattern of (a).

Detailed Description

The technical solution of the present invention is not limited to the following specific embodiments, but includes any combination of the specific embodiments.

The first embodiment is as follows: this embodiment is a flaky high catalytic activity g-C₃N₄The preparation method of the powder comprises the following steps:

preparing melamine, acetonitrile, a platinum sheet and an electric bridge experimental device, wherein the distance between a positive electrode and a negative electrode in the electric bridge experimental device is 0.1-50 cm;

weighing a certain amount of melamine and adding the melamine into acetonitrile, wherein the mass ratio of the melamine to the acetonitrile is 10: 1-10000, stirring the melamine to be clear by using a magnetic stirrer, and then putting the solution into an electric bridge experimental device which is put into a water tank of an ultrasonic oscillator;

thirdly, taking the area of 1-1000 cm²Repeatedly washing the two parts of platinum sheets with absolute ethyl alcohol and acetone for 5-8 times;

after the two platinum sheets are connected with two poles of a power supply, the ultrasonic oscillator is turned on, and the vibration mode is started, wherein the frequency of ultrasonic waves is 20 kHz-100 MHz;

fifthly, turning on a power supply, and adjusting the voltage to 500-10000V;

sixthly, electrifying for a certain time of 0.1-10000 h;

and seventhly, after the power is cut off in the step six, continuing to vibrate for 1-30 min by using an ultrasonic vibrator, and filtering the solution to obtain filter residues, namely obtaining the product.

The second embodiment is as follows: the difference between the first embodiment and the second embodiment is that in the first step, the distance between the positive electrode and the negative electrode in the bridge device is 1-40 cm. The rest is the same as the first embodiment.

The third concrete implementation mode: the second embodiment is different from the first or second embodiment in that the mass ratio of melamine to acetonitrile is 1:2 to 8000. The other is the same as in one or both of the first and second embodiments.

The fourth concrete implementation mode: the difference between this embodiment and the first to third embodiments is that in the third step, the area is 2-100 cm²The two parts of the platinum sheet are repeatedly washed for 5-7 times by absolute ethyl alcohol and acetone. The others are the same as in one of the first to third embodiments.

The fifth concrete implementation mode: the difference between this embodiment and one of the first to fourth embodiments is that in step four, after the two platinum sheets are connected to the two poles of the power supply, the frequency of the ultrasonic wave is 40kHz to 80 MHz. The other is the same as one of the first to fourth embodiments.

The sixth specific implementation mode: the difference between the present embodiment and one of the first to fifth embodiments is that in the fifth step, the power is turned on, and the voltage is adjusted to 600-9000V. The other is the same as one of the first to fifth embodiments.

The seventh embodiment: the difference between the present embodiment and one of the first to sixth embodiments is that in the fifth step, the power is turned on and the voltage is adjusted to 800-5000V. The other is the same as one of the first to sixth embodiments.

The specific implementation mode is eight: the difference between this embodiment and the first to seventh embodiments is that in the sixth step, the power is applied for a certain time of 1-400 hours. The other is the same as one of the first to seventh embodiments.

The specific implementation method nine: the difference between the present embodiment and one of the first to seventh embodiments is that in the seventh step, after the power failure of the sixth step, the ultrasonic oscillator is continued to oscillate for 5-30 min. The rest is the same as the first to eighth embodiments.

The following experiments were used to verify the effect of the present invention.

Experiment one:

flaky high-catalytic-activity g-C₃N₄The preparation method of the powder comprises the following steps:

preparing melamine, acetonitrile, a platinum sheet and an electric bridge experimental device, wherein the distance between a positive electrode and a negative electrode in the electric bridge experimental device is 10 cm;

weighing a certain amount of melamine and adding the melamine into acetonitrile, wherein the mass ratio of the melamine to the acetonitrile is 1:50, stirring the melamine to be clear by using a magnetic stirrer, and then putting the solution into an electric bridge experimental device which is put into a water tank of an ultrasonic oscillator;

thirdly, taking two parts of platinum sheets with proper areas, and repeatedly cleaning the two parts of platinum sheets for 6 times by using absolute ethyl alcohol and acetone;

after the two platinum sheets are connected with two poles of a power supply, the ultrasonic oscillator is turned on, and the vibration mode is started, wherein the frequency of ultrasonic waves is 50 MHz;

fifthly, turning on a power supply, and regulating the voltage to 1000V;

sixthly, electrifying for a certain time of 12 hours;

and seventhly, after the power is cut off in the step six, continuing to vibrate for 30min by using an ultrasonic vibrator, and filtering the solution to obtain filter residues, namely obtaining the product.

Experiment two:

flaky high-catalytic-activity g-C₃N₄The preparation method of the powder comprises the following steps:

preparing melamine, acetonitrile, a platinum sheet and an electric bridge experimental device, wherein the distance between a positive electrode and a negative electrode in the electric bridge experimental device is 5 cm;

weighing a certain amount of melamine and adding the melamine into acetonitrile, wherein the mass ratio of the melamine to the acetonitrile is 1:10, stirring the melamine to be clear by using a magnetic stirrer, and then putting the solution into an electric bridge experimental device which is put into a water tank of an ultrasonic oscillator;

thirdly, taking two parts of platinum sheets with proper areas, and repeatedly cleaning the two parts of platinum sheets for 5 times by using absolute ethyl alcohol and acetone;

after two platinum sheets are connected with two poles of a power supply, an ultrasonic oscillator is turned on, and a vibration mode is started, wherein the frequency of ultrasonic waves is 10 MHz;

fifthly, turning on a power supply, and regulating the voltage to 800V;

sixthly, electrifying for a certain time of 24 hours;

and seventhly, after the power is cut off in the step six, continuing to vibrate for 15min by using an ultrasonic vibrator, and filtering the solution to obtain filter residues, namely obtaining the product.