CN114507877A - Preparation method and application of photoelectrode film with graphite carbon nitride as substrate material - Google Patents
Preparation method and application of photoelectrode film with graphite carbon nitride as substrate material Download PDFInfo
- Publication number
- CN114507877A CN114507877A CN202210184203.5A CN202210184203A CN114507877A CN 114507877 A CN114507877 A CN 114507877A CN 202210184203 A CN202210184203 A CN 202210184203A CN 114507877 A CN114507877 A CN 114507877A
- Authority
- CN
- China
- Prior art keywords
- carbon nitride
- graphite carbon
- powder
- taking
- preparation
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Pending
Links
Images
Classifications
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B11/00—Electrodes; Manufacture thereof not otherwise provided for
- C25B11/04—Electrodes; Manufacture thereof not otherwise provided for characterised by the material
- C25B11/051—Electrodes formed of electrocatalysts on a substrate or carrier
- C25B11/073—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the electrocatalyst material
- C25B11/091—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the electrocatalyst material consisting of at least one catalytic element and at least one catalytic compound; consisting of two or more catalytic elements or catalytic compounds
- C25B11/095—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the electrocatalyst material consisting of at least one catalytic element and at least one catalytic compound; consisting of two or more catalytic elements or catalytic compounds at least one of the compounds being organic
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B1/00—Electrolytic production of inorganic compounds or non-metals
- C25B1/01—Products
- C25B1/02—Hydrogen or oxygen
- C25B1/04—Hydrogen or oxygen by electrolysis of water
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B1/00—Electrolytic production of inorganic compounds or non-metals
- C25B1/50—Processes
- C25B1/55—Photoelectrolysis
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B11/00—Electrodes; Manufacture thereof not otherwise provided for
- C25B11/04—Electrodes; Manufacture thereof not otherwise provided for characterised by the material
- C25B11/051—Electrodes formed of electrocatalysts on a substrate or carrier
- C25B11/052—Electrodes comprising one or more electrocatalytic coatings on a substrate
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
- Y02E60/36—Hydrogen production from non-carbon containing sources, e.g. by water electrolysis
Abstract
The invention relates to a preparation method and application of a photoelectrode film taking graphite carbon nitride as a substrate material, belonging to the technical field of photoelectrochemistry. Putting melamine into distilled water, heating on a stirrer until the solution is clear, adding terephthalaldehyde powder, stirring for a period of time, putting the mixture into an oven for drying to obtain a precursor, calcining the precursor at high temperature in a nitrogen environment to obtain a target product, grinding the target product into powder, and then taking a proper amount of powder to disperse the powder in the powder containing I2In acetone, ultrasonically vibrating to obtain electrophoretic deposition suspension, immersing two transparent conductive glasses with equal areas into the electrophoretic deposition suspension in a face-to-face parallel manner, and performing electrodeposition to prepare the photoelectric filmVery thin films. The photoelectrode film prepared by the method and taking the graphite carbon nitride as the substrate material can effectively separate electron hole pairs, reduce the recombination rate of the electron holes, further effectively improve the photoelectrochemical property and achieve the aim of efficiently decomposing water.
Description
Technical Field
The invention relates to a preparation method and application of a photoelectrode film taking graphite carbon nitride as a substrate material, belonging to the technical field of photoelectrochemistry.
Background
With the development of human society, the burning of fossil fuels poses a serious environmental problem. Photoelectrochemical cells that address environmental pollution and energy shortages have become the focus of attention. The photoelectrochemistry decomposition of water to produce hydrogen converts solar energy into storable chemical energy, which is a main means for solving the problems of environment and energy in the 21 st century. The graphitized carbon-nitrogen catalyst is a photocatalytic material with low price, rich resources and good stability, and is considered as a photocatalytic material with the prospects of pollution purification and energy conservation. However, unmodified graphitic carbon nitride has limited its practical application due to its relatively inefficient light absorption, low electron-hole separation efficiency and fewer active sites.
Disclosure of Invention
In order to solve the problems, the invention aims to provide a preparation method and application of a photoelectrode film taking graphite carbon nitride as a base material, and the method is easy to operate, simple, convenient, low in cost, mild in condition and beneficial to large-scale production.
The technical scheme adopted by the invention is as follows: a preparation method of a photoelectrode film taking graphite carbon nitride as a base material comprises the following steps:
1) adding melamine into distilled water, heating, magnetically stirring until the solution is clear, then adding terephthalaldehyde, continuously heating, magnetically stirring, and putting the obtained mixed solution into an oven for drying to obtain a precursor;
2) calcining the precursor obtained in the step 1) at high temperature in a nitrogen environment to obtain a target product;
3) grinding the target product obtained in the step 2) into powder, and takingDispersing the powder in acetone, adding I2Sealing and ultrasonically oscillating to obtain electrophoretic deposition suspension;
4) and (2) taking two pieces of transparent conductive glass (FTO) with equal area as positive and negative electrodes, immersing the two electrodes into the electrophoretic deposition suspension obtained in the step 3) in parallel in a face-to-face mode, applying a certain direct current voltage between the two electrodes, setting the deposition time, cutting off the current after the deposition is finished, taking the two electrodes out of the electrophoretic deposition suspension, and airing at room temperature to obtain the photoelectrode film taking graphite carbon nitride as a base material.
Further, in the preparation method, in the step 1), the weight ratio of terephthalaldehyde to melamine is 1-20: 300.
Further, in the above preparation method, step 1), the heating temperature is 100 ℃.
Further, in the preparation method, in the step 1), the drying temperature is 50-100 ℃.
Further, in the preparation method, step 2), the calcination temperature is 500-600 ℃, and the temperature rise rate is 5 ℃/min.
Further, in the preparation method, in the step 2), the calcination time is 4 hours.
Further, in the above production method, step 3), the amount of the powder added is 0.05 to 0.1 g.
Further, in the above preparation method, step 3), the acetone is 25 mL.
Further, in the preparation method, in the step 4), the direct current voltage is 25V, and the deposition time is 1-5 min.
The photoelectrode film prepared by the preparation method and taking the graphite carbon nitride as the base material is applied to photoelectrochemical water decomposition.
The invention has the beneficial effects that:
1. the photoelectrode film taking the graphite carbon nitride as the substrate material provided by the invention can more easily and effectively separate the photo-generated electron hole, reduce the recombination rate and effectively improve the photoelectrochemical property.
2. The photoelectrode thin film taking graphite carbon nitride as a base material provided by the invention has photocurrent density 4.85 times that of pure graphite carbon nitride under visible light.
3. The preparation method of the photoelectrode film with the graphite carbon nitride as the substrate material has the advantages of cheap and easily-obtained raw materials, simple and convenient operation, greatly reduced cost, provision of a new catalytic material for water decomposition, alleviation of the current situation of environmental energy shortage and good development prospect.
Drawings
FIG. 1 is a comparison graph of XRD of a photoelectrode thin film using graphite carbon nitride as a base material and a pure graphite carbon nitride photoelectrode thin film.
Fig. 2 is a graph comparing the photo-current of the photo-electrode film using graphite carbon nitride as the base material with the photo-electrode film of pure graphite carbon nitride.
FIG. 3 is a graph comparing the impedance spectra of a photo-electrode film with graphite carbon nitride as a substrate material and a pure graphite carbon nitride photo-electrode film.
In the figure, 1 represents a photoelectrode thin film using graphite carbon nitride as a base material, and 0 represents a pure graphite carbon nitride photoelectrode thin film.
Detailed Description
Example 1
Preparation of photoelectrode film with graphite carbon nitride as base material
1. Adding 3g of melamine into 200mL of distilled water, magnetically stirring at 100 ℃ until the solution is clear, then adding 0.13g of terephthalaldehyde powder, continuously stirring for 1.5h, putting the obtained mixed solution into a drying oven, and drying for 20h at 90 ℃ to obtain a precursor.
2. And grinding the obtained precursor, heating to 550 ℃ at the heating rate of 5 ℃/min in a nitrogen environment, and calcining for 4h to obtain the target product.
3. Grinding the target product into powder, placing 0.06g of the powder in 25mL of acetone solution, sealing and ultrasonically treating for 90min until the solution is uniformly dispersed, and adding 0.012g I into the uniform dispersion2And carrying out sealed ultrasonic oscillation for 30min to obtain electrophoretic deposition suspension.
4. Taking two pieces of transparent conductive glass (FTO) with equal area as positive and negative electrodes, immersing the two electrodes into the electrophoretic deposition suspension in parallel in a face-to-face manner, applying 25V direct current voltage between the two electrodes, and depositing for 5 min; and cutting off the current, taking the two electrodes out of the electrophoretic deposition suspension, and airing at room temperature to obtain the photoelectrode film taking the graphite carbon nitride as the base material. Comparative example (II): preparation of pure graphite carbon nitride optical electrode film
1. Adding 3g of melamine into 200mL of distilled water, magnetically stirring for 1.5h at 100 ℃, putting the obtained solution into an oven, and drying for 20h at 90 ℃ to obtain a precursor.
2. And grinding the obtained precursor, heating to 550 ℃ at the heating rate of 5 ℃/min in a nitrogen environment, and calcining for 4h to obtain the target product.
3. Grinding the target product into powder, placing 0.06g of the powder in 25mL of acetone solution, sealing and ultrasonically treating for 90min until the solution is uniformly dispersed, and adding 0.012g I into the uniform dispersion2And carrying out sealed ultrasonic oscillation for 30min to obtain the electrophoretic deposition suspension.
4. Taking two pieces of transparent conductive glass (FTO) with equal area as positive and negative electrodes, immersing the two electrodes into the electrophoretic deposition suspension in parallel in a face-to-face manner, applying 25V direct current voltage between the two electrodes, and depositing for 5 min; and cutting off the current, taking the two electrodes out of the electrophoretic deposition suspension, and airing at room temperature to obtain the pure graphite carbon nitride photoelectrode film.
(III) detection
Fig. 1 is an XRD test chart of the photoelectrode thin film using graphite carbon nitride as a base material and a pure graphite carbon nitride photoelectrode thin film in a powder form, and it can be seen from fig. 1 that the graphite carbon nitride as a base material has two diffraction peaks at 13.1 ° and 27.6 °, which coincide with the diffraction peaks of pure graphite carbon nitride, but compared with pure graphite carbon nitride, the material treated with terephthalaldehyde has a reduced XRD diffraction peak intensity and a reduced crystallinity of the sample.
Example 2 application of photoelectrode thin film using graphite carbon nitride as substrate material in photoelectrochemical water splitting
The photoelectrode thin film prepared in example 1 and using graphite carbon nitride as a base material and the pure graphite carbon nitride photoelectrode thin film were subjected to photoelectrochemical property tests of photocurrent and impedance.
All electrochemical experimental test procedures were performed in an electrochemical workstation (Princeton Applied Research2273) of a three-electrode system. The photoelectrode film or pure graphite carbon nitride photoelectrode film taking graphite carbon nitride as a substrate material is taken as a working electrode, a platinum sheet is taken as a counter electrode, Ag/AgCl is taken as a reference electrode, electrolyte is 0.5M sodium sulfate, and the light irradiation area of a sample is 1cm2。
And (3) testing photocurrent: the light source is a 300W xenon lamp, the bias voltage is 1.23V vs. RHE, and the test result is shown in figure 2, and the result shows that the photocurrent density of the photoelectrode thin film taking graphite carbon nitride as the base material is higher than that of a pure graphite carbon nitride photoelectrode thin film, which indicates that the photoelectrochemical property of a sample treated by taking graphite carbon nitride as the base material is improved.
Electrochemical Impedance Spectroscopy (EIS) testing: voc is 0V vs. Voc, the frequency range is 0.1-105Hz, the test result is shown in figure 3, the impedance of the photoelectrode thin film sample treated by taking the graphite carbon nitride as the base material is relatively small, and the photocurrent is maximum, which is consistent with figure 3.
Claims (10)
1. A preparation method of a photoelectrode film taking graphite carbon nitride as a substrate material is characterized by comprising the following steps:
1) adding melamine into distilled water, heating, magnetically stirring until the solution is clear, then adding terephthalaldehyde, continuously heating, magnetically stirring, and putting the obtained mixed solution into an oven for drying to obtain a precursor;
2) calcining the precursor obtained in the step 1) at high temperature in a nitrogen environment to obtain a target product;
3) grinding the target product obtained in the step 2) into powder, taking a proper amount of powder to disperse in acetone, and then adding I2Sealing and ultrasonically oscillating to obtain electrophoretic deposition suspension;
4) and (2) taking two pieces of transparent conductive glass (FTO) with equal area as positive and negative electrodes, immersing the two electrodes into the electrophoretic deposition suspension obtained in the step 3) in parallel in a face-to-face mode, applying a certain direct current voltage between the two electrodes, setting the deposition time, cutting off the current after the deposition is finished, taking the two electrodes out of the electrophoretic deposition suspension, and airing at room temperature to obtain the photoelectrode film taking graphite carbon nitride as a base material.
2. The preparation method according to claim 1, wherein in the step 1), the mass ratio of terephthalaldehyde to melamine is 1-20: 300.
3. The method according to claim 1, wherein the heating temperature in step 1) is 100 ℃.
4. The method according to claim 1, wherein the drying temperature in step 1) is 50 to 100 ℃.
5. The preparation method as claimed in claim 1, wherein in step 2), the calcination temperature is 500-600 ℃ and the temperature rise rate is 5 ℃/min.
6. The method according to claim 1, wherein the calcination time in step 2) is 4 hours.
7. The production method according to claim 1, wherein the powder is added in an amount of 0.05 to 0.1g in step 3).
8. The method according to claim 1, wherein the acetone is 25mL in the step 3).
9. The method according to claim 1, wherein in the step 4), the DC voltage is 25V, and the deposition time is 1-5 min.
10. The use of the photoelectrode thin film prepared by the preparation method according to any one of claims 1 to 9 and using graphite carbon nitride as a base material in photoelectrochemical water splitting.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN202210184203.5A CN114507877A (en) | 2022-02-23 | 2022-02-23 | Preparation method and application of photoelectrode film with graphite carbon nitride as substrate material |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN202210184203.5A CN114507877A (en) | 2022-02-23 | 2022-02-23 | Preparation method and application of photoelectrode film with graphite carbon nitride as substrate material |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| CN114507877A true CN114507877A (en) | 2022-05-17 |
Family
ID=81554037
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CN202210184203.5A Pending CN114507877A (en) | 2022-02-23 | 2022-02-23 | Preparation method and application of photoelectrode film with graphite carbon nitride as substrate material |
Country Status (1)
| Country | Link |
|---|---|
| CN (1) | CN114507877A (en) |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2024078562A1 (en) * | 2022-10-14 | 2024-04-18 | Tcl科技集团股份有限公司 | Film and preparation method therefor, and photoelectric device |
Citations (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN105195192A (en) * | 2015-07-29 | 2015-12-30 | 阜阳师范学院 | Composite photocatalyst CN-CNI as well as preparation method and application thereof |
| CN105435825A (en) * | 2015-07-06 | 2016-03-30 | 阜阳师范学院 | Composite photocatalyst SiO2/CNI, preparation method therefor and application in field of hydrogen production by water photolysis |
| CN107177859A (en) * | 2017-05-18 | 2017-09-19 | 辽宁大学 | Pb3Nb4O13The preparation method of light anode material |
| CN113198509A (en) * | 2021-05-06 | 2021-08-03 | 辽宁大学 | g-C based on terephthalaldehyde treatment3N4Photocatalytic material and preparation method and application thereof |
| FR3108628A1 (en) * | 2020-03-31 | 2021-10-01 | Imra Europe Sas | Thin film of graphitic carbon nitride, method of manufacture and use as a photoelectrode |
-
2022
- 2022-02-23 CN CN202210184203.5A patent/CN114507877A/en active Pending
Patent Citations (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN105435825A (en) * | 2015-07-06 | 2016-03-30 | 阜阳师范学院 | Composite photocatalyst SiO2/CNI, preparation method therefor and application in field of hydrogen production by water photolysis |
| CN105195192A (en) * | 2015-07-29 | 2015-12-30 | 阜阳师范学院 | Composite photocatalyst CN-CNI as well as preparation method and application thereof |
| CN107177859A (en) * | 2017-05-18 | 2017-09-19 | 辽宁大学 | Pb3Nb4O13The preparation method of light anode material |
| FR3108628A1 (en) * | 2020-03-31 | 2021-10-01 | Imra Europe Sas | Thin film of graphitic carbon nitride, method of manufacture and use as a photoelectrode |
| CN113198509A (en) * | 2021-05-06 | 2021-08-03 | 辽宁大学 | g-C based on terephthalaldehyde treatment3N4Photocatalytic material and preparation method and application thereof |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2024078562A1 (en) * | 2022-10-14 | 2024-04-18 | Tcl科技集团股份有限公司 | Film and preparation method therefor, and photoelectric device |
Similar Documents
| Publication | Publication Date | Title |
|---|---|---|
| CN110565111B (en) | Hexagonal column type WO3/Bi2WO6Preparation method of composite photoelectrode film | |
| CN107994120B (en) | Sn2Nb2O7Photoanode material and Sn2Nb2O7Photoelectrode film | |
| CN114261956B (en) | Photoanode water-splitting electrolyte solution based on amino acid carbon dots | |
| CN108821257A (en) | A kind of binary based on lotus leaf is mesoporous-micropore multilevel structure biological carbon and its preparation method and application | |
| CN110004459B (en) | Heterojunction photo-anode for driving carbon dioxide reduction and preparation method and application thereof | |
| CN103132120A (en) | Method for preparing photoelectrocatalysis electrode material capable of efficiently degrading organic pollutants | |
| CN109626422A (en) | A kind of TiO2/g-C3N4The preparation method and applications of light anode nanocomposite | |
| CN107675200A (en) | A kind of modified g C3N4Quantum dot/TiO2Nano wire light anode and its application | |
| CN114507877A (en) | Preparation method and application of photoelectrode film with graphite carbon nitride as substrate material | |
| CN113089020B (en) | Co(OH) 2 /FePO 4 Photoelectrode thin film and application thereof in photoelectrochemical water decomposition | |
| CN109821559A (en) | A kind of preparation method and applications of core-shell structure composite photoelectric material | |
| CN111298809A (en) | ZnIn rich in surface S vacancies2S4Preparation method of nanosheet array | |
| CN1900366A (en) | Ion diaphragm photoelectrolytic cell using solar energy directly decomposing water to make hydrogen | |
| CN110965074A (en) | Method for preparing composite film photoelectrode | |
| CN114592212A (en) | Heterojunction MoO3Preparation method and application of/ZnO photoelectrode film | |
| CN111778518B (en) | High-performance P: Fe 2 O 3 /FeOOH composite photoelectrode and preparation method and application thereof | |
| Long et al. | Glucose-derived porous carbon as a highly efficient and low-cost counter electrode for quantum dot-sensitized solar cells | |
| CN114369942A (en) | Carbon fiber/titanium dioxide photoelectric composite material and preparation method and application thereof | |
| Kodtharin et al. | Structures and properties of N-doped TiO2 nanotubes arrays synthesized by the anodization method for hydrogen production | |
| CN114737217B (en) | Bi (Bi) 2 MoO 6 CuO photoelectrode film, preparation method thereof and application thereof in photoelectrochemical water decomposition | |
| CN112675859A (en) | Foam nickel-based titanium dioxide nano composite material and preparation method and application thereof | |
| CN110639582A (en) | g-C with 2D/0D structure3N4/WO3Preparation method of composite photocatalyst | |
| CN111054420B (en) | Method for synthesizing composite photoelectric catalyst by using dielectric barrier discharge plasma in one step, product and application thereof | |
| CN113913848B (en) | Electricity-generating hydrogen production device based on cadmium sulfide/aluminum photocatalytic material | |
| CN109750313B (en) | Calcium bismuthate/tungsten oxide composite photoelectrode, preparation method and application thereof in photoelectrocatalysis decomposition of water |
Legal Events
| Date | Code | Title | Description |
|---|---|---|---|
| PB01 | Publication | ||
| PB01 | Publication | ||
| SE01 | Entry into force of request for substantive examination | ||
| SE01 | Entry into force of request for substantive examination |