CN116031415A - Preparation method of nitrogen-doped graphene loaded iron monoatomic catalyst - Google Patents
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Abstract
The invention discloses a preparation method of a nitrogen-doped graphene-loaded iron monoatomic catalyst, which comprises the following steps of selecting carbon nitride, tannic acid, an iron source, 4-diethylamino-salicylaldehyde, an ethanol solution and deionized water; dispersing carbon nitride in deionized water by ultrasonic waves; adding an iron source into deionized water containing tannic acid; adding 4-diethylamino-salicylaldehyde to an ethanol solution; mixing the first solution, the second solution and the third solution, and stirring to obtain a uniformly dispersed solution; carrying out hydrothermal treatment on the uniformly dispersed solution by a hydrothermal kettle; centrifuging and drying the hydrothermal solution to obtain a Fe/C3N4@TA-salicylaldehyde precursor; and calcining the Fe/C3N4@TA-salicylaldehyde precursor at a high temperature in a nitrogen atmosphere to obtain the nitrogen-doped graphene loaded iron monoatomic catalyst. According to the invention, the N-doped graphene loaded iron single-atom catalyst prepared by modifying C3N4 with tannic acid shows excellent ORR activity, and has a good oxygen reduction catalytic effect and a good application prospect.
Description
Technical Field
The invention relates to the technical field of nano materials, in particular to a preparation method of a nitrogen-doped graphene-supported iron monoatomic catalyst.
Background
The growing global energy demand and environmental concerns require more advanced energy conversion and storage devices and technologies. Renewable energy conversion and storage systems have been widely explored to alleviate energy crisis and environmental issues. Fuel cells and metal-air cells are considered promising candidates due to their high theoretical energy density, high energy efficiency and zero carbon emissions. However, the slow kinetics of designing high performance electrocatalysts to accelerate the four-electron Oxygen Reduction Reaction (ORR) remains one of the key challenges for large-scale commercialization of these technologies.
In recent decades, carbon-based materials have received attention due to their good electrocatalytic activity, low price, stable performance, environmental friendliness, and the like. However, the electrocatalytic activity of carbon-based materials is far lower than that of noble metal-based materials, which limits their use in practical energy devices. Based on this, a great deal of research effort is put into the improvement of the electrocatalytic activity of carbon-based materials. The doping of hetero atoms in the carbon skeleton can effectively change electron distribution, increase electrochemical active sites and further increase the electrocatalytic activity of the carbon-based material; in addition, the morphology and crystal form characteristics of the carbon-based material are reasonably controlled, and the electron and substance transmission channels are increased, so that the electrocatalytic activity can be improved.
Cathodic oxygen reduction (ORR) is a slow kinetic process, and currently commercially available in PEMFCs, the cathodic oxygen reduction catalyst is Pt/C or PtRu/C. Platinum reserves are scarce and expensive, and it has been found from investigation that platinum costs about 56% of the total fuel cell device. In addition, the platinum-based catalyst has poor stability, and the platinum nano particles can be dissolved and partially agglomerated in a high-temperature and high-humidity corrosive environment, so that the reduction of active sites and the reduction of specific surface area are caused, and the reduction of oxygen reduction activity is reduced; meanwhile, the platinum-based catalyst is poisoned by carbon monoxide (CO), and researches show that even a small amount of CO (10-20 ppm) can cause the activity of the platinum-based catalyst to be greatly reduced, so that the ORR performance of the catalytic material is poor. These problems have prevented the large-scale application of proton exchange membrane fuel cells.
Disclosure of Invention
In order to solve the technical problem that the ORR performance of the existing catalytic material is poor. The invention provides a preparation method of a nitrogen-doped graphene-supported iron monoatomic catalyst.
The invention is realized by the following technical scheme:
the preparation method of the nitrogen-doped graphene-supported iron monoatomic catalyst comprises the following steps of:
s1, selecting carbon nitride as a nitrogen source, tannic acid as a carbon source, ferric acetylacetonate or ferric phthalocyanine as an iron source, 4-diethylamino-salicylaldehyde, ethanol solution and deionized water;
s2, dispersing carbon nitride in deionized water through ultrasonic waves to obtain a uniformly dispersed solution I; adding an iron source into deionized water containing tannic acid, and mixing and stirring to obtain a uniform solution II; adding 4-diethylamino-salicylaldehyde into an ethanol solution, and mixing and stirring to obtain a uniform solution III;
s3, mixing the first solution, the second solution and the third solution, and stirring to obtain a uniformly dispersed solution;
s4, carrying out hydrothermal treatment on the uniformly dispersed solution in the step S2 through a hydrothermal kettle;
s5, centrifugally drying the uniformly dispersed solution after the hydrothermal reaction to obtain a Fe/C3N4@TA-salicylaldehyde precursor;
and S6, calcining the Fe/C3N4@TA-salicylaldehyde precursor at a high temperature in a nitrogen atmosphere to obtain the nitrogen-doped graphene loaded iron monoatomic catalyst.
Further, the following tannic acid, carbon nitride, iron source, 4-diethylamino-salicylaldehyde, deionized water and ethanol are used in the S1: 0.8-0.9g of tannic acid; 480-500mg of carbon nitride; 19-21mg of iron source; 0.5-0.7g of 4-diethylamino-salicylaldehyde; 58-60mL of deionized water; ethanol 24-26mL.
Further, the following tannic acid, carbon nitride, iron source, 4-diethylamino-salicylaldehyde, deionized water and ethanol are used in the S1: 0.8506g of tannic acid; 500mg of carbon nitride; 20mg of iron source; 0.6g of 4-diethylamino-salicylaldehyde; 60mL of deionized water; ethanol 25mL.
Further, the following tannic acid, carbon nitride, iron source, 4-diethylamino-salicylaldehyde, deionized water and ethanol are used in the S1: tannic acid 0.8g; 480mg of carbon nitride; 19mg of iron source; 0.5g of 4-diethylamino-salicylaldehyde; 58mL of deionized water; ethanol 24mL.
Further, the following tannic acid, carbon nitride, iron source, 4-diethylamino-salicylaldehyde, deionized water and ethanol are used in the S1: tannic acid 0.9g; 490mg of carbon nitride; 21mg of iron source; 0.7g of 4-diethylamino-salicylaldehyde; 59mL of deionized water; ethanol 26mL.
Further, the dispersion time of the ultrasonic wave in S2 is 60min, the temperature is normal temperature, the stirring time of mixing and stirring is 60min, and the temperature is normal temperature.
Further, the hydrothermal temperature in S4 is 120 ℃ and the time is 10 hours.
Further, the temperature of the centrifugal drying in S5 was 60 ℃.
Further, the high-temperature calcination temperature in S6 is 900 ℃ and the time is 2 hours.
The invention has the advantages and positive effects that: according to the method, the nitrogen-doped graphene loaded iron single-atom catalyst (Fe/NG) is obtained through mixing and stirring, hydrothermal treatment, centrifugal drying and calcination, and the obtained material has a two-dimensional nano-sheet structure, has obvious porous characteristics and is beneficial to electrolyte diffusion. No template is needed in the preparation process, no toxic or harmful gas is released, raw materials are easy to obtain, the cost is low, and the synthesis is easy.
When the catalyst is used as an ORR electrocatalyst in alkaline electrolyte (0.1M potassium hydroxide), the catalyst prepared by the product has better catalytic activity, and when the limiting current density is 5.5mA cm < -2 >, the half-wave potential of the ORR reaction is 0.91V, and the nitrogen-doped graphene loaded iron monoatomic catalyst prepared by modifying C3N4 with tannic acid shows excellent ORR activity, and has better oxygen reduction catalytic effect and better application prospect.
Drawings
FIG. 1 is a TEM image of a nitrogen-doped graphene-supported iron single-atom catalyst (Fe/NG) prepared in example 1 of the present invention;
FIG. 2 (a) is a graph showing polarization of Fe/NG obtained after calcination of the Fe/C3N4@TA-salicylaldehyde precursor prepared in example 1 and Fe/C3N4@TA prepared in comparative examples 1-3 (comparative example 1), fe/C3N4@salicylaldehyde (comparative example 2) and Fe/C3N4 (comparative example 3);
FIG. 2 (b) is a half-wave potential bar graph of Fe/NG obtained by calcining the Fe/C3N4@TA-salicylaldehyde precursor prepared in example 1 and Fe/C3N4@TA prepared in comparative examples 1-3 (comparative example 1), fe/C3N4@salicylaldehyde (comparative example 2) and Fe/C3N4 (comparative example 3).
Detailed Description
The following description of the embodiments of the present invention will be made clearly and fully with reference to the accompanying drawings, in which it is evident that the embodiments described are only some, but not all embodiments of the invention. The following description of at least one exemplary embodiment is merely exemplary in nature and is in no way intended to limit the invention, its application, or uses. All other embodiments, which can be made by those skilled in the art based on the embodiments of the invention without making any inventive effort, are intended to be within the scope of the invention.
The numerical values set forth in these examples do not limit the scope of the present invention unless specifically stated otherwise. Techniques, methods known to those of ordinary skill in the relevant art may not be discussed in detail, but should be considered part of the specification where appropriate. In all examples shown and discussed herein, any specific values should be construed as merely illustrative, and not a limitation. Thus, other examples of the exemplary embodiments may have different values.
The experimental methods in the following examples, for which specific conditions are not noted, are generally determined according to national standards; if the national standard is not corresponding, the method is carried out according to the general international standard or the standard requirements set by related enterprises. Unless otherwise indicated, all parts are parts by weight and all percentages are percentages by weight.
Example 1
The preparation method of the nitrogen-doped graphene-supported iron monoatomic catalyst comprises the following steps of:
step one, selecting carbon nitride (C 3 N 4 ) As nitrogen source, tannic acid as carbon source, ferric acetylacetonate as iron source, 4-diethylamino-salicylaldehyde, ethanol solution and deionized water, wherein the dosage of tannic acid, carbon nitride, ferric acetylacetonate, 4-diethylamino-salicylaldehyde, deionized water and ethanol is as follows: 0.8506g of tannic acid; 500mg of carbon nitride; 20mg of ferric acetylacetonate; 0.6g of 4-diethylamino-salicylaldehyde; 60mL of deionized water; ethanol 25mL.
Adding 500mg of carbon nitride into 40mL of deionized water, and dispersing for 60min at normal temperature by ultrasonic waves to obtain a uniformly dispersed solution I; 20mg of ferric acetylacetonate is added into 40mL of deionized water containing 0.8506g of tannic acid, and the mixture is mixed and stirred for 60min at normal temperature (25 ℃) to obtain a uniform solution II; adding 0.6g of 4-diethylamino-salicylaldehyde into 25mL of ethanol solution, and mixing and stirring for 60min at normal temperature to obtain a uniform solution III;
step three, mixing the solution I, the solution II and the solution III, and stirring to obtain a uniformly dispersed solution;
fourthly, carrying out hydrothermal treatment on the uniformly dispersed solution in the third step through a hydrothermal kettle, wherein the hydrothermal temperature is 120 ℃ and the time is 10 hours;
centrifuging and drying the uniformly dispersed solution after the hydrothermal treatment for two times, and putting the precipitate into a drying oven to be dried at 60 ℃ to obtain a Fe/C3N4@TA-salicylaldehyde precursor;
and step six, calcining the Fe/C3N4@TA-salicylaldehyde precursor at a high temperature in a nitrogen atmosphere to obtain the nitrogen-doped graphene loaded iron monoatomic catalyst. Wherein the high-temperature calcination temperature is 900 ℃ and the time is 2h.
Fig. 1 is a TEM image of the nitrogen doped graphene supported iron single atom catalyst (Fe/NG) prepared in example 1, from which it can be seen that the material is changed to a two-dimensional nano-sheet structure, and no metal nano-particles are apparent.
Example two
The preparation method of the nitrogen-doped graphene-supported iron monoatomic catalyst comprises the following steps of:
firstly, selecting carbon nitride as a nitrogen source, tannic acid as a carbon source, iron phthalocyanine as an iron source, 4-diethylamino-salicylaldehyde, ethanol solution and deionized water, wherein the dosage of the tannic acid, the carbon nitride, the iron phthalocyanine, the 4-diethylamino-salicylaldehyde, the deionized water and the ethanol is as follows: tannic acid 0.8g; 480mg of carbon nitride; iron phthalocyanine 19mg; 0.5g of 4-diethylamino-salicylaldehyde; 58mL of deionized water; ethanol 24mL.
Adding 480mg of carbon nitride into 18mL of deionized water, and dispersing for 60min at normal temperature by ultrasonic waves to obtain a uniformly dispersed solution I; 19mg of iron phthalocyanine is added into 40mL of deionized water containing 0.8g of tannic acid, and the mixture is mixed and stirred for 60min at normal temperature (25 ℃) to obtain a uniform solution II; adding 0.5g of 4-diethylamino-salicylaldehyde into 24mL of ethanol solution, and mixing and stirring for 60min at normal temperature to obtain a uniform solution III;
step three, mixing the solution I, the solution II and the solution III, and stirring to obtain a uniformly dispersed solution;
fourthly, carrying out hydrothermal treatment on the uniformly dispersed solution in the third step through a hydrothermal kettle, wherein the hydrothermal temperature is 120 ℃ and the time is 10 hours;
centrifuging and drying the uniformly dispersed solution after the hydrothermal treatment for two times, and putting the precipitate into a drying oven to be dried at 60 ℃ to obtain a Fe/C3N4@TA-salicylaldehyde precursor;
and step six, calcining the Fe/C3N4@TA-salicylaldehyde precursor at a high temperature in a nitrogen atmosphere to obtain the nitrogen-doped graphene loaded iron monoatomic catalyst. Wherein the high-temperature calcination temperature is 900 ℃ and the time is 2h.
Example III
The preparation method of the nitrogen-doped graphene-supported iron monoatomic catalyst comprises the following steps of:
firstly, selecting carbon nitride as a nitrogen source, tannic acid as a carbon source, ferric acetylacetonate as an iron source, 4-diethylamino-salicylaldehyde, ethanol solution and deionized water, wherein the dosage of the tannic acid, the carbon nitride, the ferric acetylacetonate, the 4-diethylamino-salicylaldehyde, the deionized water and the ethanol is as follows: the dosages of tannic acid, carbon nitride, iron source, 4-diethylamino-salicylaldehyde, deionized water and ethanol are as follows: tannic acid 0.9g; 490mg of carbon nitride; iron acetylacetonate 21mg; 0.7g of 4-diethylamino-salicylaldehyde; 59mL of deionized water; ethanol 26mL.
Adding 490mg of carbon nitride into 19mL of deionized water, and dispersing for 60min at normal temperature by ultrasonic waves to obtain a uniformly dispersed solution I; 21mg of ferric acetylacetonate is added into 40mL of deionized water containing 0.9g of tannic acid, and the mixture is mixed and stirred for 60min at normal temperature (25 ℃) to obtain a uniform solution II; adding 0.7g of 4-diethylamino-salicylaldehyde into 26mL of ethanol solution, and mixing and stirring for 60min at normal temperature to obtain a uniform solution III;
step three, mixing the solution I, the solution II and the solution III, and stirring to obtain a uniformly dispersed solution;
fourthly, carrying out hydrothermal treatment on the uniformly dispersed solution in the third step through a hydrothermal kettle, wherein the hydrothermal temperature is 120 ℃ and the time is 10 hours;
centrifuging and drying the uniformly dispersed solution after the hydrothermal treatment for two times, and putting the precipitate into a drying oven to be dried at 60 ℃ to obtain a Fe/C3N4@TA-salicylaldehyde precursor;
and step six, calcining the Fe/C3N4@TA-salicylaldehyde precursor at a high temperature in a nitrogen atmosphere to obtain the nitrogen-doped graphene loaded iron monoatomic catalyst. Wherein the high-temperature calcination temperature is 900 ℃ and the time is 2h.
Comparative example one
The comparative example and the first example are different in that a mixed solution of 4-diethylamino-salicylaldehyde and ethanol is not added, and the specific preparation process is as follows:
(1) Weigh 500mgC 3 N 4 Adding the mixture into 40ml of deionized water, and performing ultrasonic treatment on the mixture at normal temperature for 60 minutes until a uniformly dispersed solution is obtained;
20mg of ferric acetylacetonate and 0.8506g of tannic acid are weighed and added to 20ml of deionized water, and the mixture is stirred at normal temperature for 60min until a uniform solution is obtained;
(2) Adding the obtained ferric acetylacetonate and tannic acid homogeneous mixed solution into C 3 N 4 In solution;
(3) Putting the obtained uniform mixed solution into a hydrothermal kettle, and carrying out hydrothermal treatment for 10 hours at 120 ℃;
(4) Centrifuging the liquid after hydrothermal treatment twice, taking the precipitate, and drying the precipitate in an oven at 60 ℃ to obtain a Fe/C3N4@TA precursor;
(5) Calcining the dried precursor for 2 hours at 900 ℃ under the protection of nitrogen gas to obtain Fe/NG-1.
Comparative example two
The comparative example and example one differ in that no tannic acid was added, and the specific preparation process is as follows:
(1) Weigh 500mgC 3 N 4 Adding the mixture into 40ml of deionized water, and performing ultrasonic treatment on the mixture at normal temperature for 60 minutes until a uniformly dispersed solution is obtained;
weighing 20mg of ferric acetylacetonate, adding the ferric acetylacetonate to 20ml of deionized water, and stirring the mixture for 60 minutes until a uniform solution is obtained;
weighing 0.6g of 4-diethylamino-salicylaldehyde, adding the mixture into 25ml of ethanol solution, and performing ultrasonic treatment on the mixture at normal temperature for 60min until a uniform solution is obtained;
(2) Adding the obtained ferric acetylacetonate uniform mixed solution into C 3 N 4 In solution; adding the obtained salicylaldehyde solution to C 3 N 4 In solution;
(3) Putting the obtained uniform mixed solution into a hydrothermal kettle, and carrying out hydrothermal treatment for 10 hours at 120 ℃;
(4) Centrifuging the liquid after hydrothermal treatment twice, taking the precipitate, and drying the precipitate in an oven at 60 ℃ to obtain a Fe/C3N4@salicylaldehyde precursor;
(5) Calcining the dried precursor for 2 hours at 900 ℃ under the protection of nitrogen gas to obtain Fe/NG-2.
Comparative example three
The comparative example differs from example one in that no tannic acid and no salicylaldehyde solution were added, and the specific preparation process is as follows:
(1) Weigh 500mgC 3 N 4 Adding the mixture into 40ml of deionized water, and performing ultrasonic treatment on the mixture at normal temperature for 60 minutes until a uniformly dispersed solution is obtained;
weighing 20mg of ferric acetylacetonate, adding the ferric acetylacetonate to 20ml of deionized water, and stirring the mixture for 60 minutes until a uniform solution is obtained;
(2) Adding the obtained ferric acetylacetonate uniform mixed solution into C 3 N 4 In solution;
(3) Putting the obtained uniform mixed solution into a hydrothermal kettle, and carrying out hydrothermal treatment for 10 hours at 120 ℃;
(4) Centrifuging the liquid after hydrothermal treatment twice, taking the precipitate, and drying the precipitate in an oven at 60 ℃ to obtain a Fe@C3N4 precursor;
(5) Calcining the dried precursor for 2 hours at 900 ℃ under the protection of nitrogen gas to obtain Fe/NG-3.
The final products of example 1 and comparative examples 1-3 above were used as catalysts in oxygen reduction systems, respectively.
Electrochemical performance was measured using a conventional three electrode system: hg/HgCl 2 The carbon rod is used as a counter electrode, and the glassy carbon electrode modified with the catalyst is used as a working electrode.
Working electrode preparation 5mg of the samples of example 1 and comparative examples 1-3 above were mixed with 485 μl of isopropanol, 15 μl of naphthol, respectively, and sonicated for 1h to form a homogeneous mixed solution; and (3) dripping 10 mu L of the mixed solution on the surface of the glassy carbon electrode, and naturally air-drying to obtain the glassy carbon electrode modified with the catalyst.
Electrochemical performance testing was accomplished using a pin electrochemical workstation. Electrochemical performance tests were performed in 0.1M KOH solution at a fixed scan rate (5 mV.s-1).
The electrochemical performances of example 1 and comparative examples 1 to 3 are shown in FIG. 2, wherein FIG. 2 (a) is a graph showing the polarization curve of the oxygen reduction reaction, and FIG. 2 (b) is a graph showing the potential of the half-wave of the oxygen reduction reaction. The Fe/NG obtained by calcining the Fe/C3N4@TA-salicylaldehyde precursor of the embodiment 1 of the invention is used as a catalyst, when the oxygen reduction performance of the Fe/NG is tested in a 0.1M KOH solution, when the current density is 5.5mA.cm < -2 >, the half-wave potential of ORR is 0.91V, the half-wave potential of ORR is higher than that of the comparative examples 1-3, and compared with the reported related documents, the material also has good oxygen reduction performance, and the material can be used as an effective catalyst for oxygen reduction.
The foregoing is only a preferred embodiment of the present invention, but the scope of the present invention is not limited thereto, and any person skilled in the art, who is within the scope of the present invention, should make equivalent substitutions or modifications according to the technical scheme of the present invention and the inventive concept thereof, and should be covered by the scope of the present invention.
Claims (9)
1. The preparation method of the nitrogen-doped graphene-supported iron monoatomic catalyst is characterized by comprising the following steps of:
s1, selecting carbon nitride as a nitrogen source, tannic acid as a carbon source, ferric acetylacetonate or ferric phthalocyanine as an iron source, 4-diethylamino-salicylaldehyde, ethanol solution and deionized water;
s2, dispersing carbon nitride in deionized water through ultrasonic waves to obtain a uniformly dispersed solution I; adding an iron source into deionized water containing tannic acid, and mixing and stirring to obtain a uniform solution II; adding 4-diethylamino-salicylaldehyde into an ethanol solution, and mixing and stirring to obtain a uniform solution III;
s3, mixing the first solution, the second solution and the third solution, and stirring to obtain a uniformly dispersed solution;
s4, carrying out hydrothermal treatment on the uniformly dispersed solution in the step S2 through a hydrothermal kettle;
s5, centrifugally drying the uniformly dispersed solution after the hydrothermal reaction to obtain a Fe/C3N4@TA-salicylaldehyde precursor;
and S6, calcining the Fe/C3N4@TA-salicylaldehyde precursor at a high temperature in a nitrogen atmosphere to obtain the nitrogen-doped graphene loaded iron monoatomic catalyst.
2. The method for preparing the nitrogen-doped graphene-supported iron monoatomic catalyst according to claim 1, wherein the method is characterized by comprising the following steps: the dosage of tannic acid, carbon nitride, iron source, 4-diethylamino-salicylaldehyde, deionized water and ethanol in S1 is as follows: 0.8-0.9g of tannic acid; 480-500mg of carbon nitride; 19-21mg of iron source; O.5-O.7g of 4-diethylamino-salicylaldehyde; 58-60mL of deionized water; ethanol 24-26mL.
3. The method for preparing the nitrogen-doped graphene-supported iron monoatomic catalyst according to claim 2, wherein the method is characterized by comprising the following steps: the dosage of tannic acid, carbon nitride, iron source, 4-diethylamino-salicylaldehyde, deionized water and ethanol in S1 is as follows: 0.8506g of tannic acid; 500mg of carbon nitride; 20mg of iron source; 0.6g of 4-diethylamino-salicylaldehyde; 60mL of deionized water; ethanol 25mL.
4. The method for preparing the nitrogen-doped graphene-supported iron monoatomic catalyst according to claim 2, wherein the method is characterized by comprising the following steps: the dosage of tannic acid, carbon nitride, iron source, 4-diethylamino-salicylaldehyde, deionized water and ethanol in S1 is as follows: tannic acid 0.8g; 480mg of carbon nitride; 19mg of iron source; 4-diethylamino-salicylaldehyde o.5g; 58mL of deionized water; ethanol 24mL.
5. The method for preparing the nitrogen-doped graphene-supported iron monoatomic catalyst according to claim 2, wherein the method is characterized by comprising the following steps: the dosage of tannic acid, carbon nitride, iron source, 4-diethylamino-salicylaldehyde, deionized water and ethanol in S1 is as follows: tannic acid 0.9g; 490mg of carbon nitride; 21mg of iron source; 0.7g of 4-diethylamino-salicylaldehyde; 59mL of deionized water; ethanol 26mL.
6. The method for preparing the nitrogen-doped graphene-supported iron monoatomic catalyst according to claim 1, wherein the method is characterized by comprising the following steps: and S2, the dispersion time of ultrasonic waves is 60min, the temperature is normal temperature, the stirring time of mixing and stirring is 60min, and the temperature is normal temperature.
7. The ceramic composite preparation device according to claim 1, wherein: and S4, the hydrothermal temperature is 120 ℃, and the time is 10 hours.
8. The method for preparing the nitrogen-doped graphene-supported iron monoatomic catalyst according to claim 1, wherein the method is characterized by comprising the following steps: the temperature of the centrifugal drying in S5 was 60 ℃.
9. The method for preparing the nitrogen-doped graphene-supported iron monoatomic catalyst according to claim 1, wherein the method is characterized by comprising the following steps: and S6, the high-temperature calcination temperature in the process of S6 is 900 ℃ and the time is 2h.
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